Fanbo Meng, Yuwu Li, Weihao Lin, Jiahe Chen, Yuzhuo Zeng, Yuhao Xia, Bin Yuan, Hao Chen, Renzong Hu
{"title":"Recycling Spent Lithium-Ion Layered Cathodes: Toward Direct Single-Crystalline Regeneration Technology","authors":"Fanbo Meng, Yuwu Li, Weihao Lin, Jiahe Chen, Yuzhuo Zeng, Yuhao Xia, Bin Yuan, Hao Chen, Renzong Hu","doi":"10.1002/aenm.202504206","DOIUrl":"https://doi.org/10.1002/aenm.202504206","url":null,"abstract":"Direct single-crystalline regeneration (DSCR) techniques of layered cathodes in lithium-ion batteries have attracted considerable research attention. Nonetheless, current development and commercial application of DSCR techniques remain constrained by different failure conditions of cathode materials, the complexity of production processes, and the opacity of evaluation systems. Herein, recent works on DSCR techniques applied to spent layered cathodes are summarized and compared. First, the failure mechanism of LiCoO<sub>2</sub> (LCO) and Ni-based cathodes (NCM and NCA) is discussed, followed by a critical assessment of the current advantages and challenges of single-crystalline cathodes. Considering the different Li supplement and Ni contents, the electrochemical performance for the reported regenerated of LCO, Ni-lean, Ni-medium, and Ni-rich cathodes is separately studied and compared. Based on comprehensive evaluation and comparison, a multi-dimensional feasibility and strategy analysis for the development direction of targeted single-crystalline products and manufacturing techniques is provided. Finally, a prospect for future developments and challenges for the DSCR processes is further provided, with the hope of inspiring further advances toward the green and sustainable regeneration of spent lithium-ion batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"88 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153842","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}
Dongkyu Lee, Dongguk Kang, Chanho Yuk, Hyeri Kang, Eunji Lee, Wonho Lee, Jinseok Park, Bumjoon J. Kim
{"title":"Effects of Mechanical Properties of Elastomeric Electrolytes for Stable Operation of Lithium Metal Batteries","authors":"Dongkyu Lee, Dongguk Kang, Chanho Yuk, Hyeri Kang, Eunji Lee, Wonho Lee, Jinseok Park, Bumjoon J. Kim","doi":"10.1002/aenm.202503836","DOIUrl":"https://doi.org/10.1002/aenm.202503836","url":null,"abstract":"The mechanical properties of polymer electrolytes are critical for the stable operation of lithium metal batteries (LMBs), as they accommodate volume changes of the lithium (Li) metal anode, suppress dendrite formation, and maintain interfacial stability. Here, we present a systematic investigation into the role of the mechanical characteristics of fluorinated elastomeric electrolytes (FEEs) in enabling stable cycling of LMBs at ambient and low temperatures. The FEEs consist of bicontinuous elastomer and plastic crystal phases, allowing independent control of mechanical properties by adjusting the crosslinking density of the elastomer phase. Concurrently, FEEs retain the fast ion transport properties of the plastic crystal phase, exhibiting high ionic conductivity of ≈1.1 and ≈0.24 mS cm<sup>−1</sup> at 25 and −10 °C, respectively. The optimized FEE demonstrates balanced toughness (140.6 kJ m<sup>−3</sup>) and adhesion energy (31.4 J m<sup>−2</sup>), along with elastic recovery characteristic, enabling a Li|| LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> full cell to deliver a high initial discharge capacity (153 mAh g<sup>−1</sup>) with 76% capacity retention after 150 cycles at −10 °C. In contrast, lightly crosslinked FEEs undergo irreversible plastic deformation and loss of interfacial contact, while excessively crosslinked systems suffer from low toughness and are prone to fracture, both resulting in poor cycling performance.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"65 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153843","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}
Chen Cheng, Yihao Shen, Chi Chen, Simin Tang, Zengqing Zhuo, Qianjie Niu, Cheng Yuan, Tong Chen, Lei Wang, Jinghua Guo, Dan Sun, Liang Zhang
{"title":"Asymmetric-Orbital-Hybridization Induced Electron Redistribution Enabling Stable Sodium Layered Oxides","authors":"Chen Cheng, Yihao Shen, Chi Chen, Simin Tang, Zengqing Zhuo, Qianjie Niu, Cheng Yuan, Tong Chen, Lei Wang, Jinghua Guo, Dan Sun, Liang Zhang","doi":"10.1002/aenm.202504261","DOIUrl":"https://doi.org/10.1002/aenm.202504261","url":null,"abstract":"Layered transition metal (TM) oxides have garnered great attention as viable cathodes for sodium-ion batteries (SIBs), but the challenges of complicated multiphase transitions, severe structural deterioration and unstable oxygen redox reaction still hamper their practical application. Herein, a universal electron redistribution strategy based on the orbital hybridization regulation is proposed and