Novel precise separation technology will significantly improve the circulation of critical metals in automotive lithium-ion batteries | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Novel precise separation technology will significantly improve the circulation of critical metals in automotive lithium-ion batteries Yi Dou, Aya Heiho, Chiharu Tokoro, Yasunori Kikuchi This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4213507/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Recently, large-scale projects using pyro/hydrometallurgy have been introduced worldwide for recycling spent automotive lithium-ion batteries (LIBs), while a few precise separation methods are under development to support a faster, complete, eco extraction of positive electrode active materials. However, the extent to which the precise separation impacts the whole recycling system and the requirement for co-ordinated policy and system design remains poorly understood. Here, we develop an integrated assessment model with technical and policy scenarios that applies a novel precise separation method named high-voltage pulsed discharge to the emerging Japanese electric vehicles market during 2025–2050. We show that the precise separation can be a must-have process that may significantly reduce the life-cycle greenhouse gas emissions, the resource consumption potential and the in-use stocks of critical metals (Li, Ni, Co, Mn) compared with the conventional technology combination. To achieve this condition, combined efforts from technology development, system integration, secondary usage regulation and eco-design in LIBs are required. Scientific community and society/Energy and society/Energy policy Physical sciences/Engineering/Chemical engineering Earth and environmental sciences/Environmental social sciences/Environmental impact Scientific community and society/Business and industry/Industry Figures Figure 1 Figure 2 Figure 3 Figure 4 Introduction Because of global e-mobility ambitions, rapidly expanding electric vehicle fleets (EVs) worldwide require a huge capacity of automotive batteries, which cannot avoid demanding massive amounts of critical metals, such as cobalt 1 , lithium 2 , nickel and manganese 3 . Battery technology and recycling advancement are widely acknowledged as two must-have strategies, where recycling progress is expected to support a sufficient secondary supply of minerals to relieve the resource shortage in the medium to long term 4 . With the addition of the regional disparity in resource endowment, major economies, particularly the European Union and Japan, must face serious challenges in resource security while rushing to realize a decarbonized society 5 . The implementation of the EU Sustainable Batteries Regulation 6 , as an iconic event, suggests that recycling batteries has become an obligation despite many current recycling projects not being economically beneficial 7 . For decades, researchers worldwide have tried to determine an ultimate solution to recycle spent automotive lithium-ion batteries (LIBs), while huge investments have been made for scaled-up demonstration projects. Beyond various technologies remaining at a laboratory level, extractive metallurgical processes, including pyrometallurgy and hydrometallurgy, have become common industrial techniques in recycling critical metals from spent automotive LIBs 8 . Pyrometallurgy can treat batteries in a wide range of types and constitutions, using heating to convert the metal oxides into metal alloys containing Co and Ni, while Li and Al remain in the slags 9 . This method is easy to scale up with less material input and additional waste disposal, but it consumes a large amount of energy in combustion and calcination while incurring a large capital cost 10 . By contrast, hydrometallurgy uses added reagents and solvents to extract and separate metals from spent automotive LIBs 11 . It enables a high-quality recovery of critical metals, with low energy consumption, gas emissions and capital cost, but spends a long time in processing and brings about added material consumption and wastewater treatment. Despite demonstration projects revealing that the optimized combination of pyrometallurgy and hydrometallurgy can flexibly deal with various types of spent automotive LIBs while maximizing the recovery rate of critical metals on a large scale, these processes do not significantly reduce economic costs and environmental burdens that can only be reduced in the case of directly recycling the cathode materials 12 . Direct recycling is supported by advanced disassembly and separation technologies, which have been of increasing interest in recent years 13 . Optimized manual disassembly and automatic disassembly have both been considered as possible ways of dismantling batteries to their individual electrodes with up to 90% savings in processing time and cost 14 . A delamination process follows disassembly, such as soaking in ethylene glycol 15 , Cyrene and other solvents 16 , to completely separate the cathode materials from the Al foil. In principle, the recycled cathode materials can be regenerated or reincorporated into a new cathode electrode 17 . Currently, these technologies are still far from practical application, suffering from difficulties in satisfying the quality of recycled materials for remanufacturing, dealing with various types and structures of batteries, and reducing labour costs in disassembly 18 . In summary, despite commercial projects usually adopting pyrometallurgy and hydrometallurgy to recycle spent automotive LIBs because of good performance on scaling up, future improvements in economic and environmental performance are likely to be obtained from direct recycling that realizes a shorter circular route. Beyond the techniques well introduced in previous studies, the general application of precise separation technologies for composite materials, such as microwave processing 19 and ultrasonication 20 , was insufficiently assessed in recycling spent LIBs; in particular, the economic and environmental impacts were less understood. A precise separation technique is first developed to pretreat the dismantled battery cells for the following metal recovery by hydrometallurgy, but it has the potential to directly recycle the positive electrode active materials (PEAMs) if the separation is precise enough to extract and retain the properties of recovered PEAMs (Supplementary Fig. S1). Recently, an expectable precise separation method, named high-voltage pulsed discharge, that has attracted attention was proved feasible in quickly and precisely separating the PEAMs from the Al foil using a fine-tuned single pulsed power without heating and additives (Supplementary Fig. S2). The concentration of Al in the recovered PEAMs was reduced to 2.95%, while almost 99% of the recovered PEAMs retained the original chemical properties, which can be incorporated in LIB manufacture after a resynthesis process 21 . According to the purity, the recycled PEAMs can be reincorporated in new production through a direct recycling process, or otherwise sent to the hydrometallurgical process for metal recovery as an easy pretreatment. In both cases, life-cycle assessment (LCA) indicated possible significant reductions in greenhouse gas (GHG) emissions and resource consumption potential (RCP) compared with the conventional processing by pyrometallurgy and hydrometallurgy after scale-up mainly because of the much smaller input of energy and chemicals 20 . From a systemic and dynamic perspective, we need to understand the flexibility (uncertain positioning) of applying precise separation techniques and the extent to which such a precise separation technology will contribute to the performance of the recycling system, particularly considering its flexible positioning in system design and the co-ordination with resource and energy policies. Here, we aim to estimate the future changes in GHG emissions and RCP in the case of applying a high-voltage pulsed discharge method for a complete circulation of PEAMs compared with the cases in conventional technology combination and system design by combining dynamic material flow analysis (MFA) and prospective LCA (see model framework in Fig. 1 and details under Methods). The case area we chose is Japan because Japan is experiencing an energy and resource shortage, where the battery and automotive industries are rushing to promote the transition towards EVs, but a recycling system for spent automotive LIBs has not been finally established. The discussion using Japan as a case will have more flexibility in applicability than using the first movers and be referential to the late movers. First, through a yearly dynamic simulation of the changes in Japan’s automotive market and the material flow of automotive LIBs, we evaluate how the automotive LIB market may rely on the precise separation for PEAMs and analyse the feasibility and challenges of applying the high-voltage pulsed discharge method as a case from the systemic perspective. Then, through prospective LCA, we estimate the overall impacts of applying precise separation technology in the system on the annual GHG emissions and RCP, assuming the realization of a total decarbonization by 2050 in Japan. Here, we set scenarios considering three factors: the positioning of precise separation, the secondary usage or not of the spent LIBs and any future battery model changes. Finally, we compare the results with the cases using conventional technologies combining hydrometallurgy and pyrometallurgy and combustion with landfill. Because the application of precise separation technology was indicated to have great potential in improving the eco-efficiency of recycling systems, we further comment on the opportunities and challenges for actual technology diffusion. Results Capacity required for recycling spent automotive LIBs The life cycle of an automotive LIBs includes their production, primary use in EVs, secondary use in stationary energy storage, collection and recycling (Fig. 1 ). As shown in Fig. 2 , both the annual stocks and flows of critical metals in automotive LIBs will keep rapidly increasing in Japan during 2025–2050. The critical metals in use were estimated to reach 2,128 kt-LiNiCoMn (the total weight of Li, Ni, Co, Mn included in automotive LIBs) by 2050 in the case of recycling immediately, of which the number can increase to 2,679 kt-LiNiCoMn in the case of recycling after secondary usage because of the degradation of spent LIBs used for energy storage. Forcing the spent LIBs to secondary use slows down the circulation of critical metals for several years, leading to an increased annual critical metals input of 40 kt-LiNiCoMn (50% increase) in manufacturing automotive LIBs after 2035. Furthermore, the penetration of new battery models such as NMC811 and NMC955 will also be decreased. In both cases, the peak quantity of critical metals newly input in LIB manufacture appears at around 2040, but the first year of reaching the peak will be 10 years earlier in the case of immediate recycling. According to the MFA result, precise separation indicates its ability to deal with the rapidly increasing amount of spent LIBs. One such method is the high-voltage pulsed discharge method, where one high-voltage pulsed discharge will spend 10 seconds on a batch treatment of a positive electrode (PE) sheet that is around 72.45 grams. If the equipment operates 8 hours/day and 245 days/year, the treatment capacity will be 51.12 t-PE sheets annually; otherwise, the capacity can increase by 4.5 times if automatically operating 24 hours/day and 365 days/year. In the case of immediate recycling, 2,800–12,500 bases of high-voltage pulsed discharge equipment should be in operation by 2050. Considering that in Japan there were around 3,000 car dismantlers recorded in operation in 2022 22 , it is expected that a few items of precise separation equipment will be installed initially to conduct the separation of PEAMs. This substantially reduces the dependence on pyro/hydrometallurgy and can avoid excess transport as part of safety risks and environmental impacts. Environmental impact of applying precise separation in recycling spent automotive LIBs The development and application of precise separation technology play a critical role in improving the eco-efficiency of recycling spent automotive LIBs, but the potential improvement should have a synergy or trade-off with the technology combination and energy policy. We defined four kinds of technology combinations focusing on the positioning of the precise separation, with two energy policies such as immediate recycling of the PEAMs or recycling after secondary use (see Table 1 in the Methods section). As shown in Fig. 3 , the life-cycle GHG emissions relating to automotive LIBs would finally decrease from 2040 if the decarbonization strategies were strictly implemented, but the RCP would keep increasing. Among the scenarios, direct recycling of PEAMs by precise separation (a-4, b-4) led to the overall lowest environmental and resource impacts. This is because of the obvious environmental benefit of substituting raw PEAM products. During 2025–2050, a maximum of around half of the accumulated GHG emissions and RCP can be reduced compared with the cases of incineration and landfill (a-1, b-1). The scenario results indicate the secondary use of spent LIBs can to some extent suppress the environmental impact because the policy delayed the recycling processes, remanufacturing and new production towards the era of decarbonization. Thus, if manufacturers failed to directly recycle the PEAMs by precise separation, the better choice is to secondarily use the spent LIBs; however, it is better to apply the precise separation techniques for immediate and direct recycling. Of course, we need to consider secondary use, which the the user may value more, and not ignore the problem in life-cycle RCP because of various technology combinations beyond decarbonization. Another crucial indicator, circulation rate, was significantly changeable in response to the decision on secondary use (as shown in Fig. 4 ). During 2025–2050, Ni would be the resource with the greatest demand, and then Co, Li and Mn. Although secondary use of spent LIBs can reduce the annual input of critical metals in automotive LIBs manufacturing and remanufacturing by about 15%, it also greatly suppresses the circulation rate of critical metals by around 20% compared with the case of immediate recycling. In other words, the lower the circulation rate, the more Japan will need to import critical metals from overseas. Immediate recycling of the PEAMs would support a high circulation rate of critical metals and help in expanding the size of the domestic recycling market. Given the future projection prices of Li, Ni, Co and Mn as USD/t 14,000, 40,000, 100,000 23 and 4,000 (2020’s level doubled) 24 by 2050, in the case of immediate recycling, the annual market value of the four metals in Japan may reach USD 11 billion by 2050, in which circulated metals would have a market value of USD 9 billion. If directly recycling the PEAMs was finally diffused, circulated PEAMs may have a revenue of about USD 16 billion by 2050 (60 USD/kWh; cathode cost doubled from 2020’s level) 25 . Considering the probable synchronization with the EU Sustainable Batteries Regulation, immediately recycling the spent LIBs should contribute the most to achieving the minimum levels of cathode materials recovery in Japan, where directly recycling the PEAMs supported by novel precise separation should be the best approach for environmental and resource conservation. Being a large metal resource importer, a timely increasing of the circulation rate in Japan should ease the mismatch between the supply and demand of critical metals and enhance resource security and supply chain resilience as much as possible. Discussion Using the high-voltage pulsed discharge method as a case, our analysis indicated the penetration of such precise separation techniques in recycling the spent automotive LIBs is basically feasible and can significantly reduce the environmental impact and additional resource consumption. In particular, the results could suggest the expected technology features and the roadmap to implement such technologies. First, an expected precise separation technology may not perform perfectly in directly recycling the cathode materials but should at least perform well as a pretreatment process. Here, good performance means a physical approach that is generally applicable, may only use electricity, should consume significantly less energy and solvents, and avoid the following treatment of emitted gases and wastewater that yield additional environmental burden and economic cost (Supplementary Fig. S1 ). For instance, the high-voltage pulsed discharge method is also applicable to physically separating silver and copper wires from spent solar panels 26 with a designed system, potentially reducing by 17% life-cycle GHG emissions and in total saving input resources 27 . Recent experiments furthermore revealed the method can be applied to separate laminated carbon fibre–reinforced plastic composites 28 . Yet, as a roadmap, such a precise separation technique can be penetrated in three stages: Stage 1, incorporating the technique as a pretreatment process to reduce the dependency on pyrometallurgy and hydrometallurgy; Stage 2, further developing the technique with a specific design of products towards the direct recycling of PEAMs; and Stage 3, encouraging faster recycling of the spent LIBs to speed up the circulation of critical metals. Beyond our assumptions and simulation, a few opportunities and challenges have significant influences on the assessment results. The opportunities include the following. First, removing the Al in advance will greatly help us to more efficiently and ecologically recover the Li from the cathode materials 29 if combined with the appropriate method 30 . Second, the precise separation techniques should be also applicable in recycling the batteries from electric two-wheelers, electric bicycles and electric trucks 21 , leading to a much larger market than our evaluation (Supplementary Fig. S3). Third, the penetration of such precise separation techniques will support a further eco-design and standardization of batteries. In fact, the key to an efficient precise separation is in the design of adhesives 31 . In the case of using high-voltage pulsed discharge, filling a metal sphere 32 or a small proportion of carbon black 33 in the adhesives can concentrate the pulsed power to easily destroy the adhesion, supporting a better performance of the separation in an air environment compared with the separation in a water pool 34 (avoiding wastewater treatment). Of course, the overall structure of the battery should be designed for disassembly to save labour costs in competing with pyrometallurgy 35 . However, several challenges and uncertainties may influence the application of precise separation techniques. First, despite experiments of high-voltage pulsed discharge indicating 93.9% of the PEAMs can be recovered and that almost 99% of them can be used in LIB manufacture 21 , this result must be retained and improved on an industrial scale. Second, the time and cost of beforehand disassembly will be a bottleneck when applying the precise separation technique, and a corresponding design of automatic disassembly based on industrial robots is indispensable 36 . Third, in our simulation, all the recovered PEAMs can be reused for new battery manufacture because the capacity requirement for automobiles is increasing rapidly, despite the continuous improvements in battery models. If the penetration of EVs is unexpectedly slow or the battery model changes extremely quickly, directly recycled PEAMs still have to be recovered as metal elements for next-generation battery manufacture. Fourth, the capacity of spent automotive LIBs may greatly overstep the capacity required for stationary energy storage. This study revealed that spent LIBs that are in secondary usage would gradually increase to 400 GWh by 2050 (see Supplementary Fig. S11), assuming the maximum proportion in automotive LIB capacity is 25%, as projected by the International Renewable Energy Agency 37 . This proportion may further decrease considering the possible impact of vehicle–grid integration 38 . The penetration of precise separation techniques will also bring about a positive influence on the distribution of the recycling system networks for spent LIBs. The costs of collecting and transporting spent LIBs can make up 5–70% of the total costs for recycling 39 because the current production and recycling locations are concentrated 40 and because collecting and transporting LIBs needs a dedicated area that includes a large buffer zone and risk insurance to protect from frequent fires and explosions 41 . Here, the application of the precise separation after battery collection can start from a small capacity, while the outputs (Al and PEAMs) are safe and high purity. It also surely reduces the need for long-distance transportation and the safety risks associated with the transport to decrease the environmental impacts and economic costs. In particular, the recovered PEAMs do not need a pyrometallurgy process thereby avoiding a large investment in facilities and equipment. It is expected that precise separation techniques will be applied in developing a vertically integrated, in-country local recycling chain to secure the supply chain for critical metals. Having the whole world in view, wide management of critical metals should be conducted in automobile industries. Historically, Japan annually exports new and second-hand vehicles to the rest of the world, equalling one-fourth of the domestic car sales 42 . In contrast, the market share of automotive LIB production by Japanese companies has decreased from 51.7% in 2015 to 21.1% in 2020 43 . Moreover, the major countries in the European Union have strengthened the regulation on the flow of automotive LIBs and related critical metals, such as the need to label the metals’ recovery rate and carbon footprints of products 44 . Near Japan, both China and Korea have invested in recycling automotive LIBs 45 , and the costs of recycling spent LIBs in China are significantly lower than in the United Kingdom, the United States and South Korea 46 . To balance the resource demand and supply, of course, Japan could initiate international cooperation on establishing a wide-area circulation. In contrast, the application of precise separation may support another option to first extract the PEAMs, followed by the metal refining process using domestic facilities. Such a practice will surely provide knowledge and experience to other late movers that have declared their e-mobility ambitions. In summary, we strongly recommend trying to use the emerging precise separation techniques for pretreating or directly recycling the active materials in spent LIBs and faster recycling the critical metals with the help of the eco-design for easy dismantling. Combined efforts in technology, regulatory, trading, and economic areas should make the best contributions to this issue. Although our primary study was limited in domestic boundary and rough simulation because of the lack of data and various uncertainties, we believe our scenario results have provided robust conclusions about the synergy and trade-off between the targets on the e-mobility emotion, GHG emissions, resource security, circulation rate and financial balance regarding the development of the automotive LIB industry, where novel precise separation techniques were indicated to support the best solution. Methods Definitions and system boundary As shown in Fig. 1 , the stocks and flows of PEAMs in the automotive market, which contains the critical metals Li, Co, Ni and Mn, were considered totally circulated domestically in Japan through an assumption of a 100% recycling rate. These critical metals were thought to only come from overseas mining and extraction (primary supply) and domestic recycling and recovery (secondary supply). The spent LIBs were directly sent to the recycling system or used as stationary batteries for energy storage, with no export or other diversion. Here, the vehicle fleets defined in this study included passenger cars but excluded buses and trucks because of the strong competition from the fuel cell vehicle industry. Also, the LIBs included the ones served in battery electric vehicles (BEVs) and plug-in hybrid electric vehicles (PHEVs). In the boundary of LCA, the remaining parts of LIBs were considered to be newly manufactured in all scenarios, and the material losses (not caused by technical defects) in mining, extraction, manufacturing and recycling were not considered. The energy storage market was assumed to unconditionally accept the spent LIBs if the policy promoted this, of which the capacity would not exceed the market projection of stationary energy storage. Historical changes in the stocks and flows of critical metals Assuming the precise separation using a high-voltage pulsed discharge method will be applied from 2025, a dynamic MFA approach 47 was developed to quantify the cycle of critical metals from 2025 to 2050. The approach was annually iterated to simulate the changes in the passenger car market, lifetime use of vehicles and LIBs, secondary use, and recycling of spent LIBs, as usually applied 48 . First, the passenger car ownership per household \(C\) was calculated as shown below: $$C=\frac{N·\gamma ·(1-\eta ·\delta )}{1+\alpha ·\text{e}\text{x}\text{p}(-\beta ·\frac{\stackrel{-}{I}}{\stackrel{-}{P}})}$$ 1 where \(N·\gamma ·(1-\eta ·\delta )\) represents the potential passenger car market, negatively affected by the multiple of average annual income per household \(\stackrel{-}{I}\) and average purchase price per vehicle \(\stackrel{-}{P}\) . \(N\) is the number of households in Japan, \(\eta\) is the rate of membership of car sharing, and \(\delta\) is the decrease rate of car ownership by car sharing 49 . Parameters \(\alpha\) and \(\beta\) were set as 10.5 and 0.791 50 , respectively. Parameter \(\gamma\) was estimated as 0.000757 by the average fitted value because of the passenger car ownership rate during 2015–2020. The results showed that the ownership of passenger cars would gradually decrease from 61 million to 46 million during 2020–2050 mainly because of the decrease in population (Supplementary Fig. S3, S5). Then, according to the ambitious targets carried out by the Japanese government and automotive associations, the sales of internal combustion engine vehicles will be stopped domestically by the early 2030s, while the transport sector should be decarbonized by 2050 51 . Thus, we assumed that the ICEs will gradually quit the new sales market by 2035 and that the HEVs will gradually quit the new sales market by 2050, as shown in Supplementary Fig. S6. The scenario result (Supplementary Fig. S7) based on the assumption was close to the scenario ‘BEV75’ estimated by the Japan Automobile Manufacturers Association 52 . Regarding the projection of battery model changes, we referred to the high-probability scenario (named ‘NCX’) established by Xu et al. 3 (Supplementary Fig. S8). The battery producers were assumed to replace Co with Ni-rich PEAMs to reduce costs. Thus, the battery model NMC111 will gradually change to NMC523, NMC622, NMC811 and NMC955. The NCX scenario proposed that although lithium iron phosphate (LFP) has advantages in technology readiness, costs and resource availability and lithium–sulphur (Li–S) and lithium–air (Li–Air) batteries have specific energy densities three times greater than NMC LIBs, they are more difficult to use than NMC LIBs because of the low specific energy of LFP and low technology readiness of Li–S/Li–Air batteries. In 2023, the sales of BEVs and PHEVs were only 3.6% of the passenger car market 53 . The timing of collecting spent LIBs can affect both the lifespan of EVs and the service life of automotive LIBs in EVs (Fig. 1 ). To estimate the lifespan of vehicles, we conducted the following Weibull distribution equation: $$F\left(t\right)=1-{e}^{-{\left(\frac{t}{}\right)}^{m}}$$ 2 where \(F\left(t\right)\) is the survival rate of a vehicle when it services \(t\) years. Parameters \(m\) and µ are calibrated as 2.69 and 15.49, respectively, according to the age distribution of existing passenger cars surveyed in 2019 54 (Supplementary Fig. S9, S10). For easier dynamic simulation, we assumed all types of passenger cars have the same survival rate and that the lifespan does not extend yearly because of the launch of new cars. The lifespan of automotive LIBs was set as 8 years, and the lifespan of spent LIBs for secondary usage in stationary energy storage was set as 10 years, referred to in many studies such as those by Hara 55 and Zeng et al. 5 . Prospective LCA and scenarios setting Based on the scaled-up experiment of the high-voltage pulsed discharge method applied to separate the PEAMs 56 , we conducted a prospective LCA approach 57 to quantify the possible environmental impact of applying precise separation to recycle PEAMs while considering the uncertainty in evaluating such an emerging technology 58 . We set eight scenarios to simulate the different situations considering four technology combinations (landfill after incineration, pyrometallurgy and hydrometallurgy combination, hydrometallurgy after precise separation, or direct recycling after precise separation) and two choices in the timing of recycling spent LIBs (immediate recycling, or recycling after secondary use) (see Table 1 ). Table 2 summarizes the details of processes considered in the cases defined in Table 1 . In Cases a-1 and b-1, spent LIBs are incinerated and landfilled without metal resources recycling. In Cases a-2 and b-2, spent LIBs are first disassembled into cells that are then roasted and smelted for metal recovery. In Cases a-3 and b-3, spent LIBs are disassembled into cells in which the PEAMs are then separated by high-voltage pulsed discharge for metal recovery. In Cases a-4 and b-4, the PEAMs are separated by high-voltage pulsed discharge and directly incorporated for new automotive LIBs production. Table 2 Production and recycling processes defined in cases Processes in cases in Table 1 Case a-1, b-1 Case a-2, b-2 Case a-3, b-3 Case a-4, b-4 Mining and extraction 〇 〇 〇 〇 M-SO 4 production 〇 〇 〇 〇 Raw PEAM production 〇 〇 〇 〇 PEAM production 〇 〇 〇 〇 Battery production 〇 〇 〇 〇 Use in vehicle 〇 〇 〇 〇 Collection/dismantling 〇 〇 〇 〇 Incineration 〇 Landfilling 〇 Battery pack dismantling 〇 〇 〇 Roasting 〇 Smelting 〇 〇 Battery cell dismantling 〇 〇 Pulsed discharging 〇 〇 Recycling of metal resources 〇 〇 〇 Based on the scaled-up analysis in the previous study 56 , we further considered the annual changes in impact assessment in the target of realizing a carbon neutral society by 2050 59 . In the fiscal year 2022, grid electricity used in Japan emitted 0.435 kg-CO 2 /kWh 60 on average, which will be reduced to 0.25 kg-CO 2 /kWh by 2030 and net zero by 2050 because of the official projection of energy demand and supply 61 . Excluding incineration and landfilling, pyrometallurgy, hydrometallurgy, dismantling, separation, and other processes will be gradually decarbonized by 2050. However, while decarbonization may bring about more resource consumption 62 , optimistically, we assumed the following technological innovation can suppress this additional resource consumption (Supplementary Table S8). Regarding the lack of data for LCA on different types/sizes of automotive LIBs, we assumed the intensity of GHG emissions and resource consumption potential is proportional to the weight of PEAMs in a standard LIB pack (per vehicle). Accordingly, the LCA on LFP, Li–S, and Li–Air battery production and recycling as well as the secondary use of spent LIBs was out of the scope of this work. Limitations and uncertainties Applying an integrated model, our simulation and scenario analysis build on various assumptions and parameters that cannot avoid correlated limitations and uncertainties (Table 3 ). First, the EV market and stationary energy storage market in Japan may not optimistically follow the government’s ambition and institutional projections. A lower popularization rate of EVs and LIBs will de-level the simulation and analysis results in our study. Here we tested the influence on critical metals’ circulation if the energy storage market does not accept spent LIBs or is infinite to accept them (Supplementary Fig. S13). Second, the lifespan of passenger cars and automotive LIBs was fixed, but it may gradually extend in the future. Of course, compared with our simulation, the recycling of spent LIBs will slow down and the annual production of LIBs will increase in proportion. Third, the battery capacity required for EVs was assumed to be fixed in the future as the reference set 3 (Supplementary Table S5). Although the capacity for one EV will increase in the future, the increment of energy intensity in the new battery model will increase to offset the capacity requirement. Fourth, the collection rate of spent LIBs and the actual recycling rate were set as 100% for easier simulation. In the near future, all the automotive LIBs may have their own codes in the tracking system, while the recycling rate may approach 100% 63 . As a sensitivity analysis, the collection rate was found to mainly affect Cases a-1 and b-1 in terms of life-cycle GHG emissions and affect Cases a-4 and b-4 in terms of potential resource consumption because of the obvious differences in parameter on circulation and resource consumption potential (Supplementary Figs S14, S15; Supplementary Tables S9, S10). Fifth, the battery models such as LFP, Li–S and Li–Air were not considered because of the scenario adopted from Xu et al. 3 . In fact, all-solid-state batteries have advantages in application to light-duty EVs, while LFP will have a large share in heavy-duty EVs and stationary energy storage 64 . In the long term, various batteries will share the market, for which we need to verify the performance of precise separation considering different structures in the cathode active materials 65 . Sixth, in LCA, we set NMC111 as the reference standard 56 and conducted a sensitivity analysis accordingly 56 . An LCA study in China showed that the LFP battery, NMC battery and LMO battery (28 kWh) would produce GHG emissions in the production of 3,061 kg CO 2 -eq, 2,912 kg CO 2 -eq and 2,705 kg CO 2 -eq, respectively 66 ; in addition, these results vary across countries 67 . Seventh, transport distance and volume were fixed in LCA, but it could be quite reduced because of the application of precise separation. Table 3 Description and assumption of key model parameters Key parameters Description/assumptions Details Passenger car ownership Passenger car ownership is assumed to be affected by population 68 , the number of households 69 , annual income per household, consumer price of vehicles 62 , and the participation of car sharing 49 . Road infrastructure, public traffic systems, and urban shape are considered fixed parameters. The import and export of passenger cars are out of the scope of this paper. Supplementary Tables S1, S2 Supplementary Figs S3–5, S9–11 EV market share The EV market share is assumed to increase according to the Carbon Neutral Target declared in Japan 59 . The sales of internal-combustion engine vehicles will be stopped from the year 2035, and the proportion of EVs (almost BEVs) in new car sales linearly increases to 90% by 2050, while the proportion of Fuel cell vehicles reaches 10% 52 . The service life of vehicles is assumed to remain the same as in 2019 70 . Supplementary Tables S3, S4 Supplementary Figs S6, S7 Battery capacity of BEV/PHEV The battery capacity for BEVs and PHEVs is set as the sales-weighted average based on the projection of small, mid-size, and large car fleets 3 . Supplementary Table S5 Stationary energy storage market The capacity of the stationary energy storage market is set not to surpass 25% of the capacity of automotive LIBs in use in EVs 37 . Supplementary Table S13 Supplementary Fig. S12 Battery lifetime The lifetimes of automotive LIBs in use in EVs and stationary energy storage are assumed to be 8 and 10 years, respectively 3,5 . Supplementary Table S6 Battery model changes The model change of the automotive batteries in Japan is assumed to keep the same path of the worldwide market, following the ‘NCX’ scenario of Xu et al. 3 . Supplementary Fig. S8 Recycling rate and residual loss The collection rate of spent automotive LIBs is assumed to be always 100% during 2025–2050. The weight of critical metals included in the PEAMs are set as the same as those set by Xu et al. 3 . Residues are not in consideration. Supplementary Table S7 Life-cycle GHG emissions and RCP factors Except for the emissions from waste combustion, life-cycle GHG emissions are assumed to decrease in line with the decarbonization of the power generation sector in Japan 61 . Life-cycle RCP is assumed not to change in the future. Supplementary Table S8 Declarations Data availability All data analyzed in this study are included in its Supplementary information files. Code availability The mathematical algorithm used in this study is available from the corresponding author upon reasonable request. Acknowledgements This work was supported by MEXT/JSPS KAKENHI Grant Number JP21H03660, JP21K14276 and JP20K20016, JST-Mirai Program Grant Number JPMJMI19C7 and JST COI-NEXT Program Grant Number JPMJPF2003. We would like to thank Mr. Izuru Suwa for his helps in LCA data collection. Activities of the Presidential Endowed Chair for “Platinum Society” at the University of Tokyo are supported by the KAITEKI Institute Incorporated, Mitsui Fudosan Corporation, Shin-Etsu Chemical Co., ORIX Corporation, Sekisui House, Ltd., the East Japan Railway Company, and Toyota Tsusho Corporation. Author contributions Y. D. conceived the original idea and designed the research. C. T. and Y. K. supervised and led the work. Y. D. and A. H. developed the model. Y. D. and A. H. contributed to system definition and data collection. Y. D. run the simulation and prepared the figures. A. H., C. T., and Y. K. enhanced the scenarios and discussion in technology development and policy making. Y. D. drafted the paper. Y. D. analyzed the results and contributed to writing this paper. Competing interests The authors declare no competing interests. References Gent, W. E., Busse, G. M. & House, K. Z. The predicted persistence of cobalt in lithium-ion batteries. Nat. 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Fleet Composition of the Passenger Vehicles in Japan (AIRIA, 2019). Additional Declarations There is NO Competing Interest. Supplementary Files Supplementaryinformation.docx Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-4213507","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":287163946,"identity":"ed01e6ae-1a23-465f-84b9-3bb302875694","order_by":0,"name":"Yi Dou","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA60lEQVRIiWNgGAWjYFCCBAaGDwZyPBDOAaigBAEtjDMMjEFaGBuI1sLMw2DMgKoFHzA4nnxM2qbAQIZBIoH9wYczh+UY2A8/YLDcgUfLmWdp0jkGBjxALYyNM24cNmbgSTNgkDyDR8uNHDOglj9ALfkfm3k+HE5sYMhhYJBsI6DFAmoLRAv/GyK0MMC13ABqkSBgi+SZZ8mWPUAtbDwPGGfOOJNuzCbxzOAAPr/wHU8+eOPHHwN7fvYEhg8fjlnL8fMnP3wsiSfEFA5AGWwQqhnMOCzZgFuLPJpcHZhk/IhHyygYBaNgFIw4AAAVK0t0jXDy+wAAAABJRU5ErkJggg==","orcid":"https://orcid.org/0000-0002-6665-1653","institution":"The University of Tokyo","correspondingAuthor":true,"prefix":"","firstName":"Yi","middleName":"","lastName":"Dou","suffix":""},{"id":287163947,"identity":"9def814e-4cb9-44aa-91f1-56386c7f7d0f","order_by":1,"name":"Aya Heiho","email":"","orcid":"","institution":"Tokyo City University","correspondingAuthor":false,"prefix":"","firstName":"Aya","middleName":"","lastName":"Heiho","suffix":""},{"id":287163948,"identity":"158e3b3c-1869-44b9-8d7f-d538b6bc5e56","order_by":2,"name":"Chiharu Tokoro","email":"","orcid":"","institution":"Waseda University","correspondingAuthor":false,"prefix":"","firstName":"Chiharu","middleName":"","lastName":"Tokoro","suffix":""},{"id":287163949,"identity":"e4d157c0-05e2-4a1e-a6a0-37d9ab8d41c2","order_by":3,"name":"Yasunori Kikuchi","email":"","orcid":"","institution":"University of Tokyo","correspondingAuthor":false,"prefix":"","firstName":"Yasunori","middleName":"","lastName":"Kikuchi","suffix":""}],"badges":[],"createdAt":"2024-04-03 14:41:16","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4213507/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4213507/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":54162633,"identity":"202e00ea-d8c9-4ecd-b351-d828092c4256","added_by":"auto","created_at":"2024-04-05 13:10:48","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":146974,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSystem definition of the assumed life cycle of automotive LIBs in Japan.\u003c/strong\u003e Cases 1, 2, 3 and 4 represent four technical routes to dispose of spent automotive LIBs; Cases a and b represent the policy options of immediately recycling and recycling after secondary usage, respectively; the detailed definitions are described in the Methods section.\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-4213507/v1/1807f5f8b003e752ee862359.png"},{"id":54162632,"identity":"e1dbdb7f-8735-4c59-934d-4b556c9cde09","added_by":"auto","created_at":"2024-04-05 13:10:47","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":130701,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eThe annual stocks and flows of critical metals relating to automotive LIBs in Japan. a, b: \u003c/strong\u003ecritical metals in use, \u003cstrong\u003ec, d\u003c/strong\u003e: critical metals recycled and input in LIB manufacture, \u003cstrong\u003ee, f\u003c/strong\u003e: critical metals newly input in LIB manufacture. Figures a, c and e belong to the case of immediately recycling, while Figures b, d and f belong to the case of recycling after secondary use. NCA: lithium nickel cobalt aluminium oxide, NMC: lithium nickel manganese cobalt oxide.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-4213507/v1/a1f2105af7e581fc3288313e.png"},{"id":54162630,"identity":"788e156d-886c-4163-8623-7d16b7d32080","added_by":"auto","created_at":"2024-04-05 13:10:47","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":108083,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eThe changes in life-cycle GHG emissions and RCP of automotive LIBs in scenarios. a\u003c/strong\u003e: annual life-cycle GHG emissions, \u003cstrong\u003eb\u003c/strong\u003e: annual life-cycle RCP, \u003cstrong\u003ec\u003c/strong\u003e: accumulated GHG emissions during 2025–2050, \u003cstrong\u003ed\u003c/strong\u003e: accumulated RCP during 2025–2050.\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-4213507/v1/3b25a2ac4250ca279d79ad7e.png"},{"id":54162634,"identity":"c576660d-ba05-40ca-a3a3-7ecade274aee","added_by":"auto","created_at":"2024-04-05 13:10:48","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":71056,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eThe critical metals input in LIB manufacture and the changes in overall circulation rate.\u003c/strong\u003e In the case of immediately recycling (\u003cstrong\u003ea\u003c/strong\u003e) and the case of recycling after secondary use (\u003cstrong\u003eb\u003c/strong\u003e).\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-4213507/v1/a092a8f242e778efa17d4668.png"},{"id":54416162,"identity":"b6392665-765b-4cf7-bc2b-a27a8af1c864","added_by":"auto","created_at":"2024-04-10 07:03:43","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":772148,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4213507/v1/aced5f6e-21d2-4522-b1cc-79a0736f2f6e.pdf"},{"id":54162635,"identity":"1f71d4c8-e421-4b22-b18a-be89287d46c1","added_by":"auto","created_at":"2024-04-05 13:10:48","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":1082227,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cbr\u003e\u003c/p\u003e","description":"","filename":"Supplementaryinformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-4213507/v1/d400e75e5a5133d18cb838d3.docx"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Novel precise separation technology will significantly improve the circulation of critical metals in automotive lithium-ion batteries","fulltext":[{"header":"Introduction","content":"\u003cp\u003eBecause of global e-mobility ambitions, rapidly expanding electric vehicle fleets (EVs) worldwide require a huge capacity of automotive batteries, which cannot avoid demanding massive amounts of critical metals, such as cobalt\u003csup\u003e1\u003c/sup\u003e, lithium\u003csup\u003e2\u003c/sup\u003e, nickel and manganese\u003csup\u003e3\u003c/sup\u003e. Battery technology and recycling advancement are widely acknowledged as two must-have strategies, where recycling progress is expected to support a sufficient secondary supply of minerals to relieve the resource shortage in the medium to long term\u003csup\u003e4\u003c/sup\u003e. With the addition of the regional disparity in resource endowment, major economies, particularly the European Union and Japan, must face serious challenges in resource security while rushing to realize a decarbonized society\u003csup\u003e5\u003c/sup\u003e. The implementation of the EU Sustainable Batteries Regulation\u003csup\u003e6\u003c/sup\u003e, as\u0026nbsp;an iconic event, suggests that recycling batteries has become an obligation despite many current recycling projects not being economically beneficial\u003csup\u003e7\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003eFor decades, researchers worldwide have tried to determine an ultimate solution to recycle spent automotive lithium-ion batteries (LIBs), while huge investments have been made for scaled-up demonstration projects. Beyond various technologies remaining at a laboratory level, extractive metallurgical processes, including pyrometallurgy and hydrometallurgy, have become common industrial techniques in recycling critical metals from spent automotive LIBs\u003csup\u003e8\u003c/sup\u003e. Pyrometallurgy can treat batteries in a wide range of types and\u0026nbsp;constitutions, using heating to convert the metal oxides into metal alloys containing Co and Ni, while Li and Al remain in the slags\u003csup\u003e9\u003c/sup\u003e. This method is easy to scale up with less material input and additional waste disposal, but it consumes a large amount of energy in combustion and calcination while incurring a large capital cost\u003csup\u003e10\u003c/sup\u003e. By contrast, hydrometallurgy uses added reagents and solvents to extract and separate metals from spent automotive LIBs\u003csup\u003e11\u003c/sup\u003e. It enables a high-quality recovery of critical metals, with low energy consumption, gas emissions and capital cost, but spends a long time in processing and brings about added material consumption and wastewater treatment. Despite demonstration projects revealing that the optimized combination of pyrometallurgy and hydrometallurgy can flexibly deal with various types of spent automotive LIBs while maximizing the recovery rate of critical metals on a large scale, these processes do not significantly reduce economic costs and environmental burdens that can only be reduced in the case of directly recycling the cathode materials\u003csup\u003e12\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003eDirect recycling is supported by advanced disassembly and separation technologies, which have been of increasing interest in recent years\u003csup\u003e13\u003c/sup\u003e. Optimized manual disassembly and automatic disassembly have both been considered as possible ways of dismantling batteries to their individual electrodes with up to 90% savings in processing time and cost\u003csup\u003e14\u003c/sup\u003e. A delamination process follows disassembly, such as soaking in ethylene glycol\u003csup\u003e15\u003c/sup\u003e, Cyrene and other solvents\u003csup\u003e16\u003c/sup\u003e, to completely separate the cathode materials from the Al foil. In principle, the recycled cathode materials can be regenerated or reincorporated into a new cathode electrode\u003csup\u003e17\u003c/sup\u003e. Currently, these technologies are still far from practical application, suffering from difficulties in satisfying the quality of recycled materials for remanufacturing, dealing with various types and structures of batteries, and reducing labour costs in disassembly\u003csup\u003e18\u003c/sup\u003e. In summary, despite commercial projects usually adopting pyrometallurgy and hydrometallurgy to recycle spent automotive LIBs because of good performance on scaling up, future improvements in economic and environmental performance are likely to be obtained from direct recycling that realizes a shorter circular route.\u003c/p\u003e\n\u003cp\u003eBeyond the techniques well introduced in previous studies, the general application of precise separation technologies for composite materials, such as microwave processing\u003csup\u003e19\u003c/sup\u003e and ultrasonication\u003csup\u003e20\u003c/sup\u003e, was insufficiently assessed in recycling spent LIBs; in particular, the economic and environmental impacts were less understood. A precise separation technique is first developed to pretreat the dismantled battery cells for the following metal recovery by hydrometallurgy, but it has the potential to directly recycle the positive electrode active materials (PEAMs) if the separation is precise enough to extract and retain the properties of recovered PEAMs (Supplementary Fig. S1). Recently, an expectable precise separation method, named high-voltage pulsed discharge, that has attracted attention was proved feasible in quickly and precisely separating the PEAMs from the Al foil using a fine-tuned single pulsed power without heating and additives (Supplementary Fig. S2). The concentration of Al in the recovered PEAMs was reduced to 2.95%, while almost 99% of the recovered PEAMs retained the original chemical properties, which can be incorporated in LIB manufacture after a resynthesis process\u003csup\u003e21\u003c/sup\u003e. According to the purity, the recycled PEAMs can be reincorporated in new production through a direct recycling process, or otherwise sent to the hydrometallurgical process for metal recovery as an easy pretreatment. In both cases, life-cycle assessment (LCA) indicated possible significant reductions in greenhouse gas (GHG) emissions and resource consumption potential (RCP) compared with the conventional processing by pyrometallurgy and hydrometallurgy after scale-up mainly because of the much smaller input of energy and chemicals\u003csup\u003e20\u003c/sup\u003e. From a systemic and dynamic perspective, we need to understand the flexibility (uncertain positioning) of applying precise separation techniques and the extent to which such a precise separation technology will contribute to the performance of the recycling system, particularly considering its flexible positioning in system design and the co-ordination with resource and energy policies.\u003c/p\u003e\n\u003cp\u003eHere, we aim to estimate the future changes in GHG emissions and RCP in the case of applying a high-voltage pulsed discharge method for a complete circulation of PEAMs compared with the cases in conventional technology combination and system design by combining dynamic material flow analysis (MFA) and prospective LCA (see model framework in Fig. 1 and details under Methods). The case area we chose is Japan because Japan is experiencing an energy and resource shortage, where the battery and automotive industries are rushing to promote the transition towards EVs, but a recycling system for spent automotive LIBs has not been finally established. The discussion using Japan as a case will have more flexibility in applicability than using the first movers and be referential to the late movers. First, through a yearly dynamic simulation of the changes in Japan’s automotive market and the material flow of automotive LIBs, we evaluate how the automotive LIB market may rely on the precise separation for PEAMs and analyse the feasibility and challenges of applying the high-voltage pulsed discharge method as a case from the systemic perspective. Then, through prospective LCA, we estimate the overall impacts of applying precise separation technology in the system on the annual GHG emissions and RCP, assuming the realization of a total decarbonization by 2050 in Japan. Here, we set scenarios considering three factors: the positioning of precise separation, the secondary usage or not of the spent LIBs and any future battery model changes. Finally, we compare the results with the cases using conventional technologies combining hydrometallurgy and pyrometallurgy and combustion with landfill. Because the application of precise separation technology was indicated to have great potential in improving the eco-efficiency of recycling systems, we further comment on the opportunities and challenges for actual technology diffusion.\u003c/p\u003e"},{"header":"Results","content":"\u003cp\u003eCapacity required for recycling spent automotive LIBs\u003c/p\u003e\n\u003cp\u003eThe life cycle of an automotive LIBs includes their production, primary use in EVs, secondary use in stationary energy storage, collection and recycling (Fig. \u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003e). As shown in Fig. \u003cspan class=\"InternalRef\"\u003e2\u003c/span\u003e, both the annual stocks and flows of critical metals in automotive LIBs will keep rapidly increasing in Japan during 2025\u0026ndash;2050. The critical metals in use were estimated to reach 2,128 kt-LiNiCoMn (the total weight of Li, Ni, Co, Mn included in automotive LIBs) by 2050 in the case of recycling immediately, of which the number can increase to 2,679 kt-LiNiCoMn in the case of recycling after secondary usage because of the degradation of spent LIBs used for energy storage. Forcing the spent LIBs to secondary use slows down the circulation of critical metals for several years, leading to an increased annual critical metals input of 40 kt-LiNiCoMn (50% increase) in manufacturing automotive LIBs after 2035. Furthermore, the penetration of new battery models such as NMC811 and NMC955 will also be decreased. In both cases, the peak quantity of critical metals newly input in LIB manufacture appears at around 2040, but the first year of reaching the peak will be 10 years earlier in the case of immediate recycling.\u003c/p\u003e\n\u003cp\u003eAccording to the MFA result, precise separation indicates its ability to deal with the rapidly increasing amount of spent LIBs. One such method is the high-voltage pulsed discharge method, where one high-voltage pulsed discharge will spend 10 seconds on a batch treatment of a positive electrode (PE) sheet that is around 72.45 grams. If the equipment operates 8 hours/day and 245 days/year, the treatment capacity will be 51.12 t-PE sheets annually; otherwise, the capacity can increase by 4.5 times if automatically operating 24 hours/day and 365 days/year. In the case of immediate recycling, 2,800\u0026ndash;12,500 bases of high-voltage pulsed discharge equipment should be in operation by 2050. Considering that in Japan there were around 3,000 car dismantlers recorded in operation in 2022\u003csup\u003e22\u003c/sup\u003e, it is expected that a few items of precise separation equipment will be installed initially to conduct the separation of PEAMs. This substantially reduces the dependence on pyro/hydrometallurgy and can avoid excess transport as part of safety risks and environmental impacts.\u003c/p\u003e\n\u003cp\u003eEnvironmental impact of applying precise separation in recycling spent automotive LIBs\u003c/p\u003e\n\u003cp\u003eThe development and application of precise separation technology play a critical role in improving the eco-efficiency of recycling spent automotive LIBs, but the potential improvement should have a synergy or trade-off with the technology combination and energy policy. We defined four kinds of technology combinations focusing on the positioning of the precise separation, with two energy policies such as immediate recycling of the PEAMs or recycling after secondary use (see Table\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e1\u003c/span\u003e in the \u003cspan class=\"InternalRef\"\u003eMethods\u003c/span\u003e section). As shown in Fig.\u0026nbsp;\u003cspan class=\"InternalRef\"\u003e3\u003c/span\u003e, the life-cycle GHG emissions relating to automotive LIBs would finally decrease from 2040 if the decarbonization strategies were strictly implemented, but the RCP would keep increasing. Among the scenarios, direct recycling of PEAMs by precise separation (a-4, b-4) led to the overall lowest environmental and resource impacts. This is because of the obvious environmental benefit of substituting raw PEAM products. During 2025\u0026ndash;2050, a maximum of around half of the accumulated GHG emissions and RCP can be reduced compared with the cases of incineration and landfill (a-1, b-1). The scenario results indicate the secondary use of spent LIBs can to some extent suppress the environmental impact because the policy delayed the recycling processes, remanufacturing and new production towards the era of decarbonization. Thus, if manufacturers failed to directly recycle the PEAMs by precise separation, the better choice is to secondarily use the spent LIBs; however, it is better to apply the precise separation techniques for immediate and direct recycling. Of course, we need to consider secondary use, which the the user may value more, and not ignore the problem in life-cycle RCP because of various technology combinations beyond decarbonization.