Graphite For Lithium-ion Batteries Research Articles

Recycling lithium-ion battery graphite: Synthesis of adsorbent materials for highly efficient removal of dye and metal ions from wastewater

The fate of residual graphite derived from hydrometallurgical treatment of spent Lithium-ion batteries remains uncertain. This study dwells on the aim of identifying the potentialities of recycling residual graphite for wastewater treatment. Graphite was recovered hydrometallurgically, and new adsorption materials: graphite oxide (GO) and graphene oxide (GrO) were synthesized from the residual graphite using the chemical oxidization method. Synthesized materials showed higher interlayer spacings (GO = 0.81 nm, GrO = 0.78 nm) than the commercially available similar materials. Adsorption studies revealed higher adsorption capacities for both dye (>550 mg/g in all cases) and metal ions (highest ∼93 mg/g for Ni2+ and lowest ∼68 mg/g for Zn2+). GrO showed superior results than GO due to its high surface area and porosity despite GO having more functional groups. Moreover, produced materials showed about 97 % removal of dye and about 94 % removal of contaminated metals which are higher performance than existing commercial or similar materials. These findings highlight the promising recycling capabilities of waste graphite and suggest its potential as a substitute for natural graphite.

Is silicon worth it? Modelling degradation in composite silicon–graphite lithium-ion battery electrodes

The addition of silicon into graphite lithium-ion battery anodes has the potential to increase cell energy density. However, understanding the complex degradation behaviour in these composite systems remains a research challenge. Here, we developed a coupled electrochemical–mechanical model of a composite silicon/graphite electrode, including stress-driven crack formation and solid electrolyte interphase layer growth for each material, validated with experimental degradation data from an LG M50T cell. The model reveals self-limiting loss of silicon due to decreasing stress in the silicon as the silicon activity shifts to a lower state-of-charge. Higher C-rates can lead to lower degradation due to lower phase utilisation as voltage cut-offs are reached earlier. Increasing silicon content can reduce the stress in the silicon by distributing reaction current density over more material. Using this model, we explored whether the extra capacity from silicon is generally ‘worth’ the faster degradation compared to graphite-only electrodes. The model shows if you use the silicon, you lose it, as the higher initial capacity is rapidly lost with regular high depth-of-discharge events. However, silicon does have value if it enables full graphite utilisation without range anxiety; if high depth-of-discharge events are minimised then graphite’s superior longevity can be utilised while exploiting silicon’s high specific capacity. The model is integrated into PyBaMM (an open-source physics-based modelling platform); providing the research community and industry with the capability to reproduce our results and further explore the dynamic lifetime behaviour of composite electrodes.

Modulating the graphitic domains of hard carbons via tuning resin crosslinking degree to achieve high rate and stable sodium storage

Sodium-ion batteries (SIBs) are regarded as an outstanding alternative to lithium-ion batteries (LIBs) due to abundant sodium sources and their similar chemistry. As a most promising anode of SIBs, hard carbons (HCs) receive extensive attention because of their low potential and low cost, but their rational design for commercial SIBs is restricted by their variable and complicated microstructure, which is analogous to that of graphite in LIBs. Herein, a series of controllable HC materials derived from 3-aminophenol formaldehyde resin (AFR) were designed and fabricated. We discover that the optimized HC features expanded graphite regions, highly developed nanopores, and reduced defect content, contributing to the enhanced Na+ storage. This optimization is achieved by adjusting the resin crosslinking degree of the precursor. Specifically, a resin precursor with a higher crosslinking degree can produce HC with a larger interlayer distance, relatively higher crystallinity, and a lower specific surface area. Encouragingly, the as-optimized AFR-HC electrode manifests superior electrochemical performance in the aspect of high capacity (383 mAh·g-1 at 0.05 A·g-1), better rate capability (140 mAh·g-1 at 20 A·g-1), and high initial coulombic efficiency (82%) than other contrast samples. Moreover, the as-constructed full cell coupled with a Na3V2(PO4)3 cathode shows an energy density of 250 Wh·kg-1. Together with the simple synthesis, cost-efficiency of the precursors and superior electrochemical performance, AFR-HCs are promising for the commercial application.

Direct and rapid thermal shock for recycling spent graphite in lithium-ion batteries

Due to the rapid increase in the number of spent lithium-ion batteries, there has been a growing interest in the recovery of degraded graphite. In this work, a rapid thermal shock (RTS) strategy is proposed to regenerate spent graphite for use in lithium-ion batteries. The results of structural and morphological characterization demonstrate that the graphite is well regenerated by the RTS process. Additionally, an amorphous carbon layer forms and coats onto the surface of the graphite, contributing to excellent rate performance. The regenerated graphite (RG-1000) displays excellent rate performance, with capacities of 413 mAh g−1 at 50 mA g−1 and 102.1 mAh g−1 at 1000 mA g−1, respectively. Furthermore, it demonstrates long-term cycle stability, maintaining a capacity of 80 mAh g−1 at 1000 mA g−1 with a capacity retention of 78.4 % after 600 cycles. This RTS method enables rapid and efficient regeneration of spent graphite anodes for lithium-ion batteries, providing a facile and environmentally friendly strategy for their direct regeneration.

Study on the effect of low-temperature cycling on the thermal and gas production behaviors of Ni0.8Co0.1Al0.1/graphite lithium-ion batteries

With their high energy density and long cycle life, lithium-ion batteries (LIBs) are currently the most promising electrochemical energy storage system for electric vehicles. However, their safety and cycling performance can be significantly compromised in low-temperature environments due to lithium plating and other factors. Therefore, it is essential to study the safety of aging batteries. In this study, we focused on a commercially available high-specific-energy Ni0.8Co0.1Al0.1 cathode system battery and simulated the aging of the battery by long-term cycling at 0 ℃. This study compares and analyzes the samples on the basis of the previous ones in terms of heat production power, thermal runaway (TR) characteristics and gas production characteristics. It reveals the influence of low-temperature aging on the comprehensive performance of lithium batteries in a more comprehensive way. The results show that the charging pattern of all three characteristics is related to the aging degree of the battery. In terms of the thermal characteristics, the relative change in specific heat capacity of the aged battery is only between 0.32 % and 1.08 % compared to that of a fresh battery, so the effect of ageing on the specific heat capacity of the battery is negligible. The average heat generation power of batteries with different state of health (SOH) is not monotonically increasing with the decrease of SOH, the threshold of dramatic increase is SOH = 80 %. In terms of TR characteristics, the onset temperature of exothermic reactions (TOER) of aged batteries is significantly lower than that of fresh batteries. With the decrease of SOH, TOER also decreases gradually. Compared with batteries with different SOHs, the more seriously aged the battery safety valve opens earlier, and the TR occurs earlier. In terms of the TR gas production characteristics, the more severely aged the battery, the earlier the safety valve opens compared to a fresh battery. The most gas is produced when SOH = 70 %, which increases the risk of catastrophic damage.

Unravelling the Mechanism of Pulse Current Charging for Enhancing the Stability of Commercial LiNi0.5Mn0.3Co0.2O2/Graphite Lithium‐Ion Batteries

AbstractThe key to advancing lithium‐ion battery (LIB) technology, particularly with respect to the optimization of cycling protocols, is to obtain comprehensive and in‐depth understanding of the dynamic electrochemical processes during battery operation. This work shows that pulse current (PC) charging substantially enhances the cycle stability of commercial LiNi0.5Mn0.3Co0.2O2 (NMC532)/graphite LIBs. Electrochemical diagnosis unveils that pulsed current effectively mitigates the rise of battery impedance and minimizes the loss of electrode materials. Operando and ex situ Raman and X‐ray absorption spectroscopy reveal the chemical and structural changes of the negative and positive electrode materials during PC and constant current (CC) charging. Specifically, Li‐ions are more uniformly intercalated into graphite and the Ni element of NMC532 achieves a higher energy state with less Ni─O bond length variation under PC charging. Besides, PC charging suppresses the electrolyte decomposition and continuous thickening of the solid‐electrolyte‐interphase (SEI) layer on graphite anode. These findings offer mechanistic insights into Li‐ion storage in graphite and NMC532 and, more importantly, the role of PC charging in enhancing the battery cycling stability, which will be beneficial for advancing the cycling protocols for future LIBs and beyond.

Fabrication of Li4Ti5O12 (LTO) as Anode Material for Li-Ion Batteries.

The most popular anode material in commercial Li-ion batteries is still graphite. However, its low intercalation potential is close to that of lithium, which results in the dendritic growth of lithium at its surface, and the formation of a passivation film that limits the rate capability and may result in safety hazards. High-performance anodes are thus needed. In this context, lithium titanite oxide (LTO) has attracted attention as this anode material has important advantages. Due to its higher lithium intercalation potential (1.55 V vs. Li+/Li), the dendritic deposition of lithium is avoided, and the safety is increased. In addition, LTO is a zero-strain material, as the volume change upon lithiation-delithiation is negligible, which increases the cycle life of the battery. Finally, the diffusion coefficient of Li+ in LTO (2 × 10-8 cm2 s-1) is larger than in graphite, which, added to the fact that the dendritic effect is avoided, increases importantly the rate capability. The LTO anode has two drawbacks. The energy density of the cells equipped with LTO anode is lower compared with the same cells with graphite anode, because the capacity of LTO is limited to 175 mAh g-1, and because of the higher redox potential. The main drawback, however, is the low electrical conductivity (10-13 S cm-1) and ionic conductivity (10-13-10-9 cm2 s-1). Different strategies have been used to address this drawback: nano-structuration of LTO to reduce the path of Li+ ions and electrons inside LTO, ion doping, and incorporation of conductive nanomaterials. The synthesis of LTO with the appropriate structure and the optimized doping and the synthesis of composites incorporating conductive materials is thus the key to achieving high-rate capability. That is why a variety of synthesis recipes have been published on the LTO-based anodes. The progress in the synthesis of LTO-based anodes in recent years is such that LTO is now considered a substitute for graphite in lithium-ion batteries for many applications, including electric cars and energy storage to solve intermittence problems of wind mills and photovoltaic plants. In this review, we examine the different techniques performed to fabricate LTO nanostructures. Details of the synthesis recipes and their relation to electrochemical performance are reported, allowing the extraction of the most powerful synthesis processes in relation to the recent experimental results.

Superior initial Coulombic efficiency and areal capacity of hard carbon anode enabled by graphite-assisted carbonization for sodium-ion battery

Hard carbons are perceived as promising anode materials in sodium-ion batteries, while their practical implementation is largely impeded by the insufficient initial Coulombic efficiency (ICE). Hard carbons with self-supporting architecture are intriguing to enhance ICE owing to the omission of binder and conductive agent; whereas elaborate architecture and microstructure design are still required to further raise the ICE to the level of commercial graphite in lithium-ion batteries, especially under high areal capacity. Herein, we propose a graphite-assisted pressurization strategy during carbonization to achieve remarkable ICE and high areal capacity in resulting self-supporting cellulose tissue derived hard carbon anode. The intimate contact of graphite plate enables suitable local ordering of pseudo-graphitic nanodomains with low intrinsic defects, responsible for enhanced ICE. While the pressure-reinforced dense yet self-interwoven fibrous networks render high areal capacity. Consequently, the as-prepared self-supporting hard carbon anode displays remarkable ICE to 95% and areal capacity of 2.4 mAh cm−2, far exceeding the reported value of less than 0.8 mAh cm−2. Meanwhile, the rate and durability are not scarified under such superior ICE due to the well-manipulated pseudo-graphitic nanodomains and porous fibrous networks. The practicality is further demonstrated in coin-type and pouch-type full cells delivering high capacity and long-term stability. Our finding offers an impetus for the development of high ICE and areal capacity for sodium-ion battery anode.

Application of the Multi-Species, Multi-Reaction Model to Coal-Derived Graphite for Lithium-Ion Batteries

Graphite is a critical material used as the negative electrode in lithium-ion batteries. Both natural and synthetic graphites are utilized, with the latter obtained from a range of carbon raw materials. In this paper, efforts to synthesize graphite from coal as a domestic feedstock for synthetic graphite are reported. Domestic coal-derived graphite could address national security and energy issues by standing up domestic supply chains for battery critical materials. The performance in lithium-ion coin cells of this coal derived graphite is compared to a commercial battery-grade graphite. For the first time, a multi-species, multi-reaction (MSMR) modeling technique is applied to synthetic graphite derived from coal. Key thermodynamic, transport, and kinetic parameters are obtained for the coal derived graphite and compared to the same parameters for commercial battery-grade graphite. Modeling of synthetic graphites will allow for virtual evaluation of these materials toward production of domestically sourced graphite.

A Functional Electrolyte Containing P-Phenyl Diisothiocyanate (PDITC) Additive Achieves the Interphase Stability of High Nickel Cathode in a Wide Temperature Range.

The lithium-ion batteries (LIBs) with high nickel cathode have high specific energy, but as the nickel content in the cathode active material increases, batteries are suffering from temperature limitations, unstable performance, and transition metal dissolution during long cycling. In this work, a functional electrolyte with P-phenyl diisothiocyanate (PDITC) additive is developed to stabilize the performance of LiNi0.8 Co0.1 Mn0.1 O2 (NCM811)/graphite LIBs over a wide temperature range. Compared to the batteries without the additive, the capacity retention of the batteries with PDITC-containing electrolyte increases from 23 % to 74 % after 1400 cycles at 25 °C, and from 15 % to 85 % after 300 cycles at 45 °C. After being stored at 60 °C, the capacity retention rate and capacity recovery rate of the battery are also improved. In addition, the PDITC-containing battery has a higher discharge capacity at -20 °C, and the capacity retention rate increases from 79 % to 90 % after 500 cycles at 0 °C. Both theoretical calculations and spectroscopic results demonstrate that PDITC is involved in constructing a dense interphase, inhibiting the decomposition of the electrolyte and reducing the interfacial impedance. The application of PDITC provides a new strategy to improve the wide-temperature performance of the NCM811/graphite LIBs.

Stable cycling and low-temperature operation utilizing amorphous carbon-coated graphite anodes for lithium-ion batteries.

With the continuous expansion of the lithium-ion battery market, addressing the critical issues of stable cycling and low-temperature operation of lithium-ion batteries (LIBs) has become an urgent necessity. The high anisotropy and poor kinetics of pristine graphite in LIBs contribute to the formation of precipitated lithium dendrites, especially during rapid charging or low-temperature operation. In this study, we design a graphite coated with amorphous carbon (GC) through the Chemical Vapor Deposition (CVD) method. The coated carbon layer at the graphite interface exhibits enhanced reaction kinetics and expanded lithium-ion diffusion pathways, thereby reduction in polarization effectively alleviates the risk of lithium precipitation during rapid charging and low-temperature operation. The pouch cell incorporating GC‖LiCoO2 exhibits exceptional durability, retaining 87% of its capacity even after 1200 cycles at a high charge/discharge rate of 5C/5C. Remarkably, at -20 °C, the GC-2 maintains a specific capacity of 163 mA h g-1 at 0.5C, higher than that of pristine graphite (65 mA h g-1). Even at -40 °C, the GC-2‖LiCoO2 pouch cell still shows excellent capacity retention. This design realizes the practical application of graphite anode in extreme environments, and have a promising prospect of application.

Enabling a non-flammable methyl(2,2,2-trifluoroethyl) carbonate electrolyte in NMC622–graphite Li-ion cells by electrode pre-passivation

Pre-passivation of lithium-ion battery graphite electrodes allows for safer non-flammable electrolytes to be used in long-term operation with high performance.

Potential environmental and human health menace of spent graphite in lithium-ion batteries

The growing demand for lithium-ion batteries for portable electronics and electric vehicles results in a booming lithium battery market, leading to a concomitant increase in spent graphite. This research investigated the potential impacts of spent graphite on environmental and human health using standardized toxicity extraction and Life Cycle Impact Assessment models. The spent graphite samples were classified as hazardous waste due to the average nickel content of 337.14 mg/L according to Chinese regulations. Besides, cadmium and fluorine were the other elements that exceeded the regulations threshold. Easily ignored aluminum and heavy metal cobalt are other harmful elements according to the results of Life Cycle Impact Assessments. All the metallic harmful elements mainly exist in a transferable state. Thermogravimetry infrared spectrometry coupled with mass spectrometry was employed to recognize the emitted gases and explore gas emission behavior. Inorganic gases of CO, H2S, SO2, SO3, oxynitride, HCl, and fluoride-containing gases were detected. Sulfur-containing gases released from spent graphite were contributed by the residual sulfuric acid after leaching. The correlation between the evolution of emitted gases and the heating schedule was established simultaneously. The research comprehensively illustrates the pollution of spent graphite and provides assistance for the design of green recycling schemes for spent graphite.

Improving the Fast Charging Capability of Lithium-Ion Battery Graphite Anodes by Implementing an Alternative Binder System

An alternative binder system for water-processed graphite anodes for lithium-ion batteries was developed and electrochemically investigated in terms of fast charging capability. The conventionally used binder system for anode coatings, based on CMC and SBR, shows good rheological and mechanical properties, but is limited in its electrochemical performance with respect to high charging currents. However, a marked improvement in fast charging capability is necessary to accelerate the market share of battery electric vehicles. Therefore, we systematically developed an alternative, water-based binder system to improve the fast charging capability of graphite anodes. Thereby, the most promising alternative binder system consisting of alginate, PEO and PVP (2:1:1) showed an improvement in charging performance at 4 C (10 mA cm−2) in the CC-step by more than 150% in 2.5 mAh cm−2 research pouch cells, compared to the reference binder system consisting of CMC and SBR (1:1). The improvement in fast charging capability could be assigned to a reduced ionic pore resistance, as well as a larger active surface area, whereas the pore size distribution, the total surface area, as well as the wettability of the electrode, influence the active surface area. Furthermore, the alternative binder system reveals an improved cycling stability beyond 1,500 cycles.

The Modification of Graphite in Lithium-Ion Batteries and its Applications

Lithium-ion batteries (LIB) dominate the battery market because of their excellent performance. However, the potential safety hazard of lithium-ion batteries is still regarded as an important factor hindering their further development. Lithium-ion batteries are highly flammable. In fact, there have been multiple cases of explosions caused by lithium-ion battery which result in severe burns over the past decades. Other concerns including recyclability and low power density produces obstacles to this technology. Graphite is a material with excellent conductivity. It has many outstanding electronic and mechanical properties. The basic and applied research on graphite has become a current frontier and hotspot. Therefore, graphite is also used to modify lithium-ion batteries. Especially using graphite to modify the anode material greatly improves its original performance. This work firstly introduced the physical and chemical properties of graphite. Subsequently, how graphite can enhance the efficiency LIB was introduced. A detailed introduction was given concerning with graphite modified anode materials. This work will promote the application of graphite in lithium-ion batteries.

Recycling of spent lithium–ion battery graphite anodes via a targeted repair scheme

When lithium–ion batteries (LIBs) reach the end of their life, a lot of hazardous wastes will be generated. Unfortunately, the recovery of spent graphite (SG) anodes is always neglected despite the rather high production cost of battery–grade graphite. In this work, we for the first time propose a novel targeted repair scheme by systematically characterizing and analyzing the structure and composition of SG. The results show that the repair scheme achieves effective SG repair and the repaired graphite anode displays excellent lithium storage performance, which can be comparable to that of commercial graphite. In addition, the scheme is evaluated to reduce energy consumption by 79 % and harmful pollutant emission by 90 % as compared to previously reported solutions. Obviously, our work provides a feasible solution for the recovery of graphite anodes from spent LIBs by understanding the failure characteristics of graphite anodes.

Metal-organic framework-derived Nickel Diselenide grown in situ on carbon for high-performance Li storage

The creation of innovative anodes to replace graphite in lithium-ion batteries (LIBs) is necessary to meet the rising demand for energy storage devices. Based on the large Li storage capacity, transition metal selenides (TMSs) draw considerable interest for LIBs. However, volume expansion of TMSs during the cycling process hinders their large-scale commercial application for LIBs. Herein, the NiSe2 particle grown in situ on the porous carbon framework (NiSe2@C) is prepared by selenization of metal-organic frameworks (MOFs) in an argon atmosphere. NiSe2@C exhibits a high reversible Li storage capacity (770 mAh g−1 at 200 mA g−1after 100 cycles), long cycling life (308 mAh g−1 at 1 A g−1 after 1000 cycles), and good rate capability (214 mAh g−1 at 5.0 A g−1). The long cycling performance can be attributed to the fact that NiSe2@C can withstand volume expansion during the Li+ insertion and desertion process. Furthermore, cyclic voltammetry (CV) tests at various scan rates are conducted to investigate the kinetics of NiSe2@C for LIBs, indicating that the Li storage behaviour of NiSe2@C is primarily controlled by the capacitive process. The fabrication of the TMS@C composites by selenization of MOFs is a potential way to obtain anodes for high-performance Li storage.

High-performance expanded graphite regenerated from spent lithium-ion batteries by integrated oxidation and purification method

Currently, the recycling of spent lithium-ion batteries (LIBs) has mainly been focused on the extraction of precious metals, such as lithium, cobalt and nickel from cathodes, while the waste graphite anode has been overlooked due to its low-cost production and abundant resources reserve. However, there are enormous potential value and pollution risk in the view of graphite recycling. Thus, we propose an original method to prepare expanded graphite (EG) as new anode material generated from waste graphite in LIBs which integrates the oxidation and purification in one-step. By regulating the oxidizability of potassium hypermanganate in the sulfur-phosphorus mixed acid system, the expansion of graphite and removal of impurities are realized simultaneously and thoroughly. As anticipated, the shortening of preparation process and purification procedure can also reduce the generation of polluting substances and production cost. It displays excellent electrochemical performance (reversible capacity of 435.8 mAh·g−1 at 0.1C and long-term cycling property of 370 mAh·g−1 at 1C after 1000 cycles), which is even higher than that of pristine commercial graphite. This delicate strategy of high-performance expanded graphite recycling achieves the integration of purification and value-added processes, providing the instructive guide to regenerate industrial-grade anode materials for the increasing LIBs demand in the future.

Towards a Fully-Quantitative Picture of SEI Chemical Composition and Its Native Li+ Exchange in Liquid Electrolytes

Energy density requirements for next-generation batteries make the lithium (Li) metal anode a key candidate to replace graphite in lithium-ion batteries due to Li’s improved capacity (3,860 mAh/g vs. 372 mAh/g). However, Li anodes display lower Coulombic efficiency (CE, <99.9%) than graphite (>99.95%),1 resulting in faster loss of reversible Li over cycling. This shortfall derives from parasitic Li-electrolyte reactions that lead to accumulation of inactive Li0 and electrolyte-derived byproducts, which result in the formation of a native solid electrolyte interphase (SEI) on Li. In addition to contributing to capacity loss, the SEI also has the important role of regulating Li+ exchange between Li and the electrolyte, which may affect Li plating morphology and reversibility.2 Despite significant advances, the framework on which the understanding of SEI composition and function was built has largely been qualitative, often due to experimental limitations and/or lack of self-consistent techniques.To bridge this gap, my thesis work focuses on advancing experimental techniques and methodologies to precisely quantify the chemical composition and rates of Li+ exchange in native SEIs. Using a combination of cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS), self-consistent rates of Li+ exchange are reported across a wide range of electrolytes.3 Notably, we found that native SEIs formed in high CE electrolytes displayed consistently higher rates of Li+exchange. The improved transport in high-CE electrolytes was found to emerge after an SEI formation cycle, and amplified over cycling, indicating that fast Li+ exchange is beneficial to Li reversibility.In order to identify which SEI phases grant high-CE electrolytes their beneficial functional properties, we also developed and expanded upon a series of titration experiments based on GC, ICP-AES and NMR that can track an extended array of key SEI phases: semicarbonates (ROCO2Li), lithium carbide (Li2C2), olefins (RLi), LiF, P-containing phases, and total Li loss.4 In the 1 M LiPF6 EC/DEC electrolyte, we demonstrate chemical resolution up to 71% of Li loss and 33% of SEI loss. Among the quantifiable SEI phases, ROCO2Li was consistently the major phase, but its proportions were invariant with CE. Instead, Li2C2, a minor phase, exhibited clear inverse correlation with CE. We also demonstrate further quantitative chemical resolution can be achieved with online GC, which can differentiate between the different types of semicarbonate (i.e., which “R” in ROCO2Li) and alkoxide phases that form on Li.5 Altogether, these results add further nuance to the current understanding of SEI composition and their function, which we hope will allow more quantitative electrolyte design. Hobold, G. M.; Lopez, J.; Guo, R.; Minafra, N.; Banerjee, A.; Shirley Meng, Y.; Shao-Horn, Y.; Gallant, B. M., Moving Beyond 99.9% Coulombic Efficiency for Lithium Anodes in Liquid Electrolytes. Nat. Energy 2021, 6 (10), 951-960. Zheng, J.; Kim, M. S.; Tu, Z.; Choudhury, S.; Tang, T.; Archer, L. A., Regulating Electrodeposition Morphology of Lithium: Towards Commercially Relevant Secondary Li Metal Batteries. Chem. Soc. Rev. 2020, 49 (9), 2701-2750. Hobold, G. M.; Kim, K.-H.; Gallant, B. M., Beneficial Vs. Inhibiting Passivation by the Native Lithium Solid Electrolyte Interphase Revealed by Electrochemical Li+ Exchange. 2022. Hobold, G. M.; Gallant, B. M., Quantifying Capacity Loss Mechanisms of Li Metal Anodes Beyond Inactive Li0. ACS Energy Lett. 2022, 7 (10), 3458-3466. Hobold, G. M.; Khurram, A.; Gallant, B. M., Operando Gas Monitoring of Solid Electrolyte Interphase Reactions on Lithium. Chem. Mater. 2020, 32 (6), 2341-2352.

A S-phenyl Benzenethiosulfonate (SPBS)-containing electrolyte enhances the temperature performance of LiNi0.8Co0.1Mn0.1O2/graphite batteries by regulating the electrode interfaces

A sulfur-containing compound S-phenyl Benzenethiosulfonate (SPBS) is developed as an electrolyte additive to improve the electrochemical performance of LiNi0.8Co0.1Mn0.1O2 (NCM811)/graphite lithium-ion batteries (LIBs) in a wide temperature range. Compared with the batteries without SPBS, the capacity retention of the batteries containing SPBS increases from 58.15% to 91.48% after 1100 cycles at 25 °C and from 70.09% to 80.68% after 550 cycles at 45 °C. And after stored at 60 °C for 7 days, 14 days, and 28 days, the capacity retention rate and capacity recovery rate of the batteries containing SPBS are obviously improved. In addition, it is also shown that SPBS can inhibit the internal polarization and capacity attenuation of the batteries during low-temperature cycling, the capacity retention of the batteries containing SPBS increases from 46.3% to 81.9% after 100 cycles at −10 °C. The experimental and theoretical results demonstrate that SPBS facilitates the construction of high-quality electrode-electrolyte interfaces, reduces the electrolyte decomposition and inhibits the impedance increase. The excellent temperature performance of NCM811/graphite LIBs means the promising application prospect of SPBS-containing electrolyte.