NaNi<sub>0.5</sub>Mn<sub>0.35</sub>Ti<sub>0.15</sub>O<sub>2</sub> (NNMTO) is introduced as a model cathode considering the distinct electronegativity between Ni and Ti. The nonequivalent electron distribution induced by the covalency competition within asymmetric Ni<sub>3d</sub>-O<sub>2p</sub>-Ti<sub>3d</sub> backbone (Ni─O─Ti charge transfer via the bridging oxygen atom) delocalizes the electrons between Ni and O and modulates the local chemical environment around O. The enhanced orbital coupling combined with increased Ni─O covalency can not only suppress the over-oxidation of lattice oxygen and improve the reversibility of oxygen redox, but also alleviate the cooperative Jahn–Teller distortion of Ni<sup>3+</sup>O<sub>6</sub> octahedron and prevent the phase transition from O3′ to the detrimental O3″ phase by constructing a more rigid TM─O framework. As a result, NNMTO shows a sustained reversible capacity and remarkable cycling stability that is rooted in reversible oxygen and TM redox processes. This study provides an alternative avenue to construct high-performance SIBs from the perspective of local chemistry and orbital hybridization modulation.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"26 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153596","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}
Zhenwei Li, Rui Zhang, Peilun Yu, Hengyuan Hu, Zhiyu Zou, Jie Chen, Mengchuang Liu, Ping Liu, Chang Lu, Zhaoxin Meng, Yongqiang Ji, Jie Yu, Meisheng Han, Wenhua Zhang, Yuliang Cao
{"title":"Tip Effect-Driven Charge Transport Enhancement in Silicon-Carbon Anodes for All-Solid-State Lithium-Ion Batteries","authors":"Zhenwei Li, Rui Zhang, Peilun Yu, Hengyuan Hu, Zhiyu Zou, Jie Chen, Mengchuang Liu, Ping Liu, Chang Lu, Zhaoxin Meng, Yongqiang Ji, Jie Yu, Meisheng Han, Wenhua Zhang, Yuliang Cao","doi":"10.1002/aenm.202504241","DOIUrl":"https://doi.org/10.1002/aenm.202504241","url":null,"abstract":"Despite its pronounced impact on mass transport and local energy field modulation, the tip effect remains an underexplored strategy in the design of solid-state batteries. Here, a radial vertical graphene (RVG)-encapsulated silicon anode (RVG@Si-V) that strategically leverages the tip effect to modulate interfacial charge transport and direct the formation of solid electrolyte interphases (SEI) in all-solid-state lithium-ion batteries (ASSLIBs) is reported. The sharp geometry of RVG induces localized electric field enhancement at the electrode-electrolyte interfaces, which promotes charge accumulation and facilitates field-driven electrolyte decomposition toward thin and LiF-rich SEI formation. The structure-field coupling effectively overcomes the long-standing challenge of sluggish charge transfer kinetics at electrode-electrolyte interfaces and contributes to improved rate capability and long-term cycling stability. Electrochemical characterizations reveal that RVG@Si-V delivers excellent rate performance (940.9 mAh g<sup>−1</sup>, 5 A g<sup>−1</sup>) and capacity retention compared to its planar graphene (PG) counterpart (PG@Si-V) without the tip effect, retaining 76.6% of its capacity after 500 cycles at 3 A g<sup>−1</sup>. This work demonstrates a previously underexplored but highly effective strategy of employing the tip effect to modulate interfacial charge transport and SEI formation in solid-state battery systems, offering critical insights toward the development of high-performance Si anodes for advanced ASSLIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"63 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140983","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}
Mingyun Kim, Jongeun Kim, Hyeju Yun, Youngbae Jeon, Yun Jeong Hwang, Kijung Yong
{"title":"Advancing Lithium-Mediated Nitrogen Reduction using Insights from Lithium-Ion Battery: Focusing on Uniform Li Plating","authors":"Mingyun Kim, Jongeun Kim, Hyeju Yun, Youngbae Jeon, Yun Jeong Hwang, Kijung Yong","doi":"10.1002/aenm.202503638","DOIUrl":"https://doi.org/10.1002/aenm.202503638","url":null,"abstract":"Lithium-mediated nitrogen reduction reaction (Li-NRR) offers a promising alternative to the energy-intensive Haber–Bosch process for ammonia (NH<sub>3</sub>) synthesis, enabling renewable-powered NH<sub>3</sub> production. However, this technology faces multiple challenges in terms of Faradaic efficiency (FE), energy efficiency (EE), stability and scalability. These problems arise from a variety of causes, but they have one thing in common: they can be improved by uniform deposition of lithium (Li). Therefore, promoting uniform Li plating could serve as a key breakthrough in addressing these issues. This review highlights various studies focusing on the issues associated with Li-NRR and proposes ideas based on previously reported research on Li metal battery (LMB) systems, which exhibit similarities with the Li-NRR systems with respect to Li plating and the formation of a solid-electrolyte interphase (SEI). Effective cross-pollination of various methods, including electrode modifications, solvation control of Li<sup>+</sup>, and application of additives, are introduced. Elaboration of correspondences between Li-NRR and LMB systems suggests an efficient research strategy for advancing the Li-NRR field. This review underscores the synergistic potential of hybrid strategies for addressing the critical challenges related to Li-NRR and provides future research directions and possibilities in this field, which would eventually accelerate progress toward sustainable green NH<sub>3</sub> production.