{"title":"Molecular Bridging Interface Layer Engineering for Improved Stability of Zn Anodes","authors":"Jun Wang, Xiuyang Zou, Shen Zhang, Biyu Jin, Jiao Huang, Yongyuan Ren, Feng Gao, Yang Hou, Jianguo Lu, Xiaoli Zhan, Qinghua Zhang","doi":"10.1016/j.ensm.2025.104027","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104027","url":null,"abstract":"To achieve commercial-grade lifespan and charge-discharge efficiency in aqueous zinc-ion batteries, a crucial prerequisite is establishing a robust and compatible electrode-electrolyte interface to mitigate the challenges posed by excessive dendrite proliferation and side reactions. Herein, we ingeniously engineer a durable interface layer on the zinc foil surface through an in-situ chemical grafting approach using silane as a molecular bridge (SG@Zn. This functionalized polysilane layer successfully welds the metallic substrate and the organic segments, fostering a highly compatible interface via robust Si-O-Zn bonds, serving as a shielding layer to protect the electrode from corrosion. The silane framework facilitates the uniform anchoring of subsequent zinc-affinitive functional groups at the molecular level, which not only brings a rapid zinc ion reaction kinetics but also ensures dual enhancement against expansion inhibition and dendrite penetration. Consequently, the symmetrical battery thus showcases superior reversibility in stripping/planting processes and demonstrates negligible voltage fluctuations at various currents and capacities. The MnO<sub>2</sub>-based full batteries maintain a capacity of 200 mAh g <sup>-1</sup> with a negligible cyclic capacity decay rate of 0.017% over 700 cycles at 1 C. This work offers a valuable perspective on interface engineering for high performance aqueous zinc-ion batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"29 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967950","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}
Kehao Tao, Wei He, An Chen, Yanqiang Han, Jinjin Li
{"title":"Harnessing Lateral Transfer Learning for Pioneering Solid Electrolyte Interphase Innovation","authors":"Kehao Tao, Wei He, An Chen, Yanqiang Han, Jinjin Li","doi":"10.1016/j.ensm.2025.104034","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104034","url":null,"abstract":"The rapid growth in energy storage demands, particularly in electric vehicles and portable electronics, has positioned solid-state batteries (SSBs) at the forefront of cutting-edge research. Compared to conventional lithium-ion batteries, SSBs offer significant advantages, including enhanced safety, higher energy density, and extended cycle life. However, a major challenge lies in identifying solid electrolyte interphase (SEI) materials with high shear modulus (G<sub>s</sub>) and exceptional ion transport properties to prevent lithium dendrite formation and improve overall battery performance. Here, we introduce an innovative approach utilizing lateral transfer learning to accelerate the discovery of high-performance SEI materials. Traditional machine learning models often require large datasets, which are typically unavailable for specialized material properties like G<sub>s</sub>. To address this, we applied lateral transfer learning, transferring knowledge from models trained on larger datasets (bandgap data) to predict G<sub>s</sub> within smaller datasets. By leveraging Crystal Graph Convolutional Neural Networks (CGCNN), the method effectively captures structural relationships at the atomic level, achieving a G<sub>s</sub> prediction accuracy of 90%, ultimately identifying 12 promising SEI candidates. This sophisticated methodology not only accelerates material discovery but also opens new pathways for deploying artificial intelligence in advanced energy materials, driving progress toward safer and more efficient SSBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"42 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967956","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}
Rongfeng Yang, Fan Wang, Wan-er Cui, Wei Chen, Tianyu Lei, Dongjiang Chen, Dongxu Chen, Li Xia, Chi Zhang, Kaijun Cheng, Runyi Dai, Yichao Yan, Xiaobin Niu, Yin Hu
{"title":"Regenerative redox mediator for the suppression of dead lithium for lithium sulfur pouch cell","authors":"Rongfeng Yang, Fan Wang, Wan-er Cui, Wei Chen, Tianyu Lei, Dongjiang Chen, Dongxu Chen, Li Xia, Chi Zhang, Kaijun Cheng, Runyi Dai, Yichao Yan, Xiaobin Niu, Yin Hu","doi":"10.1016/j.ensm.2025.104030","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104030","url":null,"abstract":"Lithium sulfur batteries are persistently investigated by the research community due to their high energy density property. However, in order to get such performance, based on the current pouch cell strategy, less electrolyte and more stacking electrodes need be applied, leading to the aggravated dendrite growth, dead lithium accumulation and electrolyte depletion. In this context, we report a regenerative redox mediator strategy, targeting the operation window of the lithium sulfur batteries. The redox mediator can spontaneously consume the dead lithium on the anode, then be re-oxidized on the cathode through electrochemical process. Based on this design, the lithium sulfur pouch cell can be fully charged at 1C for more than 140 cycles. Moreover, the regeneration mechanism is studied by in situ UV-vis spectroscopy. This work not only validates the effectiveness of redox mediator for improving the high rate charging and cycling of lithium sulfur pouch cells, but also excludes the invalid mediator type and provides the design concept, guiding the future development of high rate charging strategy for lithium sulfur batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"36 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967951","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}
Kangjia Hu, Jiaxin Chen, Jiahui Zhang, Xiaoyu Sang, Tao Meng, Zhangci Wang, Xianluo Hu
{"title":"Binder-enabled cross-scale stabilization of high-areal-capacity micro-sized silicon anodes for high-voltage lithium-ion batteries","authors":"Kangjia Hu, Jiaxin Chen, Jiahui Zhang, Xiaoyu Sang, Tao Meng, Zhangci Wang, Xianluo Hu","doi":"10.1016/j.ensm.2025.104029","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104029","url":null,"abstract":"Sustainable micro-sized silicon (μSi) has emerged as a promising high-capacity alternative to traditional carbon-based anodes in lithium-ion batteries. However, addressing severe cracking in both electrodes and particles attributed to large volumetric change during cycling remains a challenge. Here we developed a cost-effective water-based cross-scale stabilization (CSS) binder to preserve the electrode integrity and stabilize the solid electrolyte interphase of μSi anodes. Forming a soft-rigid, electrically conductive, high-elasticity network and directing the growth of highly robust LiF-rich interphases, the CSS binder enables stable cycling of μSi anodes at impressive areal capacities of up to 5.9 mAh cm<sup>–2</sup> and a high volumetric capacity of 2458 mAh cm<sup>–3</sup>, which represents a pioneering report on high-capacity μSi anodes. Furthermore, at commercial-level areal capacities, 4.2-V μSi||LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> pouch cells (N/P = 1.15) achieve 81% capacity retention in 100 cycles. This work introduces innovative strategies for enhancing reversible lithium storage in high-capacity alloy-type anodes and advancing the development of high-energy-density batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"12 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967957","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}
Xiyan Wei, Yongbiao Mu, Jian Chen, Yuke Zhou, Youqi Chu, Lin Yang, Chaozhu Huang, Tao Xue, Limin Zang, Chao Yang, Lin Zeng
{"title":"Optimizing Zn (100) Deposition via Crystal Plane Shielding Effect towards Ultra-High Rate and Stable Zinc Anode","authors":"Xiyan Wei, Yongbiao Mu, Jian Chen, Yuke Zhou, Youqi Chu, Lin Yang, Chaozhu Huang, Tao Xue, Limin Zang, Chao Yang, Lin Zeng","doi":"10.1016/j.ensm.2025.104026","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104026","url":null,"abstract":"Aqueous zinc ion batteries (AZIBs) have gained significant attention as promising solutions for large-scale grid energy storage, however, challenges such as dendrite formation and limited operating current ranges significantly hinder their stability and practical application. This study investigates the incorporation of methylsulfonylamine (MSA) as an electrolyte additive in AZIBs. MSA can restructure the solvation structure of Zn<sup>2+</sup> ions and guide the organized deposition of zinc (Zn) along the (100) crystal plane. A crystal plane shielding effect has been proposed, which accelerates the plating-stripping processes, enhances overall stability and suppresses Zn dendrite formation. Consequently, incorporating MSA expands the current density range and enhances the practical usability of AZIBs under extreme conditions. As a result, Zn||Zn symmetric cells demonstrate an exceptional cycling life of 300 h at 80 mA/cm² and 1 mAh/cm², with an impressive 24,000 cycles. The MnO<sub>2</sub>||Zn full cells utilizing the MSA-containing electrolyte demonstrate exceptional capacity retention of 85.4% after 3,000 cycles at 0.5 A/g. These results underscore the significant effect of MSA as an electrolyte additive and provide a broad road for enhancing performance of AZIBs under the high current density conditions.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"6 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142962704","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}
Yu-Juan Xu, Ying-Ying Wang, Zhen-Yi Gu, Chen-Shuo Zhao, Xing-Long Wu, S. Ravi P. Silva, Bao-Hua Hou
{"title":"Cellulose-grafting boosted pyrolysis nucleation: Achieving low-temperature construction of hard carbon anodes with long low-voltage plateau and ultrafast Na storage kinetics","authors":"Yu-Juan Xu, Ying-Ying Wang, Zhen-Yi Gu, Chen-Shuo Zhao, Xing-Long Wu, S. Ravi P. Silva, Bao-Hua Hou","doi":"10.1016/j.ensm.2025.104031","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104031","url":null,"abstract":"Biomass-derived hard carbon (BHC) with low-voltage plateau (LP) is a promising anode material for sodium ion batteries. However, ultrahigh carbonization temperatures to obtain LP and slow electrochemical reaction kinetics in LP make it difficult to achieve low cost and high rate performance. Herein, a cellulose grafting reaction is proposed to modulate the pyrolysis nucleation process of biomass, which makes it possible to obtain a BHC with graphitic nanodomain structure at 800 °C, similar to the hard carbon prepared at the traditional 1300 °C. Moreover, the nitrogen doping introduced by the grafting reaction is highly preserved at low carbonization temperatures, which induces a dramatic shift in the electrochemical reaction kinetics and converts the typical slow diffusion control process in LP to an ultrafast pseudocapacitive control process. As a result, the prepared N-doped BHC simultaneously realizes long pseudocapacitive-control LP, high reversible capacity, excellent rate capability, and ultralong cycle life in sodium ion half/full cell. More significantly, the structure formation mechanism, Na-storage mechanism, and the root causes of electrochemical reaction kinetic shifts in the LP of such a N-doped BHC are studied in detail, which provides a constructive view for the low-temperature construction of BHCs with long LP and high rate performance.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"40 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967958","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}
Jung-In Lee, Sungjin Cho, Su Hwan Kim, Se Hun Joo, Hyeong Yong Lim, Yuri Choi, Jungki Ryu, Sang Kyu Kwak, Soojin Park
{"title":"Modulating Na-ion Solvation in Carbonate-based Electrolytes by Nitrogen-doped Carbon Dots Enables Superior Na Metal Batteries","authors":"Jung-In Lee, Sungjin Cho, Su Hwan Kim, Se Hun Joo, Hyeong Yong Lim, Yuri Choi, Jungki Ryu, Sang Kyu Kwak, Soojin Park","doi":"10.1016/j.ensm.2025.104023","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104023","url":null,"abstract":"Sodium (Na) anode for Na-metal batteries (SMBs) has gained significant attention for its high theoretical capacity and the lowest redox potential. However, challenges caused by random growth of Na dendrites and unstable solid-electrolyte-interphase (SEI) layers impede the practical applications for SMBs in carbonate-based electrolytes. In this study, we propose a novel additive, nitrogen-doped carbon quantum dots (NCQDs) in the carbonate-based electrolyte. NCQDs modify the solvation structures among Na-ion, <span><math><msubsup is=\"true\"><mtext is=\"true\">PF</mtext><mrow is=\"true\"><mn is=\"true\">6</mn></mrow><mo is=\"true\">−</mo></msubsup></math></span> anion and solvent molecules. The negatively charged NCQDs exhibit a strong affinity toward Na-ions, impeding interactions between <span><math><msubsup is=\"true\"><mtext is=\"true\">PF</mtext><mrow is=\"true\"><mn is=\"true\">6</mn></mrow><mo is=\"true\">−</mo></msubsup></math></span> anions and solvent molecules. This coordination between NCQDs and Na-ions slightly alters the solvation environment of the electrolyte, leading to a weak solvation structure. This electrolyte induces densely inorganic-rich SEI layers and thus improves the electrochemical performance. Our approach ensures a stable cycling of the Na metal anode for cycling up to 700 hrs at 0.5 mA cm<sup>-2</sup> in Na||Na batteries, along with an average Coulombic efficiency (91 %) at 1 mA cm<sup>-2</sup> in Na||Cu batteries. Moreover, practical SMBs with P2-Na<sub>0.67</sub>Ni<sub>0.33</sub>Mn<sub>0.67</sub>O<sub>2</sub> demonstrate stable cycling stability (93 % for 110 cycles), even operating up to 4.3V. This study enables high-voltage SMBs and provides guiding principles in electrolyte design for Na-based batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"16 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961959","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}
Lea C. Meyer, Abilash Kanish Thiagarajan, Alexey Koposov, Andrea Balducci
{"title":"Unravelling the Mechanism of Potassium-Ion Storage into Graphite through Electrolyte Engineering","authors":"Lea C. Meyer, Abilash Kanish Thiagarajan, Alexey Koposov, Andrea Balducci","doi":"10.1016/j.ensm.2025.104021","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104021","url":null,"abstract":"Graphite is one of the most widely used anode materials in potassium-ion batteries (PIBs). However, the exact mechanism of K<sup>+</sup> ions intercalation into graphite has not yet been fully understood. In addition, the intercalation process strongly depends on the selection of the electrolyte system. In this work, we evaluated the use of an electrolyte containing 1.5 M potassium bis(fluorosulfonyl)imide (KFSI) dissolved in a mixture of propylene carbonate (PC)/ 1,1,2,2-tetraethoxyethane (TEG)/ vinyl ethylene carbonate (VEC) (62:36:2 vol.%). Using such an electrolyte system it was possible to obtain experimental evidence for the formation of KC<sub>16</sub> during the potassium intercalation and deintercalation using in situ Raman spectroscopy and operando X-ray diffraction (XRD). The results are supported by the visual observation of a color change of the graphite electrode surface during the intercalation of K<sup>+</sup> ions into the graphite lattice. In addition, it has been demonstrated that the selected electrolyte system eliminates the co-intercalation of the solvent into the graphite structure.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"204 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961960","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}
Le Zhang, Min Lin, Zihong Yu, Youxia Huang, Qiangchao Sun, Xionggang Lu, Hongwei Cheng
{"title":"Tyrosine additives with rich-polar functional groups provide multi-protections for ultra-stable zinc metal anodes","authors":"Le Zhang, Min Lin, Zihong Yu, Youxia Huang, Qiangchao Sun, Xionggang Lu, Hongwei Cheng","doi":"10.1016/j.ensm.2025.104022","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104022","url":null,"abstract":"The widespread commercialization of aqueous zinc-ion batteries (AZIBs) is severely limited by dendrite growth and rampant parasitic reactions. While various additives have been introduced to improve the stability of zinc anodes, a single polar functional group additive cannot provide comprehensive protection for zinc anodes. Here, a low-cost, high-functionality Tyrosine (Tyr) organic small molecule is utilized as an electrolyte additive to achieve ultra-stable zinc metal anodes. The findings indicated that the electronegative carboxyl group tended to participate in the solvation sheath of Zn<sup>2+</sup>. The zinc-philic amino group and hydrophobic benzene ring synergistically construct a hydrophobic electric double layer on the surface of the zinc anode. The hydrophilic nature of the hydroxyl group enables it to capture free water molecules and reconstruct the hydrogen bonding network of the electrolyte. More importantly, the strong adsorption of Tyr molecule is beneficial to induce the formation of an <em>in-situ</em> organic-inorganic hybrid solid electrolyte interface layer, thereby further enhancing protection for the zinc anode. Profiting from the synergistic effect of the polyfunctional group in the Tyr additive, the Zn||Zn cell exhibits ultra-long cycle stability over 3800 h (∼ 20 times <em>vs</em>. ZnSO<sub>4</sub>) at 1.0 mA cm<sup>‒2</sup>, 1 mAh cm<sup>‒2</sup> and an ultra-high cumulative plated capacity of 8.75 Ah cm<sup>‒2</sup> at 5.0 mA cm<sup>−2</sup>. Furthermore, the Zn||Cu cell delivers a significantly improved reversibility with an average Coulomb efficiency of 99.88% after 3000 cycles. This finely regulated electrolyte, leveraging the synergistic effects of multiple functional groups, heralds a promising trajectory for the advancement of enduring Zn metal batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"2 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142939517","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}
Shumin Wu, Yulong Zhang, Hongcheng Liang, Hongji Pan, Lu Chen, Yanxin Jiang, Hao Ding, Peng Wang, Dongni Zhao, Qing Zhang, Lin Zeng, Shiyou Li, Yiju Li
{"title":"In-Situ Electrochemical Customization of Solid Electrolyte Interphase for Fast-Charging and Long-Cycle-Life Graphite Anodes","authors":"Shumin Wu, Yulong Zhang, Hongcheng Liang, Hongji Pan, Lu Chen, Yanxin Jiang, Hao Ding, Peng Wang, Dongni Zhao, Qing Zhang, Lin Zeng, Shiyou Li, Yiju Li","doi":"10.1016/j.ensm.2025.104024","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104024","url":null,"abstract":"The burgeoning demand for electric vehicles and electronics underscores the imperative for fast-charging graphite (Gr)-based lithium-ion batteries (LIBs) to alleviate “range anxiety”. Overcoming the fast-charging challenge necessitates tackling diffusion issues, notably the sluggish lithium-ion (Li<sup>+</sup>) transport through solid electrolyte interphase (SEI). In response, our work proposes a charge/discharge protocol that in-situ accurately customizes an inner-LiF-rich bilayer SEI in a commercial carbonate electrolyte without introducing additional functional additives to reduce the energy barrier for Li<sup>+</sup> migration and thus enable fast-charging capabilities for Gr anode. Moreover, our study reveals strong structure-dependent properties of the SEI on the Gr, including interface affinity, Li<sup>+</sup> transport, and electrical insulation, which helps to design high-ion-conductivity and stable SEI. As a result, the in-situ electrochemical customization of the inner-LiF-rich bilayer SEI significantly increases the cycling stability and rate performance of Gr anode, maintaining a high capacity retention of 70.6% after 1000 cycles at a high rate of 5 C. Moreover, the LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> (NCM622)||Gr pouch cell utilizing the new formation protocol demonstrates a 9.5% increase in capacity retention compared to the traditional charge/discharge formation protocol. Our work provides an effective and scalable strategy for advancing fast-charging capabilities and extending the longevity of Gr-based LIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"67 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142939516","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}