Man Singh, Sukhjot Kaur, Shivangi Mehta, Mukesh Kumar, Kush Kumar, Santosh Kumar Meena, Tharamani C. Nagaiah
{"title":"Boosted Capacity and Stability of Aqueous Iron-Sulfur Battery using DMSO as an Electrolyte Additive","authors":"Man Singh, Sukhjot Kaur, Shivangi Mehta, Mukesh Kumar, Kush Kumar, Santosh Kumar Meena, Tharamani C. Nagaiah","doi":"10.1016/j.ensm.2024.103965","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103965","url":null,"abstract":"Exploring metal-sulfur batteries with low cost, high safety, and capacity is the need of the hour for large storage applications. Iron (Fe) being a highly abundant and cost-effective element, provides an excellent option as an anode material which on coupling with abundant sulfur (S) in an aqueous electrolyte will be a game-changing approach. Despite a promising outlook, the stability of Fe anode due to side reactions in aqueous electrolytes and inherent corrosion tendencies limit their performance. Herein, we have explored dimethyl sulfoxide (DMSO) as an electrolyte additive in iron percholorate (Fe(ClO<sub>4</sub>)<sub>2</sub> for aqueous Fe-S battery, which exhibited high specific capacity of 1145 mAh g<sup>-1</sup> at 50 mA g<sup>-1</sup> with remarkable cycling stability for 400 continuous cycles at 2.0 and 0.5 A g<sup>-1</sup> current densities with 72% and 98% capacity retention respectively without replacing the Fe-anode. The addition of DMSO, suppressed parasitic hydrogen evolution reaction (HER) by 6.7 times and mitigated the corrosion rate of iron electrodes by 2.2 times as evidenced by the spectroscopic and gas chromatography techniques. The molecular dynamics (MD) simulations revealed that DMSO engages the water molecules through hydrogen bonding which reduced the fraction of free water molecules available for HER and corrosion of iron electrodes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"44 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142823357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Byungseok Seo, Daehyun Kim, Seonghyun Park, Dongjoon Shin, Kyungmin Kim, Wonjoon Choi
{"title":"Electrothermally tailored lithiophilic Co/CoxOy@porous graphite composites for high-performance Li-ion/metal hybrid batteries","authors":"Byungseok Seo, Daehyun Kim, Seonghyun Park, Dongjoon Shin, Kyungmin Kim, Wonjoon Choi","doi":"10.1016/j.ensm.2024.103961","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103961","url":null,"abstract":"Li-based batteries with high energy density and cyclic stability are essential for sustainable energy systems, whereas conventional design strategies are limited in restricted capacity and dendrite formation. Herein, we report precisely tunable Co/Co<sub>x</sub>O<sub>y</sub>@porous graphite (p-G) composites fabricated by the scalable electrothermal wave (ETW) process, enabling exceptional lithiophilic properties, increased surface area, and high porosity. The optimal heating-cooling rates adjusted by the ETW parameters could surpass the decomposition temperature of precursors yet suppress the excess thermal energy density inducing the aggregation of the resulting Co/Co<sub>x</sub>O<sub>y</sub>@p-G composite, thereby offering the rapid screening of their physicochemical characteristics. The screened Co/Co<sub>x</sub>O<sub>y</sub>@p-G composites as anodes in Li-ion/metal hybrid batteries, exhibit outstanding lithiation, Li plating at high capacities, and dendrite resistance. Compared to bare p-G anodes, they enhance Coulombic efficiency and cyclic stability by 600 % in half-cell tests, while maintaining an energy density ranging from 272.59 to 240.25 Wh∙kg<sup>-1</sup> over 110 cycles in full-cell tests, representing a 153.14 % improvement. The outcomes will inspire ultrafast yet effective fabrication strategies for high-performance electrochemical cells.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"41 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142820973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qiang Fu, Fangxiang Song, Changhui Mu, Qingqing Wu, Keliang Wang, Song Li, Xianquan Ao
{"title":"Activating reversible multi-electron reaction of Na3(VO)2(PO4)2F cathode via Fe/F dual-doping for high-energy and stable sodium storage","authors":"Qiang Fu, Fangxiang Song, Changhui Mu, Qingqing Wu, Keliang Wang, Song Li, Xianquan Ao","doi":"10.1016/j.ensm.2024.103960","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103960","url":null,"abstract":"Na<sub>3</sub>(VO)<sub>2</sub>(PO<sub>4</sub>)<sub>2</sub>F cathode has garnered extensive interest for its stable structure, abundant Na<sup>+</sup> migration channels, and high working voltage, though higher energy densities are sought for commercial applications. This study enhances energy density by activating multi-electron reactions through the partial substitution of V<sup>4+</sup> and dangling O<sup>2−</sup> with Fe<sup>3+</sup> and F⁻, respectively, using a straightforward hydrothermal method. This substitution successfully activates the V<sup>3+</sup>/V<sup>4+</sup> redox couple, facilitating multi-electron reactions. The modified cathode, Na₃(VO)<sub>1.8</sub>Fe<sub>0.2</sub>(PO<sub>4</sub>)<sub>2</sub>F<sub>1.2</sub> (N(VO)<sub>1.8</sub>Fe<sub>0.2</sub>PF<sub>1.2</sub>), exhibits a reversible specific capacity of 213.3 mAh g<sup>−1</sup> at 