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"91 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153841","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}
Yuting Chen, Qi Fan, Hejing Wang, Fan Kong, Boya Wang, Mei Yang, Chenying Li, Zhengyang Li, Zhiyuan Li, Zhiyuan Guo, Qin Sun, Xiaohui Zhu, Menggai Jiao, Teng Zhai, Shubiao Xia, Lin Gu, Zhen Zhou, Hui Xia
{"title":"Heterostructured Manganese-Based Cathode with Atomic Interlocking for Advanced Sodium-Ion Batteries","authors":"Yuting Chen, Qi Fan, Hejing Wang, Fan Kong, Boya Wang, Mei Yang, Chenying Li, Zhengyang Li, Zhiyuan Li, Zhiyuan Guo, Qin Sun, Xiaohui Zhu, Menggai Jiao, Teng Zhai, Shubiao Xia, Lin Gu, Zhen Zhou, Hui Xia","doi":"10.1002/aenm.202504637","DOIUrl":"https://doi.org/10.1002/aenm.202504637","url":null,"abstract":"Although manganese-rich layered oxides are promising as low-cost, high-capacity cathodes for sodium-ion batteries, their single-phase design suffers from structural degradation due to unfavorable phase transitions and lattice strain accumulation caused by inherent defects. To address this issue, we propose a functionally oriented multi-element doping strategy to construct a P2/Zig-Zag biphasic cathode (NMFCAT) with an atomically interlocked heterojunction. Unlike conventional biphasic systems, this in-plane connection design enables continuous Na⁺ diffusion through atomically shared phase boundaries while leveraging strain-complementary evolution to restrict volume fluctuation to 1.44% (vs 3.12% in pure P2). Crucially, the Zig-Zag motifs serve as mechanical anchors at phase boundaries, exploiting the interlocking effect to suppress interfacial separation and maintain heterojunction integrity during cycling. Concurrently, the integrated P2 phase lowers the Na<sup>+</sup> migration barrier to 0.19 eV, synergistically enhancing electrode kinetics and air stability (only 0.05% residual alkali increase after 7-day exposure). The rationally designed NMFCAT cathode exhibits superior electrochemical performance, fast electrode kinetics, and negligible volume variation, establishing a new paradigm for multiphase structural engineering in layered Mn-based cathodes for high-performance sodium-ion batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"4 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153597","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}
Zhuangzhi Li, Yong Wang, Haiyan Hu, Lang Qiu, Yao Xiao, Linsen Li, Zhenguo Wu, Xiaodong Guo
{"title":"Synchronous Carbonization and Phase-Formation via Flash Joule Heating for Uniform Carbon-Coated Polyanionic Cathode Materials","authors":"Zhuangzhi Li, Yong Wang, Haiyan Hu, Lang Qiu, Yao Xiao, Linsen Li, Zhenguo Wu, Xiaodong Guo","doi":"10.1002/aenm.202503894","DOIUrl":"https://doi.org/10.1002/aenm.202503894","url":null,"abstract":"Carbon coating is an effective strategy for enhancing the conductivity of polyanionic cathode materials. However, conventional carbon coating processes suffer from loose carbon coatings and excessive unbound carbon, leading to exacerbated side reactions. Here, the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> (NVP) carbon coating process in real-time is probed, revealing that the kinetic mismatch between carbon source carbonization and cathode material phase-formation causes coating failure. By introducing flash Joule heating (FJH) technology, ultrafast thermal shock is leveraged to kinetically synchronize carbonization and phase-formation, fundamentally eliminating sequential reaction stages, thereby constructing a 2-nm-thick uniform carbon coating on NVP. The FJH-engineered NVP delivers 85 mAh g<sup>−1</sup> at −40 °C, and retains 84% capacity after 3000 cycles at 30 C. The coating stabilizes interfaces, reduces resistance, enhances thermal stability, and mitigates runaway risks. The effective preparation of various polyanionic cathode materials confirmed the versatility of FJH method to improve the effect of carbon coating. These findings provide an effective strategy for designing high-safety, long-lifespan polyanionic cathode materials.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"63 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145141030","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}
