Investigation into the Properties of γ-Valerolactone and γ-Butyrolactone Imide-Based Electrolytes for Lithium-Ion Batteries

Investigation into the Properties of γ-Valerolactone and γ-Butyrolactone Imide-Based Electrolytes for Lithium-Ion Batteries | Authorea try { document.documentElement.classList.add('js'); } catch (e) { } var _gaq = _gaq || []; _gaq.push(['_setAccount', 'G-8VDV14Y67G']); _gaq.push(['_trackPageview']); (function() { var ga = document.createElement('script'); ga.type = 'text/javascript'; ga.async = true; ga.src = ('https:' == document.location.protocol ? 'https://ssl' : 'http://www') + '.google-analytics.com/ga.js'; var s = document.getElementsByTagName('script')[0]; s.parentNode.insertBefore(ga, s); })(); Skip to main content Preprints Collections Wiley Open Research IET Open Research Ecological Society of Japan All Collections About About Authorea FAQs Contact Us Quick Search anywhere Search for preprint articles, keywords, etc. Search Search ADVANCED SEARCH SCROLL Battery Energy This is a preprint and has not been peer reviewed. Data may be preliminary. 16 May 2025 V1 Latest version Share on Investigation into the Properties of γ-Valerolactone and γ-Butyrolactone Imide-Based Electrolytes for Lithium-Ion Batteries Authors : Khai Shin Teoh , Wanja Schulze 0000-0002-4025-1790 , Zihan Song , Alexander Croy , Juan Luis Gómez Urbano , Stefanie Gräfe , and Balducci Andrea 0000-0002-2887-8312 [email protected] Authors Info & Affiliations https://doi.org/10.22541/au.174740069.96800617/v1 Published Battery Energy Version of record Peer review timeline 596 views 226 downloads Contents Abstract Information & Authors Metrics & Citations View Options References Figures Tables Media Share Abstract This work presents a detailed comparative study of lactone-based electrolytes (γ‑valerolactone, GVL and γ‑butyrolactone, GBL) combined with lithium imide-based salts, namely lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium bis(fluoromethanesulfonyl)imide (LiFSI). Propylene carbonate is employed as a reference electrolyte solvent. The physicochemical properties of these electrolyte systems are determined experimentally and further calculated using our developed computational model. Besides, in-silico investigations are used to reveal valuable insights into the molecular interactions of the electrolyte components, such as self-diffusion coefficients and radial distribution functions. Furthermore, the suitability of lactone-based electrolytes for electrochemical applications is demonstrated by their promising rate capability and cycling stability over 200 cycles in graphite half-cells, especially with 1 M LiTFSI and 2 wt% vinylene carbonate. These findings support the potential of lactones as battery solvent alternatives, with GVL standing out due to its bio-based origin. Introduction Lithium-ion batteries (LIBs) represent a leading-edge technology in modern society, playing an indispensable role in daily life across diverse applications, including portable electronic devices, electric vehicles and renewable energy integration. [1] As global demand in the battery market is growing exponentially, ongoing research is focused on developing next-generation rechargeable LIBs with enhanced features, such as increased energy density, lightweight and improved safety. [2] For this goal, a key aspect in advanced battery development is the electrolyte, a fundamental component that acts as the medium facilitating ionic transport between the electrodes. [3] Modern battery electrolytes exist in various states – liquid, solid or gel – each offering unique advantages tailored to specific applications. [4] Liquid electrolytes, the most widespread category, generally consist of three primary components: conducting salt(s) that provide mobile ions, solvent(s) in which these salts are dissolved, and eventually functional additives that improve electrolyte stability, safety or interfacial compatibility. An appropriate electrolyte design is crucial, as it significantly impacts the electrochemical performance, safety and operational lifespan of the devices. [5] Lithium hexafluorophosphate (LiPF 6 ) is the most utilized conducting salt in commercial applications due to its well-balanced features, such as its excellent associated transport properties and its capability to effectively passivate the aluminum current collector. [6] It is typically dissolved in an organic solvent mixture of linear and cyclic carbonates like dimethyl carbonate (DMC), diethyl carbonate (DEC) or ethylene carbonate (EC). [3a, 7] Electrolyte additives are generally also included to fulfill specific functions, such as flame retardants or to ensure the formation of a stable solid electrolyte interphase (SEI) on the anode. [5a, 6b] Nevertheless, the inherent challenges associated with LiPF 6 due to its poor thermal stability and high sensitivity towards moisture have driven research efforts toward the development of alternative salts. [8] Among them, lithium salts with fluorinated sulfonimide anions, including lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium bis(fluoromethanesulfonyl)imide (LiFSI), have been extensively investigated in the past years. [9] These salts are well-known for their excellent thermal and chemical stability, also demonstrating a good resistance to spontaneous hydrolysis. From an economic perspective, the steadily reducing cost of these salts has positioned them as a strong competitor to LiPF 6 . [10] However, their inability to passivate aluminum current collectors at