\u003c/p\u003e\n\u003cp\u003e\u003cimg 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\"\u003e\u003c/p\u003e\n\u003cdiv class=\"gridtable\"\u003e\n \u003cdiv align=\"left\" class=\"colspec\"\u003e\u003cbr\u003e\u003c/div\u003e\n \u003cdiv align=\"left\" class=\"colspec\"\u003eAnother crucial indicator, circulation rate, was significantly changeable in response to the decision on secondary use (as shown in Fig. \u003cspan class=\"InternalRef\"\u003e4\u003c/span\u003e). During 2025\u0026ndash;2050, Ni would be the resource with the greatest demand, and then Co, Li and Mn. Although secondary use of spent LIBs can reduce the annual input of critical metals in automotive LIBs manufacturing and remanufacturing by about 15%, it also greatly suppresses the circulation rate of critical metals by around 20% compared with the case of immediate recycling. In other words, the lower the circulation rate, the more Japan will need to import critical metals from overseas. Immediate recycling of the PEAMs would support a high circulation rate of critical metals and help in expanding the size of the domestic recycling market. Given the future projection prices of Li, Ni, Co and Mn as USD/t 14,000, 40,000, 100,000\u003csup\u003e23\u003c/sup\u003e and 4,000 (2020\u0026rsquo;s level doubled)\u003csup\u003e24\u003c/sup\u003e by 2050, in the case of immediate recycling, the annual market value of the four metals in Japan may reach USD 11 billion by 2050, in which circulated metals would have a market value of USD 9 billion. If directly recycling the PEAMs was finally diffused, circulated PEAMs may have a revenue of about USD 16 billion by 2050 (60 USD/kWh; cathode cost doubled from 2020\u0026rsquo;s level)\u003csup\u003e25\u003c/sup\u003e. Considering the probable synchronization with the EU Sustainable Batteries Regulation, immediately recycling the spent LIBs should contribute the most to achieving the minimum levels of cathode materials recovery in Japan, where directly recycling the PEAMs supported by novel precise separation should be the best approach for environmental and resource conservation. Being a large metal resource importer, a timely increasing of the circulation rate in Japan should ease the mismatch between the supply and demand of critical metals and enhance resource security and supply chain resilience as much as possible.\u003c/div\u003e\n\u003c/div\u003e"},{"header":"Discussion","content":"\u003cp\u003eUsing the high-voltage pulsed discharge method as a case, our analysis indicated the penetration of such precise separation techniques in recycling the spent automotive LIBs is basically feasible and can significantly reduce the environmental impact and additional resource consumption. In particular, the results could suggest the expected technology features and the roadmap to implement such technologies. First, an expected precise separation technology may not perform perfectly in directly recycling the cathode materials but should at least perform well as a pretreatment process. Here, good performance means a physical approach that is generally applicable, may only use electricity, should consume significantly less energy and solvents, and avoid the following treatment of emitted gases and wastewater that yield additional environmental burden and economic cost (Supplementary Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e). For instance, the high-voltage pulsed discharge method is also applicable to physically separating silver and copper wires from spent solar panels\u003csup\u003e26\u003c/sup\u003e with a designed system, potentially reducing by 17% life-cycle GHG emissions and in total saving input resources\u003csup\u003e27\u003c/sup\u003e. Recent experiments furthermore revealed the method can be applied to separate laminated carbon fibre\u0026ndash;reinforced plastic composites\u003csup\u003e28\u003c/sup\u003e. Yet, as a roadmap, such a precise separation technique can be penetrated in three stages: Stage 1, incorporating the technique as a pretreatment process to reduce the dependency on pyrometallurgy and hydrometallurgy; Stage 2, further developing the technique with a specific design of products towards the direct recycling of PEAMs; and Stage 3, encouraging faster recycling of the spent LIBs to speed up the circulation of critical metals.\u003c/p\u003e \u003cp\u003eBeyond our assumptions and simulation, a few opportunities and challenges have significant influences on the assessment results. The opportunities include the following. First, removing the Al in advance will greatly help us to more efficiently and ecologically recover the Li from the cathode materials\u003csup\u003e29\u003c/sup\u003e if combined with the appropriate method\u003csup\u003e30\u003c/sup\u003e. Second, the precise separation techniques should be also applicable in recycling the batteries from electric two-wheelers, electric bicycles and electric trucks\u003csup\u003e21\u003c/sup\u003e, leading to a much larger market than our evaluation (Supplementary Fig. S3). Third, the penetration of such precise separation techniques will support a further eco-design and standardization of batteries. In fact, the key to an efficient precise separation is in the design of adhesives\u003csup\u003e31\u003c/sup\u003e. In the case of using high-voltage pulsed discharge, filling a metal sphere\u003csup\u003e32\u003c/sup\u003e or a small proportion of carbon black\u003csup\u003e33\u003c/sup\u003e in the adhesives can concentrate the pulsed power to easily destroy the adhesion, supporting a better performance of the separation in an air environment compared with the separation in a water pool\u003csup\u003e34\u003c/sup\u003e (avoiding wastewater treatment). Of course, the overall structure of the battery should be designed for disassembly to save labour costs in competing with pyrometallurgy\u003csup\u003e35\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eHowever, several challenges and uncertainties may influence the application of precise separation techniques. First, despite experiments of high-voltage pulsed discharge indicating 93.9% of the PEAMs can be recovered and that almost 99% of them can be used in LIB manufacture\u003csup\u003e21\u003c/sup\u003e, this result must be retained and improved on an industrial scale. Second, the time and cost of beforehand disassembly will be a bottleneck when applying the precise separation technique, and a corresponding design of automatic disassembly based on industrial robots is indispensable\u003csup\u003e36\u003c/sup\u003e. Third, in our simulation, all the recovered PEAMs can be reused for new battery manufacture because the capacity requirement for automobiles is increasing rapidly, despite the continuous improvements in battery models. If the penetration of EVs is unexpectedly slow or the battery model changes extremely quickly, directly recycled PEAMs still have to be recovered as metal elements for next-generation battery manufacture. Fourth, the capacity of spent automotive LIBs may greatly overstep the capacity required for stationary energy storage. This study revealed that spent LIBs that are in secondary usage would gradually increase to 400 GWh by 2050 (see Supplementary Fig. S11), assuming the maximum proportion in automotive LIB capacity is 25%, as projected by the International Renewable Energy Agency\u003csup\u003e37\u003c/sup\u003e. This proportion may further decrease considering the possible impact of vehicle\u0026ndash;grid integration\u003csup\u003e38\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eThe penetration of precise separation techniques will also bring about a positive influence on the distribution of the recycling system networks for spent LIBs. The costs of collecting and transporting spent LIBs can make up 5\u0026ndash;70% of the total costs for recycling\u003csup\u003e39\u003c/sup\u003e because the current production and recycling locations are concentrated\u003csup\u003e40\u003c/sup\u003e and because collecting and transporting LIBs needs a dedicated area that includes a large buffer zone and risk insurance to protect from frequent fires and explosions\u003csup\u003e41\u003c/sup\u003e. Here, the application of the precise separation after battery collection can start from a small capacity, while the outputs (Al and PEAMs) are safe and high purity. It also surely reduces the need for long-distance transportation and the safety risks associated with the transport to decrease the environmental impacts and economic costs. In particular, the recovered PEAMs do not need a pyrometallurgy process thereby avoiding a large investment in facilities and equipment. It is expected that precise separation techniques will be applied in developing a vertically integrated, in-country local recycling chain to secure the supply chain for critical metals.\u003c/p\u003e \u003cp\u003eHaving the whole world in view, wide management of critical metals should be conducted in automobile industries. Historically, Japan annually exports new and second-hand vehicles to the rest of the world, equalling one-fourth of the domestic car sales\u003csup\u003e42\u003c/sup\u003e. In contrast, the market share of automotive LIB production by Japanese companies has decreased from 51.7% in 2015 to 21.1% in 2020\u003csup\u003e43\u003c/sup\u003e. Moreover, the major countries in the European Union have strengthened the regulation on the flow of automotive LIBs and related critical metals, such as the need to label the metals\u0026rsquo; recovery rate and carbon footprints of products\u003csup\u003e44\u003c/sup\u003e. Near Japan, both China and Korea have invested in recycling automotive LIBs\u003csup\u003e45\u003c/sup\u003e, and the costs of recycling spent LIBs in China are significantly lower than in the United Kingdom, the United States and South Korea\u003csup\u003e46\u003c/sup\u003e. To balance the resource demand and supply, of course, Japan could initiate international cooperation on establishing a wide-area circulation. In contrast, the application of precise separation may support another option to first extract the PEAMs, followed by the metal refining process using domestic facilities. Such a practice will surely provide knowledge and experience to other late movers that have declared their e-mobility ambitions.\u003c/p\u003e \u003cp\u003eIn summary, we strongly recommend trying to use the emerging precise separation techniques for pretreating or directly recycling the active materials in spent LIBs and faster recycling the critical metals with the help of the eco-design for easy dismantling. Combined efforts in technology, regulatory, trading, and economic areas should make the best contributions to this issue. Although our primary study was limited in domestic boundary and rough simulation because of the lack of data and various uncertainties, we believe our scenario results have provided robust conclusions about the synergy and trade-off between the targets on the e-mobility emotion, GHG emissions, resource security, circulation rate and financial balance regarding the development of the automotive LIB industry, where novel precise separation techniques were indicated to support the best solution.