Yingdong Chen, Sijia Gao, Yujing Su, Tao Chen, Jiajun Fu
{"title":"Multiscale Design Strategies of Interface-Stabilized Solid Electrolytes and Dynamic Interphase Decoding from Atomic-to-Macroscopic Perspectives","authors":"Yingdong Chen, Sijia Gao, Yujing Su, Tao Chen, Jiajun Fu","doi":"10.1002/aenm.202502938","DOIUrl":"https://doi.org/10.1002/aenm.202502938","url":null,"abstract":"Solid-state lithium metal batteries (SSLMBs) are poised to revolutionize energy storage technologies, delivering unparalleled energy density and intrinsic safety through the elimination of flammable liquid electrolytes. Nevertheless, the transition from laboratory breakthroughs to commercial viability is critically impeded by persistent interfacial dilemmas, including lithium dendrite propagation, parasitic chemical/electrochemical degradation at electrode/electrolyte interfaces, and insufficient interfacial contact intimacy. This review systematically and comprehensively reviews the design strategies of interface-stabilized solid electrolytes, covering inorganic solid electrolytes, solid polymer electrolytes, and inorganic-polymer composites. The review further decodes the dynamic interplay between the microstructure of solid electrolytes, interfacial ion transport kinetics, and interphase evolution through emerging in situ/operando characterization techniques. By elucidating structure-property-interphase relationships across atomic-to-macroscopic scales, this review unveils mechanistic insights into the dynamic interfacial evolution and interfacial failure modes over multi-length scales. Finally, a forward-looking perspective on interface-stabilized solid electrolytes is proposed, thereby paving the way for the practical realization of SSLMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145141047","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}
Shanshan Zhang, Bifa Ji, Ke Ding, Yang Yang, Yongping Zheng, Yongbing Tang
{"title":"Confined Atom Escape and Nucleation Delivering Iridium-Based Nanoparticles with Ultrahigh Mass Activity for Acidic Water Oxidation","authors":"Shanshan Zhang, Bifa Ji, Ke Ding, Yang Yang, Yongping Zheng, Yongbing Tang","doi":"10.1002/aenm.202503229","DOIUrl":"https://doi.org/10.1002/aenm.202503229","url":null,"abstract":"Achieving high catalytic activity and stability with as little iridium (Ir) as possible is essential for the widespread deployment of proton exchange membrane water electrolysis (PEMWE). Although single-atom dispersion strategies could maximize the utilization of iridium, they usually suffer from unsatisfactory stability issues. Here, a method is reported of growing highly dispersed iridium-based nanoparticles with unprecedented mass activity and stability through confined atom escape and nucleation (CAEN). Unlike conventional synthesis methods in which all metal precursors are free to nucleate, CAEN is characterized by a tunable confinement of metal single atoms in the carbon substrate by asymmetric nitrogen, oxygen-coordination, which establishes a thermodynamic and kinetic equilibrium between single-atom dispersion and nucleation, prevents the growth of metastable phases, and delivers highly stable nanoparticles with durable active surfaces. The acidic oxygen evolution reaction (OER) mass activity of the designed catalyst reaches 2040.8 A g<sub>Ir</sub><sup>−1</sup>, which is about 25 times that of commercial Ir/C (81.60 A g<sub>Ir</sub><sup>−1</sup>), and the durability is improved by an order of magnitude. This CAEN method can be further extended to the synthesis of iridium-based intermetallic nanoparticles, resulting in a more than 50-fold increase in OER mass activity, opening up a completely new path for the design of high-performance catalysts.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"42 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140984","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":"Influence of Anode Reactivity and Chemical Crossover on the Formation of Cathode-Electrolyte Interphase in High-Nickel Layered Oxide Cathodes","authors":"Karla Aranda, Arumugam Manthiram","doi":"10.1002/aenm.202502617","DOIUrl":"https://doi.org/10.1002/aenm.202502617","url":null,"abstract":"As the push for lithium-ion batteries (LIBs) with high-energy density grows, systems pairing high-nickel cathodes with high-capacity anodes have become attractive; however, these electrodes individually suffer from high surface reactivities, leading to interfacial instabilities. When paired together, further issues arise, with cathode-to-anode crossover being a well-known phenomenon. In contrast, anode-to-cathode crossover remains underexplored, especially in systems that undergo large volume changes. Here, a comparison of the influence of anode reactivity on cathode surface degradation is presented by pairing LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) cathode with graