A ‘cool’ route to battery electrode material recovery

A ‘cool’ route to battery electrode material recovery | 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 Research Article A ‘cool’ route to battery electrode material recovery Lin Chen, Brij Kishore, Tengfei Song, Yazid Lakhdar, Bowen Liu, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4504057/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 Widespread adoption of alkali metal ion batteries poses a challenge for the recycling industry. Efficient recovery and reuse of valuable metals from end-of-life batteries and production scrap is paramount. A novel, cost-effective, fast, and scalable electrode delamination approach, 'ice-stripping,' is proposed. An electrode is wetted with water and frozen using a cold plate, then peeled. Volume expansion and the increased cohesive strength of the ice over the electrode adhesion results in 100% delamination from the current collector and recovery of electrode coatings with minimal water use, material waste, or damage. In stark contrast to conventional high-temperature methods. Its effectiveness is illustrated with Li-ion and Na-ion battery electrodes comprised of different binder systems, and the scalability is considered for scrap. A direct recycling case study for a Na-ion, hard carbon and Prussian white is presented. This innovation holds promise in meeting the escalating demand for efficient and sustainable battery recycling. High yield delamination ice-stripping direct recycling Na-ion battery Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Introduction The International Energy Agency (IEA) reported in its global EV Outlook 2024 1 that 14 million electric cars were sold globally in 2019, representing 18% of car sales that year, up from 14% in 2022 and only 2% 5 years earlier, in 2018. This growth remains robust as electric car markets mature 1 . Governments worldwide are looking to transition to EVs, which must be sustainable. High production levels of batteries for EVs and portable electrical devices will lead to a large increase in production scrap and end-of-life rechargeable batteries in the coming yearsClick or tap here to enter text.. Appropriate technologies and policies will be needed to ensure that processes for dealing with these used batteries and production scrap meet the full extent of their sustainability and CO 2 emissions reduction objectives. Therefore, battery recycling and reuse are attracting considerable attention and investments alongside the development of electric vehicles 2 – 4 . Considering the components of a battery, including battery casing, electrode materials, separators, electrolytes, additives and current collectors, electrode material recycling and reclamation of both cathode and anode are challenging and expensive due to the complex battery structure and chemistries involved. 5 – 7 Instead of using pyrometallurgy 8 or hydrometallurgical 9 processes to recover the metals from spent electrode materials, direct recycling/recovery 10,11 of the active material from spent batteries represents a preferred greener alternative. Indeed, direct recovery and reuse of active material powders can simplify recycling and minimise greenhouse gas emissions compared to other routes, which break down the materials into individual element salts and thus require multiple steps which increase both energy cost and waste 12 . Moreover, it represents the ideal solution for recovering and reusing production scrap from gigafactories, which will amount to a significant recycling waste stream worldwide and become the dominant waste stream in the near term. Spent batteries either go through mechanical crushing or manual disassembly for direct recycling, as presented in Fig. 1 . Unlike the crushing process, manually disassembling batteries provides tailored separation pathways to extract whole electrodes for further delamination and enables more efficient and sustainable techniques to achieve reclaimed materials for battery re-manufacturing. Separating the black mass (electrode material) from their current collector is a critical step towards materials recovery from batteries. This is challenging due to the binders' strong adhesion and chemical stability (e.g. Polyvinylidene fluoride, PVDF or carboxy-methyl cellulose and styrene butene rubber, CMC-SBR). Recycling efficiency, waste levels, and energy consumption related to subsequent processes are heavily associated with black mass delamination to provide high-purity waste streams. PVDF, the most widely used binders in both Li-ion (LIBs) and Na-ion batteries (SIBs), complicates black mass delamination from the current collectors during recycling 13 – 15 . Thermal treatments and dissolution of organic solvents/acids are well-known techniques for removing PVDF from battery electrodes. However, the decomposition by high-temperature thermal treatment (at 300–500°C) causes HF production, which is unwanted due to health and safety concerns. Dissolving PVDF in organic solvents 12 , such as N-methyl-2-pyrrolidone (NMP), dimethyl sulphoxide (DMSO) or dimethylformamide (DMF), can avoid the emission of gas; however, these volatile and toxic solvents need treating and reclaiming afterwards, which tends to increase recycling complexity, hazards and cost, and so limits their usage on large scale production. Acid/alkaline delamination causes the dissolution of metals from the current collectors and from the contents of the electrode active material. Furthermore, care should be taken with different active materials, for example, when subjecting Prussian blue/white analogues (major cathode materials for sodium-ion batteries) to acidic conditions, as they can release hydrogen cyanide gas, which is highly toxic 16 . A less toxic solvent, ethylene glycol (EG), has been used to replace NMP/DMF during the electrode delamination 12 . EG has a low toxicity inherently but produces toxic metabolites, emphasising the importance of safe handling of this solvent in some processes. Mechanical techniques such as high-energy ultrasound 17 have been employed as an efficient separation option to break the adhesive bond and enable delamination in a matter of seconds. However, these may damage the crystal structure and morphology of the reclaimed materials (as shown in recent studies on the recovery of graphite by such routes 18 , requiring more effort in the materials re-manufacturing step. Moreover, impurities from current collectors are inevitable in mechanical treatments. For water-based binder systems, water is sufficient to dissolve the binders for delamination; however, while the water dissolves the CMC, the SBR added in the electrode manufacturing process as an emulsion remains and so can hinder the delamination process. Another challenge is to minimise the damage to the Al/Cu current collector 19 , 20 . Thermal treatments, organic solvents/acids, and basic dissolution delamination processes that have been reported will inevitably result in current collector damage and Al contamination during the delamination process 21 – 24 . Cryo-milling separation has been discussed as an assisted technique during milling/grinding for Li-ion battery recycling, such as cryogenic ball mill 25 and cryogenic grinding 26 , 27 . However, milling and grinding inevitably cause significant current collector damage and contamination. This study challenges the conventional thermal solution processing approach by introducing a novel concept of lowering temperatures to sub-zero levels to harness ice's cohesive strength over the electrode adhesion to delaminate electrode coatings. This innovative technique, termed "ice-stripping" delamination technology, has been tested on sodium-ion and lithium-ion electrodes fabricated with PVDF-NMP and CMC-SBR binder systems to illustrate that it is both an electrode material and binder agnostic process. This novel methodology shows reduced water usage, improved recovery rates and less damage to the materials compared to milling and other routes. Results and Discussions Two freezing methods, tray and surface, have been investigated for their ability to delaminate both production scrap and end-of-life lithium and sodium-ion positive and negative electrodes. The processes are illustrated in Supplementary Data Figures S1-S3 . In the tray method, a 3D-printed tray was designed to stop the electrode from sinking. A tailored tray was designed and 3D-printed, as shown in Figure S1. To minimise water usage, the height of the tray was set to 1 cm, which was sufficient for the electrode delamination. To begin the delamination process, the tray was filled with water, and the electrode coating was placed on top. The tray consisted of several spikes slightly lower than 1 cm and well distributed to prevent the coating from sinking. The tray and the electrode undergoing delamination were placed on a flat surface inside a refrigerator, which was maintained at -40°C. The water penetrates the porous network inside the electrode coating, and with time, the temperature drops to sub-zero values. After one hour, the tray was removed from the refrigerator, and the electrode coating was carefully peeled off. The amount of DI water and the freezing time for CMC/SBR-based Hard Carbon electrode scrap was ~ 10 mL/cm 2 and 1 hr, respectively. The black mass was separated from the Al current collector and remained in the iced tray. The “ice-stripping” delamination technique was further improved and modified by using a cold plate, in this example, a repurposed ice cream maker (Figure S2). The method exploits the contrast between the strong chemical bonding of the ice within the electrode vs. the relatively weak bonding and adhesion of the electrode coating to the current collector. The delamination process is similar to that described above, pouring water-place coating-freeze coating-peeling coating. The temperature of the ice cream maker can reach − 8°C, which is sufficient for the delamination process, and the freezing time was reduced to 5 min because of the lower quantities of water used. The ice adhered to the cold surface. The foil was then stripped away from the electrode materials, giving the advantages of using an ice-cream maker to delaminate the same scraps as above: 1) reduction in the amount of water required for the same scrap