50 mA g<sup>−1</sup>. Characterization techniques, including in situ X-ray diffraction and <em>ex-situ</em> X-ray photoelectron spectroscopy, confirm that the activated V<sup>3+</sup>/V<sup>4+</sup> redox reaction proceeds via a solid-solution mechanism. Density functional theory analysis suggests that Na<sub>3</sub>(VO)<sub>1.8</sub>Fe<sub>0.2</sub>(PO<sub>4</sub>)<sub>2</sub>F<sub>1.2</sub> offers improved electronic conductivity and structural stability, elucidating the origins of low Na<sup>+</sup> migration energy barriers and ideal diffusion kinetics. When paired with a hard carbon (HC) anode, the full cell (HC//N(VO)<sub>1.8</sub>Fe<sub>0.2</sub>PF<sub>1.2</sub>) achieves a reversible capacity of 196.6 mAh g<sup>−1</sup> and an energy density of 287.0 Wh kg<sup>−1</sup> at 50 mA g<sup>−1</sup>, demonstrating exceptional long-term cyclic stability with a capacity retention of 94.7% after 200 cycles at 500 mA g<sup>−1</sup>. This study opens new avenues for the commercial application of sodium-ion batteries (SIBs) cathodes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"19 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142820974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Advanced Direct Recycling Technology Enables a Second Life of Spent Lithium-ion Battery","authors":"Ji Shen, Miaomiao Zhou, Wei Liu, Yiliang Shi, Wenhao Tang, Yirui Deng, Ruiping Liu, Yinze Zuo, Jiujun Zhang","doi":"10.1016/j.ensm.2024.103964","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103964","url":null,"abstract":"With the emergence of the energy crisis and the rise of human environmental awareness, lithium-ion batteries (LIBs), as a new type of energy storage device, are widely used in electric vehicles (EVs), mobile electronic products and stationary energy storage devices. The demand for LIBs has dramatically increased in recent years, leading to a shortage of raw materials for LIBs and a large number of retired LIBs. Therefore, it is particularly important to recycle spent LIBs. Compared with pyrometallurgy and hydrometallurgy, direct recycling, as a more advanced technology, focuses on repairing of the electrodes of spent LIBs. However, direct recycling technology is still in the laboratory operation stage, and there are still many difficulties and challenges to overcome. Herein, we firstly highlight the importance of recycling spent LIBs from LIB market development, raw material supply, environmental impact, and economic benefits. Subsequently, starting from the failure forms and mechanisms of electrode materials, we provide a detailed summary of various direct recycling and upcycling processes, reaction principles, as well as advantages and disadvantages. Additionally, the technology for converting waste cathodes and graphite into new functional materials, a topic rarely addressed in previous reviews, is comprehensively detailed in this review. Lastly, we provide a summary of the current status of LIB recycling and present future challenges. This review may serve as a source of inspiration for researchers and enterprises to develop more advanced recycling methodologies.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"46 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816478","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Quantification of activated carbon functional groups and active surface area by TPD-MS and their impact on supercapacitor performance","authors":"Bénédicte Réty, Hui-Yi Yiin, Camélia Matei Ghimbeu","doi":"10.1016/j.ensm.2024.103963","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103963","url":null,"abstract":"Carbon oxygenated functional groups and active sites play an important role in the interactions with the electrolytes in aqueous supercapacitors. For the first time, correlations between each type of O-surface groups and electrochemical performance are established by means of thermodesorption coupled with mass spectrometry (TPD-MS). A set of five activated carbons and one soft-salt templated carbon, were studied in three different pH electrolytes, 1M H<sub>2</sub>SO<sub>4</sub>, 1M KOH and 1M Na<sub>2</sub>SO<sub>4</sub>. Linear correlations between surface groups and capacitance were found: acidic groups such as carboxylic acid and phenol-ether groups improve capacitance, whereas carbonyl-quinone groups are detrimental. Moreover, active surface area (ASA) is for the first time measured for activated carbons thanks to a new protocol, which minimises material burn-off during oxygen chemisorption. In addition, a new approach consisting in the quantification of the ASA is proposed. It has been highlighted that certain active sites are linearly correlated to an improvement of capacitance. Although the oxygen surface groups and ASA improve the capacitance via pseudo-capacitance phenomena, the capacitive mechanisms, governed by the porosity of the activated carbons, are shown to be predominant. Among all materials, the soft-salt templated carbon gives the best electrochemical performance. Indeed, it combines a large quantity of carboxylic acid and phenol-ether surface groups as well as appropriate ASA. Moreover, it has a high specific surface area (2556 m²·g<sup>-1</sup>) and optimal pore size (0.88 nm). All these characteristics, provide a high capacitance, a high rate capability and a high capacitance retention after 10,000 cycles.