high potentials poses a drawback to their use. [6b, 11] Besides technical limitations, increasing attention has been given to the environmental impact of imide-based salts. Despite widespread research on these compounds, their classification as per- and polyfluoroalkyl substances (PFAS) has led to strict regulations enforced by the European Chemicals Agency. [12] In particular, the strong C-F bonds in LiTFSI contribute to its significant environmental persistence, posing the risk of groundwater contamination and bioaccumulation. [13] However, these concerns could be addressed by adopting suitable and sustainable recycling techniques that avoid its improper disposal and allow its reutilization. [14] Compared to LiTFSI, the weaker F‑S bonds in LiFSI reduce its stability against spontaneous hydrolysis. However, its reactivity with water remains considerably lower than that of LiPF 6 and becomes more pronounced only under extreme conditions (e.g., elevated temperatures or acidic and alkaline environments). [10b, 11c, 15] In modern electrolyte formulations, LiFSI is progressively incorporated as a co-salt complementary to LiPF 6 . While LiFSI contributes to higher ionic conductivity, LiPF 6 helps suppress the aluminum dissolution at higher potential. Furthermore, its cost-effectiveness and lower fluorine content support its potential as the next generation major lithium salt. [10d] In addition to conducting salts, the electrolyte performance is strongly related to the choice of solvents. As previously mentioned, different organic linear and cyclic carbonates are the predominant solvents in commercial LIBs. [5a] The linear carbonates DMC and DEC offer good transport properties, while the cyclic carbonate EC promotes the formation of a robust SEI on the graphite anode for reversible Li + de-/intercalation. [6b, 16] In contrast, propylene carbonate (PC), another widely studied cyclic carbonate, has shown detrimental effects when used as the sole solvent in battery electrolyte. It undergoes irreversible reduction at graphite anodes without forming a stable SEI. [17] As a potential alternative to carbonates, a similar cyclic ester, gamma-butyrolactone (GBL), has been proposed and widely studied, owing to its desirable physicochemical properties – similar to those of PC – such as broad liquid temperature range and relatively low flammability. However, due to its inefficiency as a standalone solvent in SEI formation, GBL has been explored in various formulations, such as in binary solvent mixtures or in combination with alternative lithium salts and functional additives. [18] While the selection and optimization of suitable solvent alternatives for LIBs remain crucial, electrolyte design should adopt a broader perspective beyond performance considerations. The origin and sustainability of solvents should be equally prioritized, as industrial-scale production of carbonate solvents primarily relies on fossil-based precursors (e.g., petroleum, natural gas). Moreover, it often involves highly toxic and energy-intensive processes. [19] For instance, PC is mainly obtained from propylene oxide, a compound with significant eco-toxicological hazards that needs careful handling. [20] Similarly, GBL production utilizes petroleum-derived raw materials (e.g., benzene). [21] Given these environmental concerns, the search for sustainable alternatives has gained increasing significance, aligning with the European Union’s emphasis on a bio-based and circular economy. [22] In this context, a potential alternative has emerged: gamma-valerolactone (GVL). As the methylated version of GBL, GVL shares comparable physicochemical characteristics with both PC and GBL. It can be readily derived from levulinic acid, one of the top 12 high-value biomass-derived platform chemical compounds. [23] Its renewable origin, combined with good biodegradability and low eco-toxicological profile, further enhances its appeal for electrolyte design. [24] Recently, its promising use as electrolyte has been successfully demonstrated in various energy storage devices. [25] Moreover, the challenge of stable SEI formation in GVL-based electrolytes can be effectively addressed by incorporating functional additives like vinylene carbonate (VC). [14] Although these solvents, especially PC and GBL, have been extensively investigated in different electrolyte configurations, a comprehensive comparison of their physicochemical, electrochemical properties and their interactions at the molecular level, when combined with aforementioned imide-based salts, is still lacking in literature. Previous studies have primarily reported LiTFSI and LiFSI individually in single/binary systems containing commonly used cyclic esters (e.g., EC, PC, DMC, GBL), and comparatively in binary carbonate mixtures. [9a, 26] However, the electrolyte systems containing GVL remain underexplored. [27] In this work, we present a systematic study comparing electrolytic solutions containing 1 M LiTFSI and 1 M LiFSI in PC, GBL and GVL. This study aims to provide a fundamental understanding of each salt in a single solvent system, contributing to the future optimization of electrolyte design. Initially, the physicochemical and electrochemical properties of these electrolytes are thoroughly investigated. Complementary, a computational study is carried out to investigate these different electrolytes and their physicochemical properties at the molecular level. Finally, their use in combination with graphite electrodes is considered to assess their suitability