delamination (0.1 mL/cm 2 electrode; 2) reduced the processing time (freezing time); 3) more straightforward to handle; and 4) potential to be scale-up and industrialised. This technique has been further improved by spraying water into the electrode before placing it onto the cold plate (Apply gentle pressure on the electrode and peel the Al current collector (Figure S3)). For the same electrode scrap, the amount of water and the freezing time are reduced to 0.02 mL/cm2 and 10s, respectively. No. Electrode Binder Porosity(%) Coating thickness (um) Contact Angle ( o ) 1 PW CMC/SBR 25±2 80±3 70.74 2 HC CMC/SBR 35±2 50±1 42.85 3 PW PVDF 30±2 80±3 73.01 4 NaTMO PVDF 35±1 75±1 50.36 5 EoL Graphite PVDF 28±1 75±1 25.86 6 LTMO PVDF 35±1 70±1 75.85 The success of the method in allowing efficient delamination is facilitated by the fact that water can penetrate the electrode, and when water freezes into ice, water molecules become arranged into an organized 3D network, which creates more hydrogen bonds between ice and particles surface and a strong bonding network in the porous electrode as illustrated in Fig. 2 a. Furthermore, the expanded volume from water to ice (nearly 9%) creates extra pressure within particles. To confirm this, adhesion measurements were carried out with tape-peeling at room temperature and ice-stripping at -5 o C. The adhesion forces were recorded when the whole black mass was peeled/stripped off from the current collector. For ice-stripping, the substrate was cooled to ~ -5 o C before the test. Figure 2 b- 1 shows the distance between the electrode and cold substrate, temperature vs . time during the measurement. When the wetted electrode disc (d = 8mm) surface was in contact with the cold surface, the substrate temperature increased and became stable in 5 seconds, indicating successful heat transfer and resulting in the water in the electrode being frozen. The electrode was then stripped off after a few seconds to measure the adhesion between the black mass and Al foil. With increasing distance, the pull-off force was sharply increased till the black mass delaminated from the current collector (Fig. 2 b- 2 ). During the ice-stripping process, the water penetrates the porous electrode, providing a stronger cohesive bond than the electrode's adhesive bond to the current collector. This results in the porous electrode components remaining on the cold surface after the current collector is stripped off. To further test the versatility of this delamination method, several different lithium and sodium electrodes from scrap or end-of-life, Prussian White (PW)-CMC/SBR, Hard Carbon (HC)-CMC/SBR, PW-PVDF, Sodium transition metal layered oxide (NaTMO)-PVDF, Lithium transition metal layered oxide (LTMO)-PVDF and Graphite-PVDF were also tested. The peel-off forces at room temperature and at -5 o C were compared, as illustrated in Figure S4 and Fig. 2 c. The force was reduced after the electrodes were frozen in most of the cases due to the stronger cohesive bond within the black mass from frozen water. However, there are exceptions, such as HC-CMC/SBR and LTMO-PVDF, where the pull-off force increased after freezing. The electrodes' porosity, thickness and contact angles were recorded as listed in Table 1 to understand the correlations. However, more coatings are required to obtain statistical results. As a full-cell case study, the ice stripping delamination process was evaluated for a PW-HC A7 end-of-life Na-ion pouch cell. The cell was stabilised and opened, and the electrodes were removed before washing in IPA and then drying, as shown in Figure S5. The effect of the ultrasound-assisted delamination process (hammer (ball) milling) on the efficiency and the impact on the recovered materials was investigated and compared with the ice-stripping process. For the former, multiple steps, electrode resize, ultrasound-assisted milling delamination, current collector removal and binder removal, were processed as presented in Fig. 3 . Moreover, some steps were required to be repeated a few times to maximize the delamination efficiency in this case. On the other hand, the ice-stripping process was straightforward. The compound separation efficiency of the coating is calculated using the equation below. $$CSEcoating=\frac{mass of separated coating}{initial mass of coating}$$ If we take the HC-CMC/SBR coating as an example. Only 53% separation efficiency was achieved through ultrasound-assisted ball-milling delamination, whereas the ice-stripping technique can achieve a separation efficiency as high as 96% (Fig. 3 ). The coating separation efficiency via the ice-stripping method was also calculated with several other electrodes extracted from commercial cells, Calb (LFP), Thunder Sky (LCO), UKBIC (NMC) and Nissan (NMCA), and presented in Fig. 3 b. High recovery yields were obtained at 98%, 100%, 93% and 95%, respectively. The delamination efficiency of thick electrodes can be improved by increasing the wetting time with more water. Porosity is considered a key factor as it allows water to penetrate the pores and freeze when the temperature drops. The electrode porosity of the commercial electrodes was all in the range of 25–35% (Fig. 3 b), which the results show is sufficient to allow delamination of all the electrodes examined, illustrating the versatility of this technique. The reclaimed PW and HC materials were then characterised to examine any changes in morphology and crystal structures (Fig. 4 ). After delamination of the PW cathode and HC anode, the black masses were washed and centrifuged several times with water to remove the binders. The final reclaimed PW and HC power were dried at 120°C overnight. The XRD pattern of reclaimed PW shows cell symmetry change compared to the pristine PW, as shown in Fig. 4 a. In line with this, the EDS results show that the average value of the Na/Fe ratio in the reclaimed PW power is lower at ~ 0.33, indicating Na loss from battery use and during/after the delamination process. Thus, the reclaimed PW powder is the lower Na content cubic phase rather than the as-received monoclinic phase. The HC reclamation is much simpler as the presence of water has less of an effect on the structure of HC, as shown in Fig. 4 b. Figures 4 c and 4 d display the morphology of the PW coating from end-of-life cells before delamination and pristine PW powder. Figures 4 e and 4 f show the morphologies of the reclaimed PW powder via ultrasound-assisted ball-milling and ice-stripping techniques. The ice-stripping technique maintains PW's morphology and particle size, which is beneficial for subsequent direct recycling processes. Some unevenly distributed white stains were observed on the HC anode after drying, likely from Na plating during cell operation and SEI components after exposure to air during disassembly and washing processes. Nevertheless, after ice-stripping, the reclaimed HC powder maintained both the particle size and morphology. The morphologies of the recycled Al current collectors were also studied, and the difference between ball-milling and ice-stripping delamination techniques was compared, as shown in Figure S6. Micro-wrinkles were observed on the Al surface after ball-milling, as shown in Figure S6a, which came from the zirconium balls, causing damage during milling. In addition, some un-delaminated PW powders were observed in some areas on the Al current collector (Figure S6b). These observations indicate that insufficient delamination was achieved from the ball-milling procedure. The damaged Al also reduces the chances of the current collector being directly re-used or re-manufactured for subsequent new battery production. Conversely, the Al current collector remained flat without wrinkles after ice-stripping at low temperatures (Figure S6c). After cold-plate delamination, the Al current collector surface remained flat, as shown in Figure S6d. This suggests that ice-stripping is more effective than ultrasound-assisted ball-milling as a delamination technique and offers more possibilities in current collector reuse. The reclaimed PW (re-PW) and reclaimed HC (re-HC) were assessed for direct recycling possibilities and re-manufactured into an electrode with CMC/SBR binders. The pristine and recovered PW voltage profiles are compared. Galvanostatic charge and discharge profiles of re-PW showed less distinctive and much shorter plateaus, indicating lower Na contents in the reclaimed materials, consistent with the XRD results (Fig. 4 a). This indicates that resodiation is required to recover performance. The re-HC was also tested in a half cell in the voltage window of 0.01V-3.00V at a specific current of 10mA/g. The HC half-cell discharge profile consists of two distinct phases, a sloping region at high voltage and a plateau at low voltage 0-0.1V, corresponding to the absorption-intercalation mechanism 28 – 30 . The initial reversible capacity of re-HC is 245.5 mAh/g compared to 291.1 mAh/g achieved in pristine HC half-cell, as observed in Fig. 5 b. The capacity deviation and cycling stability presented in Fig. 5 c are likely due to the unwashed impurities in the reclaimed HC. The re-HC anode was also tested in a full cell configuration to avoid the challenges (high polarization) associated with testing vs . Na metal. The 1st charge-discharge profile of the PW/re-HC and PW/pristine HC are shown in Fig. 5 d. The full cell assembled with re-HC gave similar profiles as the one with pristine HC, and the capacity was 121.8 and 128.6 mAh/g, respectively. However, the capacity decreased with time, and 70% of the capacity remained after 50 cycles for the PW/re-HC, as shown in Fig. 5 e. This is likely due to residual binders and SEI layers in the re-HC powers. Further heat treatments are required to eliminate all the non-conductive binder polymers remaining in the reclaimed HC powers to restore the material to the equivalent of the original pristine material, which will be the subject of further studies. Nevertheless, the work illustrates that the ice stripping approach is an effective initial recovery step towards this direct recycling regeneration. Sustainability and environmental impact Due to the physical black mass delamination and the low operation temperature of -10 to 0 o C ice-stripping method does not release any VOCs (volatile organic components) and environmentally harmful toxins that can be produced through high-temperature black-mass burning 24 , such as styrene, acrylates, unsaturated volatiles, or fluorinated products in the binder was fluoride-based. Moreover, due to technology flexibility and chemically non-destructive conditions, any black mass composition can be freeze-induced and delaminated from the current collector without chemical transformation or decomposition. Additionally, this procedure minimises the generation of solid or gaseous wastes. The carbon footprint for the ice-stripping process consists only of carbon emission due to energy consumption to cool the surface down to operating temperature. Measurement of electricity for the ice-stripping method was carried out using specialized meters that allow continuous recording from the beginning when the machine is turned on until the whole delamination process is completed. 0.025 kWh electricity consumption was recorded when 104g black mass was delaminated with the ice-stripping method. On the other hand, additional energy consumption, such as ethylene glycol (EG) 12 manufacturing (0.36 kg CO 2 /kg 31 ), need to be taken into consideration for the wet-chemical delamination process. Furthermore, the ice-stripping method does not require any harmful chemicals that can be found in pyrometallurgy and hydrometallurgy. The cooling agent varies from chemical cooling agents, closed-circuit Stirling engine or CO 2 32,33 . Such newer methods can reduce the environmental impact by more than four thousand times. It can reduce even further and reach zero carbon emission when taking advantage of the winter season in some Northern countries, where the temperature naturally drops to sub-zero degrees Celsius for a minimum of three months. The ice stripping process has been demonstrated at the electrode sheet level on a small scale. However, there is potential to scale this to a continuous process, which is particularly useful for scrap electrodes. The constant coating from the manufacturing of electrodes, if needed to be scrapped, could be fed through either 1) an ice stripping roller and the double-sided coatings delaminated simultaneously or 2) a cold belt to delaminate side-by-side. Stripping could also be considered before drying, as the water or solvent could freeze and be stripped away from the current collector before entering the drying zone. Examples are given in Fig. 6 . This continuous process further improves the energy cost and is used to reclaim material which can be directly reused in the manufacturing process with very little further processing. Conclusions and outlook Here, we present a novel reverse-thought concept for the electrode delamination process for battery direct recycling. Rather than the traditional elevated-temperature heat treatment process, ‘Ice-stripping’ involves wetting an electrode and cooling the temperature to sub-zero to freeze the water. The frozen water in the electrode forms a strong cohesive bond, ensuring that the weaker bond between the coating and current collector foil is broken preferentially when stripped off the surface. In this work, the ice stripping process underwent several iterations to reduce separation time, improve black mass recovery efficiency and reduce water waste. The process has been tested with various lithium and sodium-ion positive and negative electrodes, illustrating the approach's success for both PVDF and CMC-SBR binder systems. Initially, the concept was demonstrated using a tray of water; the electrode was placed on top and then frozen, the porous electrode remained bonded to the ice, and the current collector was peeled away. Further improvements were made by moving to a cold surface, where a wetted electrode was frozen and peeled. The time was reduced from 5 minutes to 30 seconds by spraying water on the surface of the electrode, hence reducing time, energy, and waste. When used in a case study using an end-of-life A7 sodium-ion pouch cell, high separation efficiency (96%) was achieved from the surface ice-stripping delamination compared to traditional ball milling (56%), and the effect upon the morphology of the reclaimed materials minimal. The reclaimed cathode and anode materials were directly reused and remanufactured into full battery cells, and the preliminary results show great potential for active material direct recycling. Compared to other delamination methods that have been reported, the ice-stripping technique offers several advantages: High delamination yield. High purity of recovered materials with original morphology and size can be directly recycled. Limited water waste and virtually no contamination Good current collector grade for recovery and recycling or even direct reuse for small-scale R&D work. Binder agnostic approach, even capable of use to delaminate coatings containing non-water-soluble binders, such as PVDF. Possibility to scale up for battery recycling of electrode scraps from gigafactories and end-of-life batteries. This work provides evidence of a novel and sustainable promising delamination process, which can become the key first stage in a direct recycling process for both Na-ion and Li-ion batteries. Methods Electrode scrap and cell disassembly Double-side coated Prussian white (PW) cathode coatings and hard carbon (HC) anode coatings are provided by the project partner Warwick Manufacturing Group (WMG, University of Warwick), as well as the end-of-life A7 size pouch cells with PW and HC as cathode and anode. The PW cathode electrode consists of 93wt% PW, 3wt% CMC/SBR (1:2) binders and 3wt% C65 and the HC anode electrodes consist of 96wt% HC, 3wt% CMC/SBR (1:2) binders and 1wt% C45. The coating weights of the cathode and anode are 150 g/m 2 and 70 g/m 2, respectively. The end-of-life A7 pouch cells were discharged and carefully opened in a fume hood after slowly releasing any gases generated during the cells' charge-discharge cycling (Figure S5a). The cell bodies were disconnected from the casing by cutting the tabs. The separator was zig-zag unwrapped to separate cathodes from anodes. The disassembled electrodes were soaked in isopropyl alcohol (IPA) overnight before drying them at 60 o C in a vacuum oven overnight. The dried electrodes were then ready for the delamination process. Figure S5b shows the component flows through the cell disassembly and cell parts sorting process. Some weight losses are found after IPA soaking, as well as binder removal after the delamination process. Ball-milling and sonication for delamination The electrode delamination was also carried out using the ultrasound-assisted ball-milling and sonication technique to compare the results with the newly developed “ice-stripping” process. In this process, the electrodes were cut into small pieces of roughly 1 cm 2 area and placed in a beaker which was filled with DI water (H 2 O/Coating weight ratio is 20:1). The beaker was placed in a sonicator bath running at full power at 40°C for 1h. As the separation under these conditions was not sufficient, zirconia balls were added to the HDPE bottle to improve the separation efficiency; the beaker's contents were poured into it and placed on a roller mill for 3h. Further, the separated black mass and current collector were collected by filtration followed by centrifugation. Characterisation The structural characteristics of the PW and HC before and after delamination were determined by X-ray diffraction using a Bruker D8 Advance instrument with a Cu Kα radiation source. The X-ray diffraction data were recorded at a scan rate of 1°min − 1 in the 2θ range between 10° and 70°at 40 KV and 30mA. Scanning electron microscopy with a field-emission SEM microscope (Sigma, Carl Zeiss, Germany) equipped with an energy-dispersive spectrometer (EDS) (Xmax 50, Oxford Instruments) was used to characterize the surface of the electrodes after cycling. SEM images were captured at 10 kV (1.6 nA) when a high-performance ion conversion and electron detector was employed or 20 kV (8.0 nA) when a secondary electron detector was employed. Adhesion and cohesion were tested by the Kinexus pro + Rheometer. 8-mm-diameter electrodes were stuck on the probe, and tape was used to remove the coating. The force data were recorded by the Rspace software. The reclaimed PW and HC were re-manufactured into electrodes, and electrochemical characterisations were carried out using both half-cell and full-cell configurations. Electrochemical characterisations The reclaimed Prussian White (re-PW) cathode material was made into an electrode with 93wt% re-PW, 3wt% CMC/SBR binders and 4wt% C65 using a slurry cast process. The reclaimed hard carbon (re-HC) negative electrode contained (96wt% re-PW, 3wt% CMC/SBR binders and 1wt% C45). The cathodes were dried in vacuum (~ 10 − 3 mbar) at 150°C overnight and the HC anode was dried at 120°C overnight prior to being transferred into a glovebox. Half-cells were first studied using 1M NaPF 6 dissolved in EC: DEC (1:1 V/V) as the electrolyte in the voltage window of 2.0-4.0V vs. Na + /Na for the cathode and 0.01V-3.00V vs. Na + /Na for the anode. The electrochemical performance of full cells was evaluated in 2032-type coin cells, with PW/re-PW cathode (12.7 mg/cm 2 ), HC/re-HC anode (8.2 mg cm − 2 ), separated by Glass fiber (Whatman®) containing enough electrolyte to wet the components (~ 100 µl). In each case three independently produced cells were tested to show standard deviations. Declarations Notes The authors declare no competing financial interest. A patent on this technique has been submitted. Acknowledgement The authors thank Dr Ivana Hasa and the team at WMG, University of Warwick, for providing end-of-life cells and electrode scrap. 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Adv Energy Mater 11 Renewable A, February C (2022) Third Pa rty a nd Critica lly Reviewed Ra y pla ntMEG TM Life Cycle Assessment (LCA) Discla imer Cytiva Going liquid nitrogen-free for low-impact cryopreservation Allen I (2023) Marlborough company goes green with its CO2 machine Additional Declarations The authors declare no competing interests. Supplementary Files IcestrippingfromcoatingHCsinglelayer.mov GA.png 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. 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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-4504057","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":308743578,"identity":"77000e20-db8d-4bcf-a44c-1a26b6eb8d0a","order_by":0,"name":"Lin Chen","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA0UlEQVRIiWNgGAWjYBACPgYGNhBdzy/BAxNjw6+FDaoiQXIGyVoMbhCvhfnZg487GPKMb/ce/HSDwU6eQSItgYAWNnPDmWcYis3unEuWzmFINmyQSDtAQAsPmzRvGwPjths5BkAtzAkMEukNhLX8BWrZPCPH+HcOQz2RWhjbGBI3SOSYAW05DNRCyGHMbGaSvW0SxhJ3zphZ5xgcN2zjeZaAVws/e/MziZ9tNnL8s3uMb+dUVMvzs6cZ4NXCwAwmJaA8A4KxMgpGwSgYBaOAGAAA3pk05nuBMZgAAAAASUVORK5CYII=","orcid":"","institution":"University of Birmingham","correspondingAuthor":true,"prefix":"","firstName":"Lin","middleName":"","lastName":"Chen","suffix":""},{"id":308743579,"identity":"39b85b70-0b5d-4f50-940e-fff7672d7fc2","order_by":1,"name":"Brij Kishore","email":"","orcid":"","institution":"University of Birmingham","correspondingAuthor":false,"prefix":"","firstName":"Brij","middleName":"","lastName":"Kishore","suffix":""},{"id":308743580,"identity":"bbd45eb0-4f43-4674-b0e5-9eea3f9336a6","order_by":2,"name":"Tengfei Song","email":"","orcid":"","institution":"University of Birmingham","correspondingAuthor":false,"prefix":"","firstName":"Tengfei","middleName":"","lastName":"Song","suffix":""},{"id":308743581,"identity":"9168ee60-33b7-485d-90b6-2089ff5804e4","order_by":3,"name":"Yazid Lakhdar","email":"","orcid":"","institution":"University of Birmingham","correspondingAuthor":false,"prefix":"","firstName":"Yazid","middleName":"","lastName":"Lakhdar","suffix":""},{"id":308743582,"identity":"88cc3408-da81-470f-b0ba-987e20a028f5","order_by":4,"name":"Bowen Liu","email":"","orcid":"","institution":"University of Birmingham","correspondingAuthor":false,"prefix":"","firstName":"Bowen","middleName":"","lastName":"Liu","suffix":""},{"id":308743583,"identity":"ecbba303-2cbb-42ac-a785-de0071172ada","order_by":5,"name":"Osaze Omoregbe","email":"","orcid":"","institution":"University of Birmingham","correspondingAuthor":false,"prefix":"","firstName":"Osaze","middleName":"","lastName":"Omoregbe","suffix":""},{"id":308743584,"identity":"75c1165a-3613-4c94-a33c-0f5f46674d7b","order_by":6,"name":"Peter Slater","email":"","orcid":"","institution":"University of Birmingham","correspondingAuthor":false,"prefix":"","firstName":"Peter","middleName":"","lastName":"Slater","suffix":""},{"id":308743585,"identity":"af229b8f-5c80-4fb9-9d98-3eb6385de250","order_by":7,"name":"Emma Kendrick","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA5klEQVRIie3RvQrCMBDA8ZPAuVzJ2lLRV2gpKE6+SovgLAhODoLQLtW5j+Gka6VQl9pZCYhQ8AUEF0H8wsUh1c0hf8iQgx9JCIBK9ZfhcxEQS9l7Vhl/R7D3GwEgan5HOKBX9If7Gg+zc9EfLYAHMRqRhBhjTJwoH5C+mS6dKBWgZy4acwmx4qpvar5LFtcWJqEA2AIaBwnpxNXg8iJ0NOkqoFFGLMCUPYkW4v04AdaDyC6mJ9g1KXdJz9KWo80E2Zk3acuezwPfPtHQ7fCweyzoLOr1dbLahRIC7GNPpR+pUqlUqvJuJ69CbyIZM9gAAAAASUVORK5CYII=","orcid":"https://orcid.org/0000-0002-4219-964X","institution":"University of Birmingham","correspondingAuthor":true,"prefix":"","firstName":"Emma","middleName":"","lastName":"Kendrick","suffix":""}],"badges":[],"createdAt":"2024-05-30 15:32:01","currentVersionCode":1,"declarations":{"humanSubjects":false,"vertebrateSubjects":false,"conflictsOfInterestStatement":false,"humanSubjectEthicalGuidelines":false,"humanSubjectConsent":false,"humanSubjectClinicalTrial":false,"humanSubjectCaseReport":false,"vertebrateSubjectEthicalGuidelines":false},"doi":"10.21203/rs.3.rs-4504057/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4504057/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":57518380,"identity":"17882778-1a20-4a76-a994-b814a39b4e91","added_by":"auto","created_at":"2024-05-31 20:31:15","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":207229,"visible":true,"origin":"","legend":"\u003cp\u003eBinder removal processes for directly recycling in LIBs/SIBs.\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/08a71df2f073c6d62ddafa38.png"},{"id":57519202,"identity":"f5be34e7-8530-4c2e-a708-8355021281c8","added_by":"auto","created_at":"2024-05-31 20:39:15","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":322180,"visible":true,"origin":"","legend":"\u003cp\u003ea. The mechanism of ice-stripping technique on electrode. b. the Rheometer results of the CMC-SBR HC electrode: (above) detector distance and base temperature recorded in time during contact; (below) detector distance and force recorded in time during pull-off; and (c) the composition of adhesion force and delamination force via ice-stripping on different electrodes. d. Table summary of the electrodes tested in this work, the material, formulation, porosity adhesion/delamination and time to freeze.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/2bbf73a6a6e3c7eb7fd7a73a.png"},{"id":57518381,"identity":"753d6c43-a803-4f27-bfe7-773e315f1e37","added_by":"auto","created_at":"2024-05-31 20:31:15","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":173463,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cem\u003ea. The HC electrode delamination processes are done using different techniques: Red routes on the left represent the ultrasound-assisted ball-milling process, and the green route represents the ice-stripping process. Coating separation efficiency of electrodes with varying techniques of delamination. The results show much greater separation efficiency using the ice delamination process. b. Coating separation efficiency via ice-stripping, average contact angle, thickness and the porosity of the coatings obtained from commercial batteries.\u003c/em\u003e\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/dbdee52b45d347e0d99a1801.png"},{"id":57518382,"identity":"a02b5282-07d5-4bce-9bb4-598052cb3d85","added_by":"auto","created_at":"2024-05-31 20:31:15","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":674386,"visible":true,"origin":"","legend":"\u003cp\u003eXRD patterns of the reclaimed PW (a) and HC (b) powders after the ice-stripping process compared with the pristine PW and HC, respectively. SEM images of (c)PW cathode coating before recycling,(d) pristine PW, reclaimed PW with (e) ball-milling technique and with (f) ice-stripping technique. g and h: SEM of HC coating and reclaimed HC with ice-stripping technique.\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/1b9058436f1fe749b27c50cb.png"},{"id":57518386,"identity":"5f5f5c84-6a9e-44be-991c-60b091bb8ff7","added_by":"auto","created_at":"2024-05-31 20:31:15","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":217654,"visible":true,"origin":"","legend":"\u003cp\u003eCell testing at 10 mA/g with 1M NaPF\u003csub\u003e6\u003c/sub\u003e in EC: DEC (1:1 v/v). a. Initial voltage profile of pristine PW and re-PW half-cell. b, c. Initial voltage profile and the cycling stability of re-HC. d,e. Initial full cell voltage profile and cycling comparison between PW|re-HC and PW| Pristine HC.\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/8ecc7f29f793f29e10bebe86.png"},{"id":57518383,"identity":"03194016-526a-4965-8d08-53f700b7e657","added_by":"auto","created_at":"2024-05-31 20:31:15","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":187030,"visible":true,"origin":"","legend":"\u003cp\u003eDemonstration of continuous delamination process for scrapped electrodes.\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/6cd075f5b8c7433d3e12432d.png"},{"id":57519596,"identity":"d4cc15d9-d153-4cd0-a6da-c6f41472ff1a","added_by":"auto","created_at":"2024-05-31 20:47:16","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2187942,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/4d976178-d757-4056-b6ae-f97e6bc2d579.pdf"},{"id":57518388,"identity":"1b6159a0-fab0-416e-bd37-25bad3955583","added_by":"auto","created_at":"2024-05-31 20:31:17","extension":"mov","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":172898145,"visible":true,"origin":"","legend":"","description":"","filename":"IcestrippingfromcoatingHCsinglelayer.mov","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/c6f6ee3cd04662501b9ebbc9.mov"},{"id":57518379,"identity":"f249556e-264a-4c54-8c3b-a6c973706477","added_by":"auto","created_at":"2024-05-31 20:31:15","extension":"png","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":234684,"visible":true,"origin":"","legend":"","description":"","filename":"GA.png","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/d585923964effb02dd2f2d04.png"},{"id":57518387,"identity":"875b4c8a-53bd-4516-bf7d-b712ba9b2584","added_by":"auto","created_at":"2024-05-31 20:31:15","extension":"docx","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":8923660,"visible":true,"origin":"","legend":"","description":"","filename":"SupplementaryInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-4504057/v1/7abebfb560d2e0725b8e37ef.docx"}],"financialInterests":"The authors declare no competing interests.","formattedTitle":"\u003cp\u003eA ‘cool’ route to battery electrode material recovery\u003c/p\u003e","fulltext":[{"header":"Introduction","content":"\u003cp\u003eThe International Energy Agency (IEA) reported in its global EV Outlook 2024\u003csup\u003e1\u003c/sup\u003e that 14\u0026nbsp;million electric cars were sold globally in 2019, representing 18% of car sales that year, up from 14% in 2022 and only 2% 5 years earlier, in 2018. This growth remains robust as electric car markets mature\u003csup\u003e\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u003c/sup\u003e. Governments worldwide are looking to transition to EVs, which must be sustainable. High production levels of batteries for EVs and portable electrical devices will lead to a large increase in production scrap and end-of-life rechargeable batteries in the coming yearsClick or tap here to enter text.. Appropriate technologies and policies will be needed to ensure that processes for dealing with these used batteries and production scrap meet the full extent of their sustainability and CO\u003csub\u003e2\u003c/sub\u003e emissions reduction objectives. Therefore, battery recycling and reuse are attracting considerable attention and investments alongside the development of electric vehicles\u003csup\u003e\u003cspan additionalcitationids=\"CR3\" citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eConsidering the components of a battery, including battery casing, electrode materials, separators, electrolytes, additives and current collectors, electrode material recycling and reclamation of both cathode and anode are challenging and expensive due to the complex battery structure and chemistries involved.\u003csup\u003e\u003cspan additionalcitationids=\"CR6\" citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e\u003c/sup\u003e Instead of using pyrometallurgy\u003csup\u003e\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e\u003c/sup\u003e or hydrometallurgical\u003csup\u003e\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e\u003c/sup\u003e processes to recover the metals from spent electrode materials, direct recycling/recovery\u003csup\u003e10,11\u003c/sup\u003e of the active material from spent batteries represents a preferred greener alternative. Indeed, direct recovery and reuse of active material powders can simplify recycling and minimise greenhouse gas emissions compared to other routes, which break down the materials into individual element salts and thus require multiple steps which increase both energy cost and waste\u003csup\u003e\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e. Moreover, it represents the ideal solution for recovering and reusing production scrap from gigafactories, which will amount to a significant recycling waste stream worldwide and become the dominant waste stream in the near term. Spent batteries either go through mechanical crushing or manual disassembly for direct recycling, as presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. Unlike the crushing process, manually disassembling batteries provides tailored separation pathways to extract whole electrodes for further delamination and enables more efficient and sustainable techniques to achieve reclaimed materials for battery re-manufacturing.\u003c/p\u003e \u003cp\u003eSeparating the black mass (electrode material) from their current collector is a critical step towards materials recovery from batteries. This is challenging due to the binders' strong adhesion and chemical stability (e.g. Polyvinylidene fluoride, PVDF or carboxy-methyl cellulose and styrene butene rubber, CMC-SBR). Recycling efficiency, waste levels, and energy consumption related to subsequent processes are heavily associated with black mass delamination to provide high-purity waste streams.\u003c/p\u003e \u003cp\u003ePVDF, the most widely used binders in both Li-ion (LIBs) and Na-ion batteries (SIBs), complicates black mass delamination from the current collectors during recycling\u003csup\u003e\u003cspan additionalcitationids=\"CR14\" citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u003c/sup\u003e. Thermal treatments and dissolution of organic solvents/acids are well-known techniques for removing PVDF from battery electrodes. However, the decomposition by high-temperature thermal treatment (at 300\u0026ndash;500\u0026deg;C) causes HF production, which is unwanted due to health and safety concerns. Dissolving PVDF in organic solvents\u003csup\u003e\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e, such as N-methyl-2-pyrrolidone (NMP), dimethyl sulphoxide (DMSO) or dimethylformamide (DMF), can avoid the emission of gas; however, these volatile and toxic solvents need treating and reclaiming afterwards, which tends to increase recycling complexity, hazards and cost, and so limits their usage on large scale production. Acid/alkaline delamination causes the dissolution of metals from the current collectors and from the contents of the electrode active material. Furthermore, care should be taken with different active materials, for example, when subjecting Prussian blue/white analogues (major cathode materials for sodium-ion batteries) to acidic conditions, as they can release hydrogen cyanide gas, which is highly toxic\u003csup\u003e\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u003c/sup\u003e. A less toxic solvent, ethylene glycol (EG), has been used to replace NMP/DMF during the electrode delamination\u003csup\u003e\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e. EG has a low toxicity inherently but produces toxic metabolites, emphasising the importance of safe handling of this solvent in some processes. Mechanical techniques such as high-energy ultrasound\u003csup\u003e\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u003c/sup\u003e have been employed as an efficient separation option to break the adhesive bond and enable delamination in a matter of seconds. However, these may damage the crystal structure and morphology of the reclaimed materials (as shown in recent studies on the recovery of graphite by such routes\u003csup\u003e\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u003c/sup\u003e, requiring more effort in the materials re-manufacturing step. Moreover, impurities from current collectors are inevitable in mechanical treatments.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFor water-based binder systems, water is sufficient to dissolve the binders for delamination; however, while the water dissolves the CMC, the SBR added in the electrode manufacturing process as an emulsion remains and so can hinder the delamination process.\u003c/p\u003e \u003cp\u003eAnother challenge is to minimise the damage to the Al/Cu current collector\u003csup\u003e\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e,\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u003c/sup\u003e. Thermal treatments, organic solvents/acids, and basic dissolution delamination processes that have been reported will inevitably result in current collector damage and Al contamination during the delamination process\u003csup\u003e\u003cspan additionalcitationids=\"CR22 CR23\" citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e. Cryo-milling separation has been discussed as an assisted technique during milling/grinding for Li-ion battery recycling, such as cryogenic ball mill\u003csup\u003e\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e\u003c/sup\u003e and cryogenic grinding\u003csup\u003e\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e,\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e\u003c/sup\u003e. However, milling and grinding inevitably cause significant current collector damage and contamination.\u003c/p\u003e \u003cp\u003eThis study challenges the conventional thermal solution processing approach by introducing a novel concept of lowering temperatures to sub-zero levels to harness ice's cohesive strength over the electrode adhesion to delaminate electrode coatings. This innovative technique, termed \"ice-stripping\" delamination technology, has been tested on sodium-ion and lithium-ion electrodes fabricated with PVDF-NMP and CMC-SBR binder systems to illustrate that it is both an electrode material and binder agnostic process. This novel methodology shows reduced water usage, improved recovery rates and less damage to the materials compared to milling and other routes.\u003c/p\u003e"},{"header":"Results and Discussions","content":"\u003cp\u003eTwo freezing methods, tray and surface, have been investigated for their ability to delaminate both production scrap and end-of-life lithium and sodium-ion positive and negative electrodes. The processes are illustrated in Supplementary Data \u003cb\u003eFigures S1-S3\u003c/b\u003e.\u003c/p\u003e \u003cp\u003eIn the tray method, a 3D-printed tray was designed to stop the electrode from sinking. A tailored tray was designed and 3D-printed, as shown in Figure S1. To minimise water usage, the height of the tray was set to 1 cm, which was sufficient for the electrode delamination. To begin the delamination process, the tray was filled with water, and the electrode coating was placed on top. The tray consisted of several spikes slightly lower than 1 cm and well distributed to prevent the coating from sinking. The tray and the electrode undergoing delamination were placed on a flat surface inside a refrigerator, which was maintained at -40\u0026deg;C. The water penetrates the porous network inside the electrode coating, and with time, the temperature drops to sub-zero values. After one hour, the tray was removed from the refrigerator, and the electrode coating was carefully peeled off. The amount of DI water and the freezing time for CMC/SBR-based Hard Carbon electrode scrap was ~\u0026thinsp;10 mL/cm\u003csup\u003e2\u003c/sup\u003e and 1 hr, respectively. The black mass was separated from the Al current collector and remained in the iced tray.\u003c/p\u003e \u003cp\u003eThe \u0026ldquo;ice-stripping\u0026rdquo; delamination technique was further improved and modified by using a cold plate, in this example, a repurposed ice cream maker (Figure S2). The method exploits the contrast between the strong chemical bonding of the ice within the electrode \u003cem\u003evs.\u003c/em\u003e the relatively weak bonding and adhesion of the electrode coating to the current collector. The delamination process is similar to that described above, pouring water-place coating-freeze coating-peeling coating. The temperature of the ice cream maker can reach \u0026minus;\u0026thinsp;8\u0026deg;C, which is sufficient for the delamination process, and the freezing time was reduced to 5 min because of the lower quantities of water used. The ice adhered to the cold surface. The foil was then stripped away from the electrode materials, giving the advantages of using an ice-cream maker to delaminate the same scraps as above: 1) reduction in the amount of water required for the same scrap delamination (0.1 mL/cm\u003csup\u003e2\u003c/sup\u003e electrode; 2) reduced the processing time (freezing time); 3) more straightforward to handle; and 4) potential to be scale-up and industrialised.\u003c/p\u003e \u003cp\u003eThis technique has been further improved by spraying water into the electrode before placing it onto the cold plate (Apply gentle pressure on the electrode and peel the Al current collector (Figure S3)). For the same electrode scrap, the amount of water and the freezing time are reduced to 0.02 mL/cm2 and 10s, respectively.\u003c/p\u003e\n\u003ctable border=\"1\" cellspacing=\"0\" cellpadding=\"0\" width=\"576\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.159722222222221%\"\u003e\n \u003cp\u003eNo.