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"40 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142815981","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Effective Control of the Solution Environment in Aqueous Zinc-ion Batteries for Promoting (002)-Textured Zinc Growth by a Bio-Electrolyte Additive","authors":"Yarui Xiong, Weiyu Teng, Zhiwei Zhao, Shiling Xu, Yingyuan Ma, Yingzhen Gong, Dehua Li, Xun Wang, Yaoxi Shen, Zhen Shen, Yi Hu","doi":"10.1016/j.ensm.2024.103959","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103959","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) have garnered considerable interest due to their intrinsic safety features and high energy density. However, challenges such as the growth of Zn dendrites and the prevalence of parasitic reactions during cycling have impeded their broader application. This study introduces Silk Sericin (SS), a multifunctional natural protein, as an electrolyte additive designed to overcome these obstacles. Through a series of detailed experimental validations and theoretical analyses, it is demonstrated that SS molecules, rich in polar functional groups, effectively anchor onto the anode-electrolyte interphase. This anchoring leads to the formation of a stable solid electrolyte interface (SEI) layer while simultaneously modulating the coordination environment of zinc ions through strong interactions with water molecules. The adsorption energies and substantial binding affinity of SS induce a synergistic effect, preferentially orienting zinc ions deposition on the (002) plane, thereby promoting the formation of a flat and compact deposition layer. The modified Zn || Zn cells containing 1% SS exhibit exceptional durability, surpassing 5200 h of operation at 1 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup> with highly reversible Zn plating/stripping behavior. Moreover, Zn || VO<sub>2</sub> full cells deliver a high specific capacity of 213 mAh g<sup>−1</sup> at 4 A g<sup>−1</sup>, maintaining robust performances over 3800 cycles. Additionally, Aqueous zinc-ion micro-batteries (AZMBs) based on SS demonstrate superior capacity retention, underscoring their potential for advanced energy storage applications. This research presents a novel electrolyte engineering approach that combines interface control with solution environment optimization, offering an effective strategy to enhance both the reversibility and stability of Zn anodes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"73 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816404","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Preparation, Design and Interfacial Modification of Sulfide Solid Electrolytes for All-Solid-State Lithium Metal Batteries","authors":"Jianwei Li, Yuanyuan Li, Yuxiao Wang, Xiaojun Wang, Peng Wang, Lijie Ci, Zhiming Liu","doi":"10.1016/j.ensm.2024.103962","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103962","url":null,"abstract":"All-solid-state batteries (ASSBs) have garnered significant interest as a potential energy storage solution, primarily because of their enhanced safety features and high energy density. Sulfide solid electrolytes have emerged as a focal point in solid-state battery research, attributed to their exceptional ionic conductivity, wide electrochemical stability range, and robust mechanical properties. However, their practical performance is frequently limited by interfacial compatibility issues with lithium-metal anodes and challenges associated with the high-cost of sulfide solid electrolyte. Therefore, the design and optimization of low-cost sulfide solid electrolytes, as well as compatibility strategies for lithium metal anodes, are vital for broadening the application prospects of sulfide solid electrolytes. This review systematically analyses the classification and synthesis methods of sulfide solid electrolytes, focusing on low-cost synthesis approaches. Furthermore, this review examines recent advancements in optimizing the interface between sulfide solid electrolytes and lithium-metal anodes, and provides strategic insights into the optimal selection and engineering of materials for the interfacial layer of lithium-metal anodes by synthesizing the latest experimental and theoretical findings. Finally, this review provides insights into the developmental trends and future prospects of sulfide all-solid-state lithium-metal batteries (ASSLMBs), offering valuable guidance for the practical application of high-performance ASSLMBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"29 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142810008","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ultrafast cathode assembled using small reduced graphene oxide sheets enables a 2,000 C rate supercapacitor with high energy density","authors":"Mengzhao Yang, Huayan Liu, Chenxin Zhou, Haoyang Chen, Xin Chen, Qinglei Liu, Jiajun Gu","doi":"10.1016/j.ensm.2024.103951","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103951","url":null,"abstract":"To realize ultrafast supercapacitors, a series of ultrahigh-rate (≥1,000 mV s<sup>−1</sup>) anodes that break a well-known “energy vs. power dilemma” in aqueous electrolytes have been successfully