for electrochemical applications. Results and Discussion Electrolyte Physicochemical Characterization Despite chemical similarities of PC, GBL and GVL, they exhibit distinct solvent properties (see Table 1 ). Therefore, electrolytes containing these solvents will also differ in their characteristics. Table 1. Relevant physicochemical properties for the three neat solvents (PC, GBL and GVL). [5a, 24, 28] Chemical structure Chemical formula C 4 H 6 O 3 C 4 H 6 O 2 C 5 H 8 O 2 Melting temperature [°C] -49 -44 -31 Boiling temperature [°C] 242 204 207 Flash point [°C] 132 98 96 Dielectric constant* 64.9 39 36.5 Viscosity [mPa s]* 2.8 1.7 2.0 Vapor pressure [mm Hg]* 0.045 0.45 0.33 Density [g cm -3 ]* 1.19 1.13 1.05 LD 50 , oral for rat [mg kg -1 ] >5000 1540 8800 *Values at 25 °C. At 20 °C, the LiFSI-based electrolytes exhibit overall higher conductivity and lower viscosity compared to their LiTFSI-based counterparts, as shown in Figure 1a and 1b . For example, a conductivity of 11.0 mS cm -1 and a viscosity of 4.3 mPa s are achieved by 1 M LiFSI in GBL, outperforming 1 M LiTFSI in GBL (7.5 mS cm -1 ; 4.9 mPa s). Regardless of the imide-based salt employed, the transport properties (i.e., high conductivity, low viscosity) of the solvents follow the trend: GBL > GVL > PC. Specifically, 1 M LiFSI in GVL shows a conductivity of 6.9 mS cm -1 and a viscosity of 5.9 mPa s, while 1 M LiFSI in PC demonstrates slightly inferior transport properties (5.1 mS cm -1 ; 9.3 mPa s). As illustrated in Figure 1c , slightly higher densities are shown in LiTFSI-based electrolytes relative to their LiFSI counterparts, primarily associated with the molecular structure of the LiTFSI salt. Besides, the electrolyte densities vary with the solvent used, following the sequence: PC > GBL > GVL. Further insights into the temperature-dependent conductivity (measured from -30 °C to 80 °C), viscosity (measured from -20 °C to 80 °C) and density (measured from 0 °C to 80 °C) of the investigated electrolytes are provided in Figure S1 . Figure 1 . Measured a) conductivity, b) viscosity and c) density of LiTFSI- and LiFSI-based electrolytes with 1 M concentration in noted solvents at 20 °C. The thermal stability of the electrolytes was evaluated through thermogravimetric analysis (TGA) under nitrogen atmosphere in dynamic and isothermal modes, as depicted in Figure S2 . In general, an increasing solvent evaporation of the electrolytes is observed in the trend: GBL > GVL > PC, which correlates well with their respective vapor pressures ( Table 1 ). Besides, the difference in mass retention between LiTFSI- and LiFSI-based electrolytes is mainly attributed to their respective proportions in the electrolytes. As an indicator of the flammability of the studied electrolytes, their flash points were also measured. Despite minor differences between the LiTFSI- and LiFSI-based electrolytes, those in lactone solvents achieve flash points above 105 °C, whereas the PC-based electrolytes have flash points ranging from 140 – 150 °C. Although flash point is not the sole factor that defines the safety profile of an electrolyte, the considerably enhanced flash points of the studied electrolytes, compared to conventional battery electrolytes, ensure safer handling and storage. [29] Computational Modelling Conductivity, viscosity and density values of the electrolytes were further calculated using our developed computational model. Although the calculated conductivity and viscosity underestimate the measured values, they demonstrate the same trend as for their corresponding experimentally determined results, following the sequence GBL > GVL > PC ( Figures S3 and S4 ). Calculated densities deviate from the experimental values by only 0 . 01 to 0 . 06 g cm -3 ( Figure S5 ). Ultimately, the good agreement among calculated and experimentally obtained physicochemical properties served to validate the feasibility of the developed model. This, in turn, enables the derivation of additional molecular-scale parameters of the electrolyte components, such as their diffusion and structural properties. The self-diffusion coefficients ( D ) of the components in all studied electrolytes at 20 °C are presented in Table 2 , including the experimental and computed parameters. Temperature-dependent self-diffusivity of the electrolyte components is also depicted in Figure S6 . Regardless of the conducting salt employed, the self-diffusion coefficients of each component in the electrolytes follow the trend: GBL > GVL > PC, agreeing well with their transport properties ( Figure S1 vs. Figure S6 ). More in detail, the calculated diffusivity values for the solvents are about one order of magnitude larger than those of the ions. On the other hand, the self-diffusion coefficients of the lithium cation and the corresponding anion are similar, with the lithium cation exhibiting on average a value about 7% higher than that of the anions. It is noteworthy that the self-diffusion coefficients for the anions, such as D (TFSI - ) in 1 M LiTFSI in PC and D (FSI - ) in 1 M LiFSI in GVL, are in good agreement with values reported in the literature, despite the comparatively larger values obtained for the lithium cation. [27, 30] Overall, the self-diffusion of the ions in the electrolytes is strongly governed by the solvent diffusion and its associated transport properties. Table 2. Experimental and simulated physicochemical properties of the listed electrolytes in 1 M concentration at 20 °C: conductivity, viscosity, density and self-diffusion