\u003c/p\u003e"},{"header":"Methods","content":"\u003cp\u003eDefinitions and system boundary\u003c/p\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, the stocks and flows of PEAMs in the automotive market, which contains the critical metals Li, Co, Ni and Mn, were considered totally circulated domestically in Japan through an assumption of a 100% recycling rate. These critical metals were thought to only come from overseas mining and extraction (primary supply) and domestic recycling and recovery (secondary supply). The spent LIBs were directly sent to the recycling system or used as stationary batteries for energy storage, with no export or other diversion. Here, the vehicle fleets defined in this study included passenger cars but excluded buses and trucks because of the strong competition from the fuel cell vehicle industry. Also, the LIBs included the ones served in battery electric vehicles (BEVs) and plug-in hybrid electric vehicles (PHEVs). In the boundary of LCA, the remaining parts of LIBs were considered to be newly manufactured in all scenarios, and the material losses (not caused by technical defects) in mining, extraction, manufacturing and recycling were not considered. The energy storage market was assumed to unconditionally accept the spent LIBs if the policy promoted this, of which the capacity would not exceed the market projection of stationary energy storage.\u003c/p\u003e \u003cp\u003eHistorical changes in the stocks and flows of critical metals\u003c/p\u003e \u003cp\u003eAssuming the precise separation using a high-voltage pulsed discharge method will be applied from 2025, a dynamic MFA approach\u003csup\u003e47\u003c/sup\u003e was developed to quantify the cycle of critical metals from 2025 to 2050. The approach was annually iterated to simulate the changes in the passenger car market, lifetime use of vehicles and LIBs, secondary use, and recycling of spent LIBs, as usually applied\u003csup\u003e48\u003c/sup\u003e. First, the passenger car ownership per household \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(C\\)\u003c/span\u003e\u003c/span\u003e was calculated as shown below:\u003cdiv id=\"Equ1\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ1\" name=\"EquationSource\"\u003e\n$$C=\\frac{N\u0026middot;\\gamma \u0026middot;(1-\\eta \u0026middot;\\delta )}{1+\\alpha \u0026middot;\\text{e}\\text{x}\\text{p}(-\\beta \u0026middot;\\frac{\\stackrel{-}{I}}{\\stackrel{-}{P}})}$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e1\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003ewhere \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(N\u0026middot;\\gamma \u0026middot;(1-\\eta \u0026middot;\\delta )\\)\u003c/span\u003e\u003c/span\u003e represents the potential passenger car market, negatively affected by the multiple of average annual income per household \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\stackrel{-}{I}\\)\u003c/span\u003e\u003c/span\u003e and average purchase price per vehicle \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\stackrel{-}{P}\\)\u003c/span\u003e\u003c/span\u003e. \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(N\\)\u003c/span\u003e\u003c/span\u003e is the number of households in Japan, \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\eta\\)\u003c/span\u003e\u003c/span\u003e is the rate of membership of car sharing, and \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\delta\\)\u003c/span\u003e\u003c/span\u003e is the decrease rate of car ownership by car sharing\u003csup\u003e49\u003c/sup\u003e. Parameters \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\alpha\\)\u003c/span\u003e\u003c/span\u003e and \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\beta\\)\u003c/span\u003e\u003c/span\u003e were set as 10.5 and 0.791\u003csup\u003e50\u003c/sup\u003e, respectively. Parameter \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\gamma\\)\u003c/span\u003e\u003c/span\u003e was estimated as 0.000757 by the average fitted value because of the passenger car ownership rate during 2015\u0026ndash;2020. The results showed that the ownership of passenger cars would gradually decrease from 61\u0026nbsp;million to 46\u0026nbsp;million during 2020\u0026ndash;2050 mainly because of the decrease in population (Supplementary Fig. S3, S5).\u003c/p\u003e \u003cp\u003eThen, according to the ambitious targets carried out by the Japanese government and automotive associations, the sales of internal combustion engine vehicles will be stopped domestically by the early 2030s, while the transport sector should be decarbonized by 2050\u003csup\u003e51\u003c/sup\u003e. Thus, we assumed that the ICEs will gradually quit the new sales market by 2035 and that the HEVs will gradually quit the new sales market by 2050, as shown in Supplementary Fig. S6. The scenario result (Supplementary Fig. S7) based on the assumption was close to the scenario \u0026lsquo;BEV75\u0026rsquo; estimated by the Japan Automobile Manufacturers Association\u003csup\u003e52\u003c/sup\u003e. Regarding the projection of battery model changes, we referred to the high-probability scenario (named \u0026lsquo;NCX\u0026rsquo;) established by Xu et al.\u003csup\u003e3\u003c/sup\u003e (Supplementary Fig. S8). The battery producers were assumed to replace Co with Ni-rich PEAMs to reduce costs. Thus, the battery model NMC111 will gradually change to NMC523, NMC622, NMC811 and NMC955. The NCX scenario proposed that although lithium iron phosphate (LFP) has advantages in technology readiness, costs and resource availability and lithium\u0026ndash;sulphur (Li\u0026ndash;S) and lithium\u0026ndash;air (Li\u0026ndash;Air) batteries have specific energy densities three times greater than NMC LIBs, they are more difficult to use than NMC LIBs because of the low specific energy of LFP and low technology readiness of Li\u0026ndash;S/Li\u0026ndash;Air batteries.\u003c/p\u003e \u003cp\u003eIn 2023, the sales of BEVs and PHEVs were only 3.6% of the passenger car market\u003csup\u003e53\u003c/sup\u003e. The timing of collecting spent LIBs can affect both the lifespan of EVs and the service life of automotive LIBs in EVs (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e). To estimate the lifespan of vehicles, we conducted the following Weibull distribution equation:\u003cdiv id=\"Equ2\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equ2\" name=\"EquationSource\"\u003e\n$$F\\left(t\\right)=1-{e}^{-{\\left(\\frac{t}{}\\right)}^{m}}$$\u003c/div\u003e\u003cdiv class=\"EquationNumber\"\u003e2\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003ewhere \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(F\\left(t\\right)\\)\u003c/span\u003e\u003c/span\u003e is the survival rate of a vehicle when it services \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(t\\)\u003c/span\u003e\u003c/span\u003e years. Parameters \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(m\\)\u003c/span\u003e\u003c/span\u003e and \u003cem\u003e\u0026micro;\u003c/em\u003e are calibrated as 2.69 and 15.49, respectively, according to the age distribution of existing passenger cars surveyed in 2019\u003csup\u003e54\u003c/sup\u003e (Supplementary Fig. S9, S10). For easier dynamic simulation, we assumed all types of passenger cars have the same survival rate and that the lifespan does not extend yearly because of the launch of new cars. The lifespan of automotive LIBs was set as 8 years, and the lifespan of spent LIBs for secondary usage in stationary energy storage was set as 10 years, referred to in many studies such as those by Hara\u003csup\u003e55\u003c/sup\u003e and Zeng et al.\u003csup\u003e5\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eProspective LCA and scenarios setting\u003c/p\u003e \u003cp\u003eBased on the scaled-up experiment of the high-voltage pulsed discharge method applied to separate the PEAMs\u003csup\u003e56\u003c/sup\u003e, we conducted a prospective LCA approach\u003csup\u003e57\u003c/sup\u003e to quantify the possible environmental impact of applying precise separation to recycle PEAMs while considering the uncertainty in evaluating such an emerging technology\u003csup\u003e58\u003c/sup\u003e. We set eight scenarios to simulate the different situations considering four technology combinations (landfill after incineration, pyrometallurgy and hydrometallurgy combination, hydrometallurgy after precise separation, or direct recycling after precise separation) and two choices in the timing of recycling spent LIBs (immediate recycling, or recycling after secondary use) (see Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e).\u003c/p\u003e \u003cp\u003eTable\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e summarizes the details of processes considered in the cases defined in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. In Cases a-1 and b-1, spent LIBs are incinerated and landfilled without metal resources recycling. In Cases a-2 and b-2, spent LIBs are first disassembled into cells that are then roasted and smelted for metal recovery. In Cases a-3 and b-3, spent LIBs are disassembled into cells in which the PEAMs are then separated by high-voltage pulsed discharge for metal recovery. In Cases a-4 and b-4, the PEAMs are separated by high-voltage pulsed discharge and directly incorporated for new automotive LIBs production.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab2\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 2\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eProduction and recycling processes defined in cases\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"5\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eProcesses in cases in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCase a-1, b-1\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eCase a-2, b-2\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eCase a-3, b-3\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003eCase a-4, b-4\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eMining and extraction\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eM-SO\u003csub\u003e4\u003c/sub\u003e production\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRaw PEAM production\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePEAM production\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBattery production\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eUse in vehicle\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eCollection/dismantling\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eIncineration\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eLandfilling\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBattery pack dismantling\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRoasting\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eSmelting\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e\u0026nbsp;\u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBattery cell dismantling\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePulsed discharging\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRecycling of metal resources\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e\u0026nbsp;\u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c5\"\u003e \u003cp\u003e〇\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eBased on the scaled-up analysis in the previous study\u003csup\u003e56\u003c/sup\u003e, we further considered the annual changes in impact assessment in the target of realizing a carbon neutral society by 2050\u003csup\u003e59\u003c/sup\u003e. In the fiscal year 2022, grid electricity used in Japan emitted 0.435 kg-CO\u003csub\u003e2\u003c/sub\u003e/kWh\u003csup\u003e60\u003c/sup\u003e on average, which will be reduced to 0.25 kg-CO\u003csub\u003e2\u003c/sub\u003e/kWh by 2030 and net zero by 2050 because of the official projection of energy demand and supply\u003csup\u003e61\u003c/sup\u003e. Excluding incineration and landfilling, pyrometallurgy, hydrometallurgy, dismantling, separation, and other processes will be gradually decarbonized by 2050. However, while decarbonization may bring about more resource consumption\u003csup\u003e62\u003c/sup\u003e, optimistically, we assumed the following technological innovation can suppress this additional resource consumption (Supplementary Table S8). Regarding the lack of data for LCA on different types/sizes of automotive LIBs, we assumed the intensity of GHG emissions and resource consumption potential is proportional to the weight of PEAMs in a standard LIB pack (per vehicle). Accordingly, the LCA on LFP, Li\u0026ndash;S, and Li\u0026ndash;Air battery production and recycling as well as the secondary use of spent LIBs was out of the scope of this work.\u003c/p\u003e \u003cp\u003eLimitations and uncertainties\u003c/p\u003e \u003cp\u003eApplying an integrated model, our simulation and scenario analysis build on various assumptions and parameters that cannot avoid correlated limitations and uncertainties (Table\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e). First, the EV market and stationary energy storage market in Japan may not optimistically follow the government\u0026rsquo;s ambition and institutional projections. A lower popularization rate of EVs and LIBs will de-level the simulation and analysis results in our study. Here we tested the influence on critical metals\u0026rsquo; circulation if the energy storage market does not accept spent LIBs or is infinite to accept them (Supplementary Fig. S13). Second, the lifespan of passenger cars and automotive LIBs was fixed, but it may gradually extend in the future. Of course, compared with our simulation, the recycling of spent LIBs will slow down and the annual production of LIBs will increase in proportion. Third, the battery capacity required for EVs was assumed to be fixed in the future as the reference set\u003csup\u003e3\u003c/sup\u003e (Supplementary Table S5). Although the capacity for one EV will increase in the future, the increment of energy intensity in the new battery model will increase to offset the capacity requirement. Fourth, the collection rate of spent LIBs and the actual recycling rate were set as 100% for easier simulation. In the near future, all the automotive LIBs may have their own codes in the tracking system, while the recycling rate may approach 100%\u003csup\u003e63\u003c/sup\u003e. As a sensitivity analysis, the collection rate was found to mainly affect Cases a-1 and b-1 in terms of life-cycle GHG emissions and affect Cases a-4 and b-4 in terms of potential resource consumption because of the obvious differences in parameter on circulation and resource consumption potential (Supplementary Figs S14, S15; Supplementary Tables S9, S10). Fifth, the battery models such as LFP, Li\u0026ndash;S and Li\u0026ndash;Air were not considered because of the scenario adopted from Xu et al.\u003csup\u003e3\u003c/sup\u003e. In fact, all-solid-state batteries have advantages in application to light-duty EVs, while LFP will have a large share in heavy-duty EVs and stationary energy storage\u003csup\u003e64\u003c/sup\u003e. In the long term, various batteries will share the market, for which we need to verify the performance of precise separation considering different structures in the cathode active materials\u003csup\u003e65\u003c/sup\u003e. Sixth, in LCA, we set NMC111 as the reference standard\u003csup\u003e56\u003c/sup\u003e and conducted a sensitivity analysis accordingly\u003csup\u003e56\u003c/sup\u003e. An LCA study in China showed that the LFP battery, NMC battery and LMO battery (28 kWh) would produce GHG emissions in the production of 3,061 kg CO\u003csub\u003e2\u003c/sub\u003e-eq, 2,912 kg CO\u003csub\u003e2\u003c/sub\u003e-eq and 2,705 kg CO\u003csub\u003e2\u003c/sub\u003e-eq, respectively\u003csup\u003e66\u003c/sup\u003e; in addition, these results vary across countries\u003csup\u003e67\u003c/sup\u003e. Seventh, transport distance and volume were fixed in LCA, but it could be quite reduced because of the application of precise separation.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab3\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 3\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003eDescription and assumption of key model parameters\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"3\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eKey parameters\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eDescription/assumptions\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eDetails\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003ePassenger car ownership\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003ePassenger car ownership is assumed to be affected by population\u003csup\u003e68\u003c/sup\u003e, the number of households\u003csup\u003e69\u003c/sup\u003e, annual income per household, consumer price of vehicles\u003csup\u003e62\u003c/sup\u003e, and the participation of car sharing\u003csup\u003e49\u003c/sup\u003e. Road infrastructure, public traffic systems, and urban shape are considered fixed parameters. The import and export of passenger cars are out of the scope of this paper.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Tables S1, S2\u003c/p\u003e \u003cp\u003eSupplementary Figs S3\u0026ndash;5, S9\u0026ndash;11\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eEV market share\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThe EV market share is assumed to increase according to the Carbon Neutral Target declared in Japan\u003csup\u003e59\u003c/sup\u003e. The sales of internal-combustion engine vehicles will be stopped from the year 2035, and the proportion of EVs (almost BEVs) in new car sales linearly increases to 90% by 2050, while the proportion of Fuel cell vehicles reaches 10%\u003csup\u003e52\u003c/sup\u003e. The service life of vehicles is assumed to remain the same as in 2019\u003csup\u003e70\u003c/sup\u003e.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Tables S3, S4\u003c/p\u003e \u003cp\u003eSupplementary Figs S6, S7\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBattery capacity of BEV/PHEV\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThe battery capacity for BEVs and PHEVs is set as the sales-weighted average based on the projection of small, mid-size, and large car fleets\u003csup\u003e3\u003c/sup\u003e.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Table S5\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eStationary energy storage market\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThe capacity of the stationary energy storage market is set not to surpass 25% of the capacity of automotive LIBs in use in EVs\u003csup\u003e37\u003c/sup\u003e.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Table S13\u003c/p\u003e \u003cp\u003eSupplementary Fig. S12\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBattery lifetime\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThe lifetimes of automotive LIBs in use in EVs and stationary energy storage are assumed to be 8 and 10 years, respectively\u003csup\u003e3,5\u003c/sup\u003e.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Table S6\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eBattery model changes\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThe model change of the automotive batteries in Japan is assumed to keep the same path of the worldwide market, following the \u0026lsquo;NCX\u0026rsquo; scenario of Xu et al.\u003csup\u003e3\u003c/sup\u003e.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Fig. S8\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRecycling rate and residual loss\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThe collection rate of spent automotive LIBs is assumed to be always 100% during 2025\u0026ndash;2050. The weight of critical metals included in the PEAMs are set as the same as those set by Xu et al.\u003csup\u003e3\u003c/sup\u003e. Residues are not in consideration.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Table S7\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003eLife-cycle GHG emissions and RCP factors\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eExcept for the emissions from waste combustion, life-cycle GHG emissions are assumed to decrease in line with the decarbonization of the power generation sector in Japan\u003csup\u003e61\u003c/sup\u003e. Life-cycle RCP is assumed not to change in the future.\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eSupplementary Table S8\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e"},{"header":"Declarations","content":"\u003ch1\u003eData availability\u003c/h1\u003e\n\u003cp\u003eAll data analyzed in this study are included in its Supplementary information files.\u003c/p\u003e\n\u003ch1\u003eCode availability\u003c/h1\u003e\n\u003cp\u003eThe mathematical algorithm used in this study is available from the corresponding author upon reasonable request.\u003c/p\u003e\n\u003ch1\u003eAcknowledgements\u003c/h1\u003e\n\u003cp\u003eThis work was supported by MEXT/JSPS KAKENHI Grant Number JP21H03660,\u0026nbsp;JP21K14276 and\u0026nbsp;JP20K20016,\u0026nbsp;JST-Mirai Program Grant Number JPMJMI19C7\u0026nbsp;and JST COI-NEXT Program Grant Number JPMJPF2003. We would like to thank Mr. Izuru Suwa for his helps in LCA data collection. Activities of the Presidential Endowed Chair\u0026nbsp;for “Platinum Society” at the University of Tokyo are supported by the\u0026nbsp;KAITEKI Institute Incorporated, Mitsui Fudosan Corporation, Shin-Etsu\u0026nbsp;Chemical Co., ORIX Corporation, Sekisui House, Ltd., the East Japan\u0026nbsp;Railway Company, and Toyota Tsusho Corporation.\u0026nbsp;\u003c/p\u003e\n\u003ch1\u003eAuthor contributions\u003c/h1\u003e\n\u003cp\u003eY. D. conceived the original idea and designed the research. C. T. and Y. K. supervised and led the work. Y. D. and A. H. developed the model. Y. D. and A. H. contributed to system definition and data collection. Y. D. run the simulation and prepared the figures. A. H., C. T., and Y. K. enhanced the scenarios and discussion in technology development and policy making. Y. D. drafted the paper. Y. D. analyzed the results and contributed to writing this paper.\u0026nbsp;\u003c/p\u003e\n\u003ch1\u003eCompeting interests\u003c/h1\u003e\n\u003cp\u003eThe authors declare no competing interests.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eGent, W. E., Busse, G. M. \u0026amp; House, K. Z. The predicted persistence of cobalt in lithium-ion batteries. \u003cem\u003eNat. Energy\u003c/em\u003e\u003cstrong\u003e7\u003c/strong\u003e, 1132\u0026ndash;1143 (2022). https://doi.org/10.1038/s41560-022-01129-z\u003c/li\u003e\n\u003cli\u003eGreim, P., Solomon, A. A. \u0026amp; Breyer, C. Assessment of lithium criticality in the global energy transition and addressing policy gaps in transportation. \u003cem\u003eNat. Commun.\u003c/em\u003e\u003cstrong\u003e11\u003c/strong\u003e, 4570 (2020). https://doi.org/10.1038/s41467-020-18402-y\u003c/li\u003e\n\u003cli\u003eXu, C. J.et al. Future material demand for automotive lithium-based batteries. \u003cem\u003eCommun. 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