developed over the past five years. However, their matching cathodes are still limited by slow ion transport dynamics and oxidation. Here, we report a series of hydrated films that comprise small sheets of reduced graphene oxide (SSs−rGO, <100 nm in average lateral size) and feature short interlayered pathways (∼100 nm) for rapid ion transport and high oxidation resistance. As the first ultrahigh-rate cathode with areal capacitance (<em>C</em><sub>a</sub>) satisfying an industrial requirement (>0.6 F cm<sup>−2</sup>), the SSs−rGO electrode (5.0 mg cm<sup>−2</sup>) delivers a <em>C</em><sub>a</sub> of 0.61 F cm<sup>−2</sup> and a gravimetric capacitance of 123 F g<sup>−1</sup> at an ultrahigh-rate of 3,000 mV s<sup>−1</sup>. Combining with a Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> anode, the cathode enables a 1.8 V ultrafast aqueous supercapacitor that delivers energy densities of 0.14 and 0.09 mWh cm<sup>−2</sup> for discharges in 1.79 and 0.97 s (∼2,000 and 3,700 C rate), respectively. These values double (at 2,000 C) and almost ten-fold (at 3,700 C) those of the ever-reported supercapacitors operating at the corresponding rates. The present strategy paves a road to ultrafast (>1,000 C) and high-energy-density supercapacitors, by which energy charge/discharge can finish within 3.6 s.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"200 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142804723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Tailoring Electrolyte Solvation of Dimethyl Sulfite with Fluoride Dominant via Electrolyte Engineering for Enabling Low-Temperature Batteries","authors":"Heng Zhang, Xiaolong Wu, Weilong Kong, Minghao Huang, Yejuan Xue, Hongfa Xiang, Zhimei Huang","doi":"10.1016/j.ensm.2024.103955","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103955","url":null,"abstract":"Carbonate electrolytes are the primary determinant for the development of low-temperate lithium metal batteries (LT-LMBs). However, conventional ethyl carbonate (EC)-based electrolytes with solvent-dominated solvation configuration suffer from sluggish reaction kinetics, severe interfacial side reactions and high Li<sup>+</sup> desolvation energy under low temperature. Herein, an EC-free and weakly solvated electrolyte consisting of LiDFOB and mixed solvents including dimethyl sulfite (DMS), ethyl trifluoroacetate (ETFA) and fluoroethylene carbonate (FEC) was designed to facilitate the reaction kinetics and stabilize the interfaces of LT-LMBs, where a fluoride-rich solvation structure including FEC, ETFA and DFOB<sup>-</sup> is formed in the designed electrolyte. Such solvation configuration could significantly facilitate the desolvation process and induce the homogeneous Li deposition by forming high ionic conductive and inorganics-rich protective film on the electrode surfaces. With such electrolyte, the Li||NCM811 cell retains a high capacity retention of 81.7% after 1000 cycles, which is far superior to the 31.3% for EC-based electrolyte. Even at -40°C, the cell exhibits a capacity of 125.7 mAh g<sup>-1</sup> with almost no capacity attenuation after 200 cycles. This work confirms the necessity of fluoride-dominated solvation structure in decreasing the desolvation energy and accelerating the ionic transfer, contributing a promising solution to the development of low-temperature LMBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"20 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797678","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tingting Xu, Kun Qin, Chunxi Tian, Liangdong Lin, Weiping Li, Liumin Suo
{"title":"Searching for the Ideal Li1+xTMO2 Cathode for Anode-free Li Metal Batteries","authors":"Tingting Xu, Kun Qin, Chunxi Tian, Liangdong Lin, Weiping Li, Liumin Suo","doi":"10.1016/j.ensm.2024.103956","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103956","url":null,"abstract":"Anode-free lithium metal batteries push the energy density higher and minimize battery production costs as low as possible. However, the fast capacity decay impedes their commercial viability, primarily due to the lack of excessive Li from the anode to compensate for the irreversible lithium loss. Thus, the Li-rich NCM cathode is a feasible way to solve the issue. In this work, to search for the ideal Li<sub>1+x</sub>TMO<sub>2</sub> cathode for anode-free Li metal batteries, we selected the two types of commonly used layered cathode materials (LiTMO<sub>2</sub>: NCM622 and NCM811) to enrich Li converting into Li<sub>2</sub>TMO<sub>2</sub> by both chemical lithiation (C-Li) and electrochemical lithiation (E-Li) methods. Our findings show that the Li-rich NCM622 lithiated by the E-Li method is an ideal choice among our candidates, which has a high lithiation degree that almost covers the entire reversible transition range from Li<sub>1</sub> to Li<sub>2</sub> without additional by-products and a negative impact on kinetic performance. Based on the above results, we further demonstrated that the Li<sub>1.33</sub>NCM622|Cu pouch cell presents a longer cycle life of more than 200 times with a high capacity retention of 74%.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"37 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797679","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}