coefficients (computed), D + for the lithium cation, D - for the anion and D s for the solvent. Salt Solvent Exp. Calc. Exp. Calc. Exp. Calc. D + D - D s LiTFSI PC 4.70 3.41 9.28 7.00 1.32 1.30 0.75 0.66 3.17 GBL 7.52 6.10 4.89 3.03 1.26 1.21 1.34 1.25 5.00 GVL 6.29 4.17 6.45 5.04 1.19 1.18 0.88 0.85 3.38 LiFSI PC 5.15 3.78 7.90 6.06 1.28 1.27 0.80 0.77 3.49 GBL 11.20 5.38 4.29 2.52 1.22 1.17 1.17 1.13 5.63 GVL 6.86 4.10 5.92 6.62 1.15 1.13 0.90 0.80 3.37 Following, radial distribution functions (RDFs) were determined to analyze the average distance of specific molecular components in multi-molecular mixtures and facilitate the examination of solvation shells. Figure 2a‑c illustrate the RDFs of Li + -anion and Li + -solvent interactions for the studied electrolytes at 20 °C, by showing the probability g ( r ) of finding the corresponding anion or solvent molecules at a distance r from the Li cations. Across all electrolyte solvents studied, the largest g ( r ) peaks correspond to Li + -anion interactions, indicating a greater probability of finding the anion (TFSI ‑ or FSI ‑ ) in the first solvation shell around Li cations. The FSI ‑ anions form two distinct solvation shells around Li + at 3 Å and around 4.5 Å, whereas the TFSI ‑ anions exhibit slightly more distant solvation shells around Li + at 3.5 Å and 5 Å. This difference is probably attributed to the larger ionic size of the TFSI ‑ anion. [31] In contrast, the probability of locating solvent molecules around Li + is lower. These results align with the trends in self-diffusion coefficients of the electrolyte components ( Figure S6 ), suggesting that Li cations are preferentially associated with their counterions, as evidenced by their similar diffusion rates. [32] Besides, the solvation behavior of solvent molecules around Li cations differs among the PC-, GBL- and GVL-based electrolytes (inset of Figure 2a‑c ). Notably, the GVL solvent demonstrates two well-defined solvation shells around Li cations at 3.1 Å and 4.3 Å (inset of Figure 2c ). In comparison, GBL molecules exhibit a reduced probability in the first solvation shell at a similar distance, with a more pronounced presence observed at 4 Å around Li cations (inset of Figure 2b ). In the case of Li + -PC interactions, a clear solvation structuring of PC molecules around Li cations is located at 4.3 Å, with a much lower probability at r<4 Å, as indicated by the shoulder on the left side of the peak (inset of Figure 2a ). To further confirm the RDF findings, spatial distribution functions (SDFs) were investigated to provide three-dimensional insights into the density distribution between two interacting species. The volume slices of the corresponding Li + -solvent SDFs for LiFSI-based electrolytes are displayed in Figure 2d‑f , where red colored areas indicate a higher Li + density surrounding the solvent molecules and blue indicates low densities. In all cases, Li + predominantly coordinates with the oxygen atom of the carbonyl (‑C=O) group in the solvent molecules (denoted as position X in Figure 2d‑f ), as represented by the solvation shell at r≥4 Å in the RDFs (insets of Figure 2a‑c ). Moreover, the first solvation shell at r<4 Å for Li + ‑GVL interactions is further visualized by a significant Li + density observed around the oxygen atom in the ring of GVL molecules (position Y in Figure 2f ). However, this interaction is less pronounced in GBL and even weaker in PC molecules (position Y in Figure 2d and 2e ), as indicated by the lower probability at r<4 Å in the RDFs. Figure 2g and 2h present the SDFs of Li + and GVL around the TFSI - and FSI - anions. Similar to the behavior observed in Li + -solvent SDFs, Li cations primarily coordinate near the oxygen atoms of the anions, as indicated by the purple shades surrounding them. [33] Due to the presence of multiple oxygen atoms in each anion, individual anions can coordinate with several Li + , leading to ion clusters within the electrolyte. This could explain the lower self-diffusivity of the ions, compared to that of the solvents, as a result of stronger ionic interactions. The positional distribution of GVL molecules around the anions is also demonstrated in Figure 2g and 2h . A slightly higher probability of finding a close GVL molecule is evident around TFSI - anions compared to FSI - anions (blue regions). Overall, in the studied electrolytes, Li cations tend to coordinate with their counterions, with considerable differences in their interactions with the three solvent molecules (PC, GBL and GVL). Figure 2. a-c) Calculated Li + -anion and Li + -solvent RDFs at 20 °C for the noted electrolytes. Insets illustrate the RDFs of the Li + -solvent interactions. d‑f) Volume slices of calculated Li + -solvent SDFs for the LiFSI-based electrolytes at 20 °C. Red shade represents high densities of lithium cations while blue represents low densities. SDFs use the C-O-C bonds as the reference. g-h) Calculated SDFs of Li + (purple) and GVL (blue) around the TFSI - and FSI - anion in GVL-based electrolytes at 20 °C. All isosurfaces use a value of 6.7 times the average density of the respective component. SDFs use the centering S-N-S bonds as the reference. For the solvent, all atoms have been included in the SDF calculation. Electrolyte Electrochemical Characterization The lactone-based electrolytes were further electrochemically characterized to assess their potential use for battery applications. Previous studies have shown that the lactone solvents, GBL and GVL, similar to PC, exhibit limited capability