\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"14.756944444444445%\"\u003e\n \u003cp\u003eElectrode\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.319444444444443%\"\u003e\n \u003cp\u003eBinder\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.493055555555557%\"\u003e\n \u003cp\u003ePorosity(%)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"21.354166666666668%\"\u003e\n \u003cp\u003eCoating thickness (um)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"22.916666666666668%\"\u003e\n \u003cp\u003eContact Angle (\u003csup\u003eo\u003c/sup\u003e)\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.159722222222221%\"\u003e\n \u003cp\u003e1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"14.756944444444445%\"\u003e\n \u003cp\u003ePW\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.319444444444443%\"\u003e\n \u003cp\u003eCMC/SBR\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.493055555555557%\"\u003e\n \u003cp\u003e25\u0026plusmn;2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"21.354166666666668%\"\u003e\n \u003cp\u003e80\u0026plusmn;3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"22.916666666666668%\"\u003e\n \u003cp\u003e70.74\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.159722222222221%\"\u003e\n \u003cp\u003e2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"14.756944444444445%\"\u003e\n \u003cp\u003eHC\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.319444444444443%\"\u003e\n \u003cp\u003eCMC/SBR\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.493055555555557%\"\u003e\n \u003cp\u003e35\u0026plusmn;2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"21.354166666666668%\"\u003e\n \u003cp\u003e50\u0026plusmn;1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"22.916666666666668%\"\u003e\n \u003cp\u003e42.85\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.159722222222221%\"\u003e\n \u003cp\u003e3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"14.756944444444445%\"\u003e\n \u003cp\u003ePW\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.319444444444443%\"\u003e\n \u003cp\u003ePVDF\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.493055555555557%\"\u003e\n \u003cp\u003e30\u0026plusmn;2\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"21.354166666666668%\"\u003e\n \u003cp\u003e80\u0026plusmn;3\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"22.916666666666668%\"\u003e\n \u003cp\u003e73.01\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.159722222222221%\"\u003e\n \u003cp\u003e4\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"14.756944444444445%\"\u003e\n \u003cp\u003eNaTMO\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.319444444444443%\"\u003e\n \u003cp\u003ePVDF\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.493055555555557%\"\u003e\n \u003cp\u003e35\u0026plusmn;1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"21.354166666666668%\"\u003e\n \u003cp\u003e75\u0026plusmn;1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"22.916666666666668%\"\u003e\n \u003cp\u003e50.36\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.159722222222221%\"\u003e\n \u003cp\u003e5\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"14.756944444444445%\"\u003e\n \u003cp\u003eEoL Graphite\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.319444444444443%\"\u003e\n \u003cp\u003ePVDF\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.493055555555557%\"\u003e\n \u003cp\u003e28\u0026plusmn;1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"21.354166666666668%\"\u003e\n \u003cp\u003e75\u0026plusmn;1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"22.916666666666668%\"\u003e\n \u003cp\u003e25.86\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd width=\"8.159722222222221%\"\u003e\n \u003cp\u003e6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"14.756944444444445%\"\u003e\n \u003cp\u003eLTMO\u0026nbsp;\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.319444444444443%\"\u003e\n \u003cp\u003ePVDF\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"16.493055555555557%\"\u003e\n \u003cp\u003e35\u0026plusmn;1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"21.354166666666668%\"\u003e\n \u003cp\u003e70\u0026plusmn;1\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd width=\"22.916666666666668%\"\u003e\n \u003cp\u003e75.85\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n\u003c/table\u003e\u003c/br\u003e\n \u003cp\u003eThe success of the method in allowing efficient delamination is facilitated by the fact that water can penetrate the electrode, and when water freezes into ice, water molecules become arranged into an organized 3D network, which creates more hydrogen bonds between ice and particles surface and a strong bonding network in the porous electrode as illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea. Furthermore, the expanded volume from water to ice (nearly 9%) creates extra pressure within particles.\u003c/p\u003e \u003cp\u003eTo confirm this, adhesion measurements were carried out with tape-peeling at room temperature and ice-stripping at -5\u003csup\u003eo\u003c/sup\u003eC. The adhesion forces were recorded when the whole black mass was peeled/stripped off from the current collector. For ice-stripping, the substrate was cooled to ~ -5\u003csup\u003eo\u003c/sup\u003eC before the test. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb-\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e shows the distance between the electrode and cold substrate, temperature \u003cem\u003evs\u003c/em\u003e. time during the measurement. When the wetted electrode disc (d\u0026thinsp;=\u0026thinsp;8mm) surface was in contact with the cold surface, the substrate temperature increased and became stable in 5 seconds, indicating successful heat transfer and resulting in the water in the electrode being frozen. The electrode was then stripped off after a few seconds to measure the adhesion between the black mass and Al foil. With increasing distance, the pull-off force was sharply increased till the black mass delaminated from the current collector (Fig.\u0026nbsp;\u0026lt;link rid=\"fig2\"\u0026gt;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u0026lt;/link\u0026gt;\u003c/span\u003eb-\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e). During the ice-stripping process, the water penetrates the porous electrode, providing a stronger cohesive bond than the electrode's adhesive bond to the current collector. This results in the porous electrode components remaining on the cold surface after the current collector is stripped off. To further test the versatility of this delamination method, several different lithium and sodium electrodes from scrap or end-of-life, Prussian White (PW)-CMC/SBR, Hard Carbon (HC)-CMC/SBR, PW-PVDF, Sodium transition metal layered oxide (NaTMO)-PVDF, Lithium transition metal layered oxide (LTMO)-PVDF and Graphite-PVDF were also tested. The peel-off forces at room temperature and at -5\u003csup\u003eo\u003c/sup\u003eC were compared, as illustrated in Figure S4 and Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec. The force was reduced after the electrodes were frozen in most of the cases due to the stronger cohesive bond within the black mass from frozen water. However, there are exceptions, such as HC-CMC/SBR and LTMO-PVDF, where the pull-off force increased after freezing. The electrodes' porosity, thickness and contact angles were recorded as listed in Table\u0026nbsp;1 to understand the correlations. However, more coatings are required to obtain statistical results.\u003c/p\u003e \u003cp\u003eAs a full-cell case study, the ice stripping delamination process was evaluated for a PW-HC A7 end-of-life Na-ion pouch cell. The cell was stabilised and opened, and the electrodes were removed before washing in IPA and then drying, as shown in Figure S5. The effect of the ultrasound-assisted delamination process (hammer (ball) milling) on the efficiency and the impact on the recovered materials was investigated and compared with the ice-stripping process. For the former, multiple steps, electrode resize, ultrasound-assisted milling delamination, current collector removal and binder removal, were processed as presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e. Moreover, some steps were required to be repeated a few times to maximize the delamination efficiency in this case. On the other hand, the ice-stripping process was straightforward. The compound separation efficiency of the coating is calculated using the equation below.\u003cdiv id=\"Equa\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equa\" name=\"EquationSource\"\u003e\n$$CSEcoating=\\frac{mass of separated coating}{initial mass of coating}$$\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIf we take the HC-CMC/SBR coating as an example. Only 53% separation efficiency was achieved through ultrasound-assisted ball-milling delamination, whereas the ice-stripping technique can achieve a separation efficiency as high as 96% (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e). The coating separation efficiency via the ice-stripping method was also calculated with several other electrodes extracted from commercial cells, Calb (LFP), Thunder Sky (LCO), UKBIC (NMC) and Nissan (NMCA), and presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb. High recovery yields were obtained at 98%, 100%, 93% and 95%, respectively. The delamination efficiency of thick electrodes can be improved by increasing the wetting time with more water. Porosity is considered a key factor as it allows water to penetrate the pores and freeze when the temperature drops. The electrode porosity of the commercial electrodes was all in the range of 25\u0026ndash;35% (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb), which the results show is sufficient to allow delamination of all the electrodes examined, illustrating the versatility of this technique.\u003c/p\u003e \u003cp\u003eThe reclaimed PW and HC materials were then characterised to examine any changes in morphology and crystal structures (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAfter delamination of the PW cathode and HC anode, the black masses were washed and centrifuged several times with water to remove the binders. The final reclaimed PW and HC power were dried at 120\u0026deg;C overnight. The XRD pattern of reclaimed PW shows cell symmetry change compared to the pristine PW, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea. In line with this, the EDS results show that the average value of the Na/Fe ratio in the reclaimed PW power is lower at ~\u0026thinsp;0.33, indicating Na loss from battery use and during/after the delamination process. Thus, the reclaimed PW powder is the lower Na content cubic phase rather than the as-received monoclinic phase. The HC reclamation is much simpler as the presence of water has less of an effect on the structure of HC, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb. Figures\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec and \u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed display the morphology of the PW coating from end-of-life cells before delamination and pristine PW powder. Figures\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee and \u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef show the morphologies of the reclaimed PW powder via ultrasound-assisted ball-milling and ice-stripping techniques. The ice-stripping technique maintains PW's morphology and particle size, which is beneficial for subsequent direct recycling processes. Some unevenly distributed white stains were observed on the HC anode after drying, likely from Na plating during cell operation and SEI components after exposure to air during disassembly and washing processes. Nevertheless, after ice-stripping, the reclaimed HC powder maintained both the particle size and morphology.\u003c/p\u003e \u003cp\u003eThe morphologies of the recycled Al current collectors were also studied, and the difference between ball-milling and ice-stripping delamination techniques was compared, as shown in Figure S6. Micro-wrinkles were observed on the Al surface after ball-milling, as shown in Figure S6a, which came from the zirconium balls, causing damage during milling. In addition, some un-delaminated PW powders were observed in some areas on the Al current collector (Figure S6b). These observations indicate that insufficient delamination was achieved from the ball-milling procedure. The damaged Al also reduces the chances of the current collector being directly re-used or re-manufactured for subsequent new battery production. Conversely, the Al current collector remained flat without wrinkles after ice-stripping at low temperatures (Figure S6c). After cold-plate delamination, the Al current collector surface remained flat, as shown in Figure S6d. This suggests that ice-stripping is more effective than ultrasound-assisted ball-milling as a delamination technique and offers more possibilities in current collector reuse.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe reclaimed PW (re-PW) and reclaimed HC (re-HC) were assessed for direct recycling possibilities and re-manufactured into an electrode with CMC/SBR binders. The pristine and recovered PW voltage profiles are compared. Galvanostatic charge and discharge profiles of re-PW showed less distinctive and much shorter plateaus, indicating lower Na contents in the reclaimed materials, consistent with the XRD results (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea). This indicates that resodiation is required to recover performance.\u003c/p\u003e \u003cp\u003eThe re-HC was also tested in a half cell in the voltage window of 0.01V-3.00V at a specific current of 10mA/g. The HC half-cell discharge profile consists of two distinct phases, a sloping region at high voltage and a plateau at low voltage 0-0.1V, corresponding to the absorption-intercalation mechanism\u003csup\u003e\u003cspan additionalcitationids=\"CR29\" citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e\u003c/sup\u003e. The initial reversible capacity of re-HC is 245.5 mAh/g compared to 291.1 mAh/g achieved in pristine HC half-cell, as observed in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e5\u003c/span\u003eb. The capacity deviation and cycling stability presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e5\u003c/span\u003ec are likely due to the unwashed impurities in the reclaimed HC. The re-HC anode was also tested in a full cell configuration to avoid the challenges (high polarization) associated with testing \u003cem\u003evs\u003c/em\u003e. Na metal. The 1st charge-discharge profile of the PW/re-HC and PW/pristine HC are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e5\u003c/span\u003ed. The full cell assembled with re-HC gave similar profiles as the one with pristine HC, and the capacity was 121.8 and 128.6 mAh/g, respectively. However, the capacity decreased with time, and 70% of the capacity remained after 50 cycles for the PW/re-HC, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e5\u003c/span\u003ee. This is likely due to residual binders and SEI layers in the re-HC powers. Further heat treatments are required to eliminate all the non-conductive binder polymers remaining in the reclaimed HC powers to restore the material to the equivalent of the original pristine material, which will be the subject of further studies. Nevertheless, the work illustrates that the ice stripping approach is an effective initial recovery step towards this direct recycling regeneration.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003eSustainability and environmental impact\u003c/h2\u003e \u003cp\u003eDue to the physical black mass delamination and the low operation temperature of -10 to 0\u003csup\u003eo\u003c/sup\u003eC ice-stripping method does not release any VOCs (volatile organic components) and environmentally harmful toxins that can be produced through high-temperature black-mass burning\u003csup\u003e\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e, such as styrene, acrylates, unsaturated volatiles, or fluorinated products in the binder was fluoride-based. Moreover, due to technology flexibility and chemically non-destructive conditions, any black mass composition can be freeze-induced and delaminated from the current collector without chemical transformation or decomposition. Additionally, this procedure minimises the generation of solid or gaseous wastes. The carbon footprint for the ice-stripping process consists only of carbon emission due to energy consumption to cool the surface down to operating temperature. Measurement of electricity for the ice-stripping method was carried out using specialized meters that allow continuous recording from the beginning when the machine is turned on until the whole delamination process is completed. 0.025 kWh electricity consumption was recorded when 104g black mass was delaminated with the ice-stripping method. On the other hand, additional energy consumption, such as ethylene glycol (EG)\u003csup\u003e\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e manufacturing (0.36 kg CO\u003csub\u003e2\u003c/sub\u003e/kg\u003csup\u003e31\u003c/sup\u003e), need to be taken into consideration for the wet-chemical delamination process. Furthermore, the ice-stripping method does not require any harmful chemicals that can be found in pyrometallurgy and hydrometallurgy. The cooling agent varies from chemical cooling agents, closed-circuit Stirling engine or CO\u003csub\u003e2\u003c/sub\u003e\u003csup\u003e32,33\u003c/sup\u003e. Such newer methods can reduce the environmental impact by more than four thousand times. It can reduce even further and reach zero carbon emission when taking advantage of the winter season in some Northern countries, where the temperature naturally drops to sub-zero degrees Celsius for a minimum of three months.\u003c/p\u003e \u003cp\u003eThe ice stripping process has been demonstrated at the electrode sheet level on a small scale. However, there is potential to scale this to a continuous process, which is particularly useful for scrap electrodes. The constant coating from the manufacturing of electrodes, if needed to be scrapped, could be fed through either 1) an ice stripping roller and the double-sided coatings delaminated simultaneously or 2) a cold belt to delaminate side-by-side. Stripping could also be considered before drying, as the water or solvent could freeze and be stripped away from the current collector before entering the drying zone. Examples are given in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e6\u003c/span\u003e. This continuous process further improves the energy cost and is used to reclaim material which can be directly reused in the manufacturing process with very little further processing.\u003c/p\u003e \u003c/div\u003e "},{"header":"Conclusions and outlook","content":"\u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003cp\u003eHere, we present a novel reverse-thought concept for the electrode delamination process for battery direct recycling. Rather than the traditional elevated-temperature heat treatment process, \u0026lsquo;Ice-stripping\u0026rsquo; involves wetting an electrode and cooling the temperature to sub-zero to freeze the water. The frozen water in the electrode forms a strong cohesive bond, ensuring that the weaker bond between the coating and current collector foil is broken preferentially when stripped off the surface.\u003c/p\u003e \u003cp\u003eIn this work, the ice stripping process underwent several iterations to reduce separation time, improve black mass recovery efficiency and reduce water waste. The process has been tested with various lithium and sodium-ion positive and negative electrodes, illustrating the approach's success for both PVDF and CMC-SBR binder systems. Initially, the concept was demonstrated using a tray of water; the electrode was placed on top and then frozen, the porous electrode remained bonded to the ice, and the current collector was peeled away. Further improvements were made by moving to a cold surface, where a wetted electrode was frozen and peeled. The time was reduced from 5 minutes to 30 seconds by spraying water on the surface of the electrode, hence reducing time, energy, and waste.\u003c/p\u003e \u003cp\u003eWhen used in a case study using an end-of-life A7 sodium-ion pouch cell, high separation efficiency (96%) was achieved from the surface ice-stripping delamination compared to traditional ball milling (56%), and the effect upon the morphology of the reclaimed materials minimal. The reclaimed cathode and anode materials were directly reused and remanufactured into full battery cells, and the preliminary results show great potential for active material direct recycling.\u003c/p\u003e \u003cp\u003eCompared to other delamination methods that have been reported, the ice-stripping technique offers several advantages:\u003c/p\u003e \u003cp\u003e \u003cul\u003e \u003cli\u003e \u003cp\u003eHigh delamination yield.\u003c/p\u003e \u003c/li\u003e \u003cli\u003e \u003cp\u003eHigh purity of recovered materials with original morphology and size can be directly recycled.\u003c/p\u003e \u003c/li\u003e \u003cli\u003e \u003cp\u003eLimited water waste and virtually no contamination\u003c/p\u003e \u003c/li\u003e \u003cli\u003e \u003cp\u003eGood current collector grade for recovery and recycling or even direct reuse for small-scale R\u0026amp;D work.\u003c/p\u003e \u003c/li\u003e \u003cli\u003e \u003cp\u003eBinder agnostic approach, even capable of use to delaminate coatings containing non-water-soluble binders, such as PVDF.\u003c/p\u003e \u003c/li\u003e \u003cli\u003e \u003cp\u003ePossibility to scale up for battery recycling of electrode scraps from gigafactories and end-of-life batteries.\u003c/p\u003e \u003c/li\u003e \u003c/ul\u003e \u003c/p\u003e \u003cp\u003eThis work provides evidence of a novel and sustainable promising delamination process, which can become the key first stage in a direct recycling process for both Na-ion and Li-ion batteries.\u003c/p\u003e \u003c/div\u003e"},{"header":"Methods","content":"\u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003eElectrode scrap and cell disassembly\u003c/h2\u003e \u003cp\u003eDouble-side coated Prussian white (PW) cathode coatings and hard carbon (HC) anode coatings are provided by the project partner Warwick Manufacturing Group (WMG, University of Warwick), as well as the end-of-life A7 size pouch cells with PW and HC as cathode and anode. The PW cathode electrode consists of 93wt% PW, 3wt% CMC/SBR (1:2) binders and 3wt% C65 and the HC anode electrodes consist of 96wt% HC, 3wt% CMC/SBR (1:2) binders and 1wt% C45. The coating weights of the cathode and anode are 150 g/m\u003csup\u003e2\u003c/sup\u003e and 70 g/m\u003csup\u003e2,\u003c/sup\u003e respectively.\u003c/p\u003e \u003cp\u003eThe end-of-life A7 pouch cells were discharged and carefully opened in a fume hood after slowly releasing any gases generated during the cells' charge-discharge cycling (Figure S5a). The cell bodies were disconnected from the casing by cutting the tabs. The separator was zig-zag unwrapped to separate cathodes from anodes. The disassembled electrodes were soaked in isopropyl alcohol (IPA) overnight before drying them at 60\u003csup\u003eo\u003c/sup\u003eC in a vacuum oven overnight. The dried electrodes were then ready for the delamination process. Figure S5b shows the component flows through the cell disassembly and cell parts sorting process. Some weight losses are found after IPA soaking, as well as binder removal after the delamination process.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003eBall-milling and sonication for delamination\u003c/h2\u003e \u003cp\u003eThe electrode delamination was also carried out using the ultrasound-assisted ball-milling and sonication technique to compare the results with the newly developed \u0026ldquo;ice-stripping\u0026rdquo; process. In this process, the electrodes were cut into small pieces of roughly 1 cm\u003csup\u003e\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/sup\u003e area and placed in a beaker which was filled with DI water (H\u003csub\u003e2\u003c/sub\u003eO/Coating weight ratio is 20:1). The beaker was placed in a sonicator bath running at full power at 40\u0026deg;C for 1h. As the separation under these conditions was not sufficient, zirconia balls were added to the HDPE bottle to improve the separation efficiency; the beaker's contents were poured into it and placed on a roller mill for 3h. Further, the separated black mass and current collector were collected by filtration followed by centrifugation.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003eCharacterisation\u003c/h2\u003e \u003cp\u003eThe structural characteristics of the PW and HC before and after delamination were determined by X-ray diffraction using a Bruker D8 Advance instrument with a Cu Kα radiation source. The X-ray diffraction data were recorded at a scan rate of 1\u0026deg;min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e in the 2θ range between 10\u0026deg; and 70\u0026deg;at 40 KV and 30mA.\u003c/p\u003e \u003cp\u003eScanning electron microscopy with a field-emission SEM microscope (Sigma, Carl Zeiss, Germany) equipped with an energy-dispersive spectrometer (EDS) (Xmax 50, Oxford Instruments) was used to characterize the surface of the electrodes after cycling. SEM images were captured at 10 kV (1.6 nA) when a high-performance ion conversion and electron detector was employed or 20 kV (8.0 nA) when a secondary electron detector was employed.\u003c/p\u003e \u003cp\u003eAdhesion and cohesion were tested by the Kinexus pro\u0026thinsp;+\u0026thinsp;Rheometer. 8-mm-diameter electrodes were stuck on the probe, and tape was used to remove the coating. The force data were recorded by the Rspace software. The reclaimed PW and HC were re-manufactured into electrodes, and electrochemical characterisations were carried out using both half-cell and full-cell configurations.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003eElectrochemical characterisations\u003c/h2\u003e \u003cp\u003eThe reclaimed Prussian White (re-PW) cathode material was made into an electrode with 93wt% re-PW, 3wt% CMC/SBR binders and 4wt% C65 using a slurry cast process. The reclaimed hard carbon (re-HC) negative electrode contained (96wt% re-PW, 3wt% CMC/SBR binders and 1wt% C45). The cathodes were dried in vacuum (~\u0026thinsp;10\u003csup\u003e\u0026minus;\u0026thinsp;3\u003c/sup\u003e mbar) at 150\u0026deg;C overnight and the HC anode was dried at 120\u0026deg;C overnight prior to being transferred into a glovebox.\u003c/p\u003e \u003cp\u003eHalf-cells were first studied using 1M NaPF\u003csub\u003e6\u003c/sub\u003e dissolved in EC: DEC (1:1 V/V) as the electrolyte in the voltage window of 2.0-4.0V vs. Na\u003csup\u003e+\u003c/sup\u003e/Na for the cathode and 0.01V-3.00V vs. Na\u003csup\u003e+\u003c/sup\u003e/Na for the anode. The electrochemical performance of full cells was evaluated in 2032-type coin cells, with PW/re-PW cathode (12.7 mg/cm\u003csup\u003e2\u003c/sup\u003e), HC/re-HC anode (8.2 mg cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e), separated by Glass fiber (Whatman\u0026reg;) containing enough electrolyte to wet the components (~\u0026thinsp;100 \u0026micro;l). In each case three independently produced cells were tested to show standard deviations.\u003c/p\u003e \u003c/div\u003e "},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eNotes\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors declare no competing financial interest. A patent on this technique has been submitted.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgement\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors thank Dr Ivana Hasa and the team at WMG, University of Warwick, for providing end-of-life cells and electrode scrap. They also thank Ben Pye for helping with 3D printing and the EU\u0026rsquo;s Horizon 2020-funded SIMBA project for funding (Grant agreement ID: 963542; DOI 10.3030/963542).\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eInternational Energy Agency. 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Adv Energy Mater 11\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eRenewable A, February C (2022) Third Pa rty a nd Critica lly Reviewed Ra y pla ntMEG \u003csup\u003eTM\u003c/sup\u003e Life Cycle Assessment (LCA) Discla imer\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eCytiva Going liquid nitrogen-free for low-impact cryopreservation\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eAllen I (2023) Marlborough company goes green with its CO2 machine\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[{"identity":"024fae4d-d4c4-4878-9a89-aa47705d07e6","identifier":"10.13039/100010661","name":"Horizon 2020 Framework Programme","awardNumber":"Grant agreement ID: 963542","order_by":0}],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"University of Birmingham","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":true,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"High yield, delamination, ice-stripping, direct recycling, Na-ion battery","lastPublishedDoi":"10.21203/rs.3.rs-4504057/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4504057/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eWidespread adoption of alkali metal ion batteries poses a challenge for the recycling industry. Efficient recovery and reuse of valuable metals from end-of-life batteries and production scrap is paramount. A novel, cost-effective, fast, and scalable electrode delamination approach, 'ice-stripping,' is proposed. An electrode is wetted with water and frozen using a cold plate, then peeled. Volume expansion and the increased cohesive strength of the ice over the electrode adhesion results in 100% delamination from the current collector and recovery of electrode coatings with minimal water use, material waste, or damage. In stark contrast to conventional high-temperature methods. Its effectiveness is illustrated with Li-ion and Na-ion battery electrodes comprised of different binder systems, and the scalability is considered for scrap. A direct recycling case study for a Na-ion, hard carbon and Prussian white is presented. This innovation holds promise in meeting the escalating demand for efficient and sustainable battery recycling.\u003c/p\u003e","manuscriptTitle":"A ‘cool’ route to battery electrode material recovery","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-05-31 20:31:10","doi":"10.21203/rs.3.rs-4504057/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"1aa79b63-69df-46e3-b666-d8810aecf1c6","owner":[],"postedDate":"May 31st, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2024-05-31T20:31:10+00:00","versionOfRecord":[],"versionCreatedAt":"2024-05-31 20:31:10","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-4504057","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4504057","identity":"rs-4504057","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}