in forming an effective SEI on the anode. [14, 18f, 34] Consequently, the use of the studied electrolytes in battery systems does not guarantee adequate performance. To enable their use in such applications, the incorporation of a functional additive, such as vinylene carbonate (VC), is necessary. Therefore, we decided to introduce 2 wt% VC into these electrolytes and use the latter formulations for the electrochemical investigations that will be reported below. It is worth mentioning that the presence of 2 wt% VC has a minimal impact on the electrolyte transport properties, density and thermal stability of these electrolytes ( Figure S7 and S8 ). The aforementioned parameters for all studied electrolytes, including their electrochemical stability window (ESW) are summarized in Table S1 . The ESW was evaluated using linear sweep voltammetry with a platinum disc as working electrode. The anodic and cathodic potential limits were determined at the current density threshold of ±0.1 mA cm -2 . In Figure 3 , when comparing the ESW of the VC-containing electrolytes, a narrower ESW is observed in LiFSI-based electrolytes compared to their LiTFSI counterparts. This phenomenon can be ascribed to the lower stability of FSI - anion, which results from the weaker S‑F bonds in the FSI - anion compared to the TFSI - anion. [35] While LiFSI-based electrolytes display ESW values ranging from 4.2 – 4.7 V vs. Li + /Li, the LiTFSI dissolved in GBL, GVL and PC exhibit a comparable ESW of approximately 5.1 V vs. Li + /Li. Besides, a comparison of Figure 3 (VC-containing) and Figure S9 (VC‑free) reveals that the addition of 2 wt% VC generally reduces the ESW of the electrolytes, particularly the anodic potential limit. This behavior can be related to the lower oxidative stability of VC. [36] Overall, the wide ESW achieved by the investigated electrolytes underlines their potential application in LIBs. Figure 3. Comparison of the experimentally evaluated electrochemical stability window for the noted electrolytes in the presence of 2 wt% VC. For full-cell battery applications, the electrolyte should withstand high potentials without inducing anodic dissolution, particularly of aluminum. However, the imide-based salts often struggle to form an effective passivation layer on aluminum, leading to corrosion issues. [37] Therefore, the VC-containing electrolytes were scanned by a staircase potential-step chronoamperometry method from 3.5 V towards higher potentials against metallic lithium, with bare aluminum foil as working electrode. As depicted in Figure S10 , no significant current evolution related to anodic dissolution was observed up to 4.0 V vs. Li + /Li for the studied electrolytes. These results indicate their potential suitability when combined with lithium iron phosphate cathode, a cathode material used in commercial LIBs. However, careful consideration for the electrolyte configuration design is required for further applications involving high-voltage cathode materials. Electrolyte Investigation on Graphite Electrodes To evaluate the suitability of the studied electrolytes for battery electrodes, the VC-containing electrolytes in three different solvents (PC, GBL and GVL) were tested on graphite electrodes in a half-cell configuration. Figure S11 presents the differential capacity curves of the first galvanostatic cycle at 0.05 C for electrolytes containing 1 M LiTFSI and 1 M LiFSI with 2 wt% VC, respectively. The reversible Li + de-/intercalation in graphite for all electrolytes is validated by the presence of three distinct peaks at lower potentials (<0.5 V vs. Li + /Li), which are characteristic of the typical staging mechanism of Li + intercalation in graphite. Besides, the VC reduction, contributing to the SEI formation, is evident from the small peaks/bumps at the potential range of 1.1 – 1.5 V vs. Li + /Li (insets of Figure S11a and S11b ). It is noteworthy that the initial coulombic efficiency of the graphite half-cells employing these electrolytes ranges from 82 – 85%, comparable to that of systems using conventional carbonate-based electrolytes on graphite. [38] Figure 4a and 4b illustrate the galvanostatic charge/discharge profiles of graphite half-cells using the tested electrolytes at 0.1 C (the subsequent profiles at 1 C and 5 C are depicted in Figure S12 ). As shown, independently of the used electrolytes, the graphite electrodes exhibit the characteristic voltage profiles, indicating good reversibility during the charge/discharge process. The rate capability performance of graphite half-cells employing all studied electrolytes at various C‑rates is also reported in Figure 4 . To ensure a fair evaluation of the electrochemical performance of each electrolyte on graphite, the mean specific capacities and mean coulombic efficiencies were calculated based on the results from three independent graphite half-cells for every electrolyte. As presented in Figure 4c and 4d , both the LiTFSI and LiFSI salts show excellent rate capability, particularly up to 1 C, in three different solvents (PC, GBL and GVL), delivering comparable specific capacities. Particularly, the electrolytes containing LiTFSI achieve mean specific capacity values of approximately 250 mAh g ‑1 at 2 C, similar to their LiFSI counterparts (240 – 266 mAh g ‑1 at 2 C). It is worth mentioning that the cells can nearly restore their initial capacities at 0.1 C after experiencing the transition from higher to lower C-rates, highlighting the remarkable efficiency of these electrolytes during de‑/intercalation processes. Furthermore, the mean specific capacities at each C‑rate are presented along with the corresponding standard deviations, calculated from measurements of three individual cells for each electrolyte. Greater capacity deviations are observed at higher C‑rates, likely due to the kinetic factors within the cell. The mean coulombic efficiencies achieved by the studied electrolytes in graphite half-cells are illustrated in Figure 4e and 4f . Along with the gradual increase in coulombic efficiencies during the initial galvanostatic cycles at 0.1 C, both LiTFSI- and LiFSI-based cells maintain consistent coulombic efficiencies above 99% in the subsequent cycles. For each electrolyte, the cells exhibit almost negligible deviation in coulombic efficiency, as indicated by the minor error bars in Figure 4e and 4f . Overall, as the electrolytes based on three different solvents (PC, GBL and GVL) perform comparably, the renewable origin of the GVL solvent positions it as a viable alternative to PC- and GBL-based electrolytes. Figure 4. Measured voltage profiles at 0.1 C, mean specific capacity and the corresponding mean coulombic efficiency of LiTFSI-based electrolytes (a, c, e) and LiFSI-based electrolytes (b, d, f) in graphite half-cells against metallic lithium. The long-term stability of the studied electrolytes on graphite electrodes was assessed through the galvanostatic charge/discharge cycling at 1 C over 100 cycles. The cycling stability results for a representative cell of each electrolyte are shown in Figure 5 . For LiTFSI-based cells, lactone-based electrolytes maintain stable capacity values of around 340 mAh g ‑1 over 100 cycles, with coulombic efficiency remaining above 99.7%. In comparison, fluctuations in coulombic efficiency after 60 cycles are observed in the PC-based system ( Figure 5a ), although it retains average capacity values of 315 mAh g -1 . The exceptional cycling stability of the lactone-based electrolytes with graphite is further validated by their good retention over 200 cycles, as depicted in Figure S13 . Similar to LiTFSI-based systems, LiFSI-based electrolytes with lactone solvents show comparable capacity values ranging from 335 – 350 mAh g -1 at 1 C over 100 cycles ( Figure 5b ). Nevertheless, cycling instability in the LiFSI-based electrolytes is evident from fluctuations in coulombic efficiency over 100 cycles. This phenomenon is likely attributed to the weaker F‑S bonds in LiFSI compared to LiTFSI. Among them, the LiFSI-based system using PC as solvent displays pronounced inconsistencies in both capacity values and coulombic efficiency, evident even during the initial stages of galvanostatic cycling. These results, which could be further optimized through future electrolyte design, remark the potential of lactone-based electrolytes for their application in LIBs. Finally, it is worth noting the promising features of GVL solvent, not only demonstrating good compatibility with the imide-based salts and a stable performance with graphite anodes but also due to its bio-based origin. Figure 5. Measured long-term galvanostatic cycling at 1 C in graphite half-cells using (a) LiTFSI-based electrolytes and (b) LiFSI-based electrolytes with 2 wt% VC. Conclusions This work presented a detailed comparative study of electrolytes based on different combinations of solvents (PC, GBL and GVL) and imide-based salts (LiTFSI and LiFSI). Despite the structural similarity of the solvents, the electrolytes exhibited favorable transport properties (i.e., conductivity, viscosity), following the trend: GBL > GVL > PC. In contrast to LiTFSI-based electrolytes, higher conductivity and lower viscosity were shown by their LiFSI counterparts. The significantly elevated flash points of these electrolytes (>100 °C) offer improved safety during handling and storage. Besides, the feasibility of the computational model developed in this work has been validated. The molecular dynamics calculations presented good agreement with experimental physicochemical properties, accurately predicting trends in transport properties and densities across different electrolyte configurations. For all studied electrolytes, the components diffuse in the sequence: D (solvent) > D (Li cation) ≥ D (anion). The interactions among the electrolyte components were also analyzed. Li cations primarily coordinate with their anions, especially around the oxygen atoms of the TFSI or FSI anion. Although the probability of locating solvent molecules around Li cations is slightly lower, the cations still form distinct solvation structures, mainly with the oxygen atom in the carbonyl group of the solvent molecules. The electrochemical characterization of the electrolytes revealed that a narrower electrochemical window is displayed by LiFSI-based electrolytes (4.2 – 4.7 V vs. Li + /Li) when compared to their LiTFSI counterparts (ca. 5.1 V vs. Li + /Li). Through electrochemical assessment in graphite half-cells, the PC-, GBL- and GVL-based electrolytes achieved comparable rate capability performance with both LiTFSI and LiFSI salts. Notably, outstanding cycling stability was demonstrated by the lactone-based electrolytes, especially with 1 M LiTFSI and 2 wt% VC, retaining consistent specific capacities of 340 mAh g ‑1 over 200 cycles. In contrast, considerable cycling instability was shown by PC-based systems combined with LiFSI. Overall, these results reveal the potential of lactones, and more specifically to bio-based GVL, for their application in energy storage devices. Experimental Section Chemicals and Materials The solvents PC (Sigma-Aldrich, anhydrous 99.7%), GBL (Sigma Aldrich, ≥99%) and GVL (Sigma Aldrich, ≥99%) were dried over 3 Å molecular sieves to reduce their water content below 20 ppm, as confirmed by Karl-Fischer titration (C20 Coulometric KF Titrator, METTLER TOLEDO). Electrolyte solutions in 1 M concentration were prepared by dissolving the salts LiTFSI (Solvionic, 99.9%) or LiFSI (Solvionic, 99.9%) in PC, GBL or GVL with or without the addition of 2 wt% VC (Thermo Scientific Chemicals, 98%). Physicochemical Characterization Electrolyte conductivities were measured from -30 to 80 °C using a potentiostat (Solatron Modulab XM ECS) in combination with a climatic chamber (BINDER). For each measurement, 0.5 mL of electrolyte was transferred into a conductivity cell with a known cell constant. The alternating current resistance of the electrolyte between two parallel platinum electrodes was determined through electrochemical impedance measurements (amplitude of 5 mV, frequency range from 100 mHz to 100 MHz), resulting in the electrolyte conductivity. Electrolyte viscosities were determined over a temperature range from ‑20 to 80 °C using a rotational viscometer (Anton Paar, Modular Compact Rheometer MCR 102) at a constant shear rate of 1000 s ‑1 . Electrolyte density measurements were performed from 0 to 80 °C using a density meter (Anton Paar DMA 4100 M) based on the oscillating U-tube principle. [39] Flash points were measured by introducing 2 mL of electrolyte into a flash point tester (Normalab, NPV 310 model), following a rapid equilibrium closed cup method in accordance with the EN ISO 3679 standard. Thermal stability of the electrolytes was assessed via TGA using a simultaneous thermal analyzer (PerkinElmer STA 6000). A 10 μL sample was purged with nitrogen as carrier gas at a flow rate of 30 mL min ‑1 under a pressure of 2.2 bar. Dynamic TGA measurements were carried out from 30 to 550 °C at a heating rate of 10 °C min ‑1 . For isothermal measurements, the electrolyte sample was held at 60 °C for 24 h. Molecular Dynamics Simulations Molecular dynamics simulations were conducted using the LAMMPS software package [40] provided by NixOS-QChem [41] , utilizing the OPLS-AA force field [42] , suited for modelling liquid systems. Force field parameters for the solvents were obtained from LigParGen. [43] Specifically, for the lithium cation, the default OPLS-AA parameters were used while for the TFSI and the FSI anion, the parameters from Ref. [44] were applied. The missing parameters were adapted from Ref. [45] . The InterMol tool was used to convert the force field files to the LAMMPS format. [46] The simulation cells were initialized with randomized atomic coordinates using Moltemplate [47] and Packmol [48] . The number of molecules in the simulation cell has been adapted to fit the experimental densities. The cells were cubic boxes with periodic boundary conditions. Two cell sizes were investigated: one with initial side lengths of 50 Å (with approx. 11000 atoms) and one with 80 Å (with approx. 45000 atoms). The long-range coulombic interaction used a particle-particle particle-mesh solver with an accuracy of 10 kcal -4 mol -1 Å -1 . The pairwise neighbor lists were updated every second time step. Long-range Van-der-Waals tail correction was enabled. [49] The time step was set to 1 fs. To correct for charge screenings due to polarization effects, a charge scaling of 0.8 was applied. [44, 50] The production runs were prepared in four sequential steps. First, an energy minimization was performed. Second, an annealing step was performed for 1 ns from 100 °C to the desired temperature in the NVT ensemble, employing the Nosé–Hoover thermostat. [51] Third, an NPT equilibration with a Hoover-style barostat was performed for 3 ns. [52] In the last nanosecond of the NPT ensemble, the average cell size was computed. Afterwards, the cell was resized to the average cell size. At last, the resized cell was equilibrated in an NVT ensemble for 2 ns. To calculate viscosities, five independent trajectories – initialized with different randomized velocities – ran for 5 ns using the initial cell length of 50 Å. The conductivity calculations used the cell length of 80 Å. Here, the calculation included three independent trajectories that ran for 0 . 5 ns. Atom positions were recorded every 5 fs to calculate the self-diffusion coefficients and conductivities using the Nernst–Einstein relation. Due to the relatively large size of the simulation cell, the effects of system-size dependence [53] are negligible. It is also important to note that the self-diffusion coefficients of the solvents have been calculated from one trajectory only due to the excessive amount of solvent in the simulation and therefore tremendous trajectory sizes. Therefore, no standard deviation was included for the solvent diffusivity. Transport properties and center-of-mass RDFs were calculated using a modified version of PyLAT [54] , implementing best practices for calculating transport properties. [55] SDFs were obtained using TRAVIS. [56] Displayed error bars represent the standard deviations derived from the computed properties of independent trajectories. Electrode and Cell Preparation For graphite electrode preparation, graphite active material (C-NERGY Actilion GHDR 15) was mixed with carbon black Super P C65 (C‑NERGY, Imerys) and binder sodium carboxymethylcellulose NaCMC (CRT 2000 GA, Walocel) in water using a mass ratio of 90:5:5. A total of 1 mL distilled water was used for a total solid mass of 500 mg. The mixture was processed in a ball mill (Fritsch, Pulverisette 23) for 7 min at 50 Hz. The resulting graphite slurry was coated onto a copper foil using doctor blade, with a wet film thickness of 50 μm. The electrode film was then dried overnight under ambient conditions. Subsequently, electrode discs with a diameter of 12 mm were punched and weighed. Before being transferred into an argon-filled glovebox (Mbraun, O 2 and H 2 O <1 ppm), the electrodes were further dried overnight under vacuum at 70 °C. The active mass loading of graphite electrodes was measured to be 1.2 – 1.4 mg cm ‑2 . Cell assembly was carried out using Swagelok-type cells inside an argon-filled glovebox. Glass-fiber (Whatman GF/D) was employed as the separator, soaked with 150 μL of electrolyte in each cell. Before starting the electrochemical measurements, the cells were manually pressed with a clamp. Electrochemical Measurements The electrochemical stability window of the electrolytes was assessed in a three-electrode setup. A platinum disc served as the working electrode, an oversized activated carbon electrode as the counter electrode and a silver wire as the quasi-reference electrode. The positive and negative potential limits were determined in two separate cells using linear sweep voltammetry at a scan rate of 1 mV s ‑1 , with a current threshold of ±0.1 mA cm ‑2 . To investigate the onset potential for aluminum dissolution using the electrolytes, the chronoamperometry technique was applied to a three-electrode cell, using pristine aluminum disc as the working electrode and metallic lithium as the counter and reference electrode. The working electrode potential was stepped from 3.5 to 4.4 V vs. Li + /Li in 0.1 V increments. The cell was held at each potential for one hour, and the resulting current was recorded. The electrolytes were investigated with graphite electrodes as the working electrode in a half-cell configuration. Metallic lithium was used simultaneously as the counter and reference electrode. For rate capability tests, galvanostatic charge/discharge measurements were carried out between 0.005 and 2.0 V vs. Li + /Li at different C‑rates (0.05 to 5 C with 1 C: 372 mA g ‑1 ). The long-term stability of the cells was assessed through galvanostatic cycling for 200 cycles at 1 C. Specific capacity values were calculated with respect to the electrode active mass. For rate capability tests, it is important to note that the mean specific capacity values were calculated from three individual cells, with their corresponding standard deviations. Acknowledgements K.S.T., A.B., W.T.S. and S.G. highly acknowledge funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - Research unit FuncHeal, project ID 455748945 - FOR 5301 (projects P1 and P5). J.L.G.U. would also like to thank the German Chemical Industry Fund for the financial support through a Liebig Fellowship. Conflict of Interest The authors declare no conflict of interest. References [1] a) A. Manthiram, ACS Cent. Sci. 2017 , 3, 1063; b) G. Zubi, R. Dufo-López, M. Carvalho, G. Pasaoglu, Renewable Sustainable Energy Rev. 2018 , 89, 292; c) B. Diouf, R. Pode, Renewable Energy 2015 , 76, 375; d) S. Choi, G. Wang, Adv. Mater. Technol. 2018 , 3, 1700376.[2] a) F. Wu, J. Maier, Y. Yu, Chem. 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Table of Contents Lactone as electrolyte solvent : This work explores γ-valerolactone (GVL) and γ-butyrolactone (GBL) lithium-imide-based electrolytes for their application in lithium-ion batteries. The electrolytes and their individual components were analyzed through a wide range of techniques, including computational methods, to disclose their physicochemical, electrochemical and molecular characteristics. Their promising electrochemical performance was demonstrated in graphite half-cells, reinforcing the potential of bio-based GVL as a viable solvent alternative. Information & Authors Information Version history V1 Version 1 16 May 2025 Peer review timeline Published Battery Energy Version of Record 17 Oct 2025 Published Copyright This work is licensed under a Non Exclusive No Reuse License. Collection Battery Energy Keywords bio-based electrolyte graphite imide lactone lithium-ion battery Authors Affiliations Khai Shin Teoh Friedrich-Schiller-Universitat Jena View all articles by this author Wanja Schulze 0000-0002-4025-1790 Friedrich-Schiller-Universitat Jena View all articles by this author Zihan Song Friedrich-Schiller-Universitat Jena View all articles by this author Alexander Croy Friedrich-Schiller-Universitat Jena View all articles by this author Juan Luis Gómez Urbano Friedrich-Schiller-Universitat Jena View all articles by this author Stefanie Gräfe Friedrich-Schiller-Universitat Jena View all articles by this author Balducci Andrea 0000-0002-2887-8312 [email protected] Friedrich-Schiller-Universitat Jena View all articles by this author Metrics & Citations Metrics Article Usage 596 views 226 downloads .FvxKWukQNSOunydq8rnd { width: 100px; } Citations Download citation Khai Shin Teoh, Wanja Schulze, Zihan Song, et al. Investigation into the Properties of γ-Valerolactone and γ-Butyrolactone Imide-Based Electrolytes for Lithium-Ion Batteries. Authorea . 16 May 2025. DOI: https://doi.org/10.22541/au.174740069.96800617/v1 If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download. For more information or tips please see 'Downloading to a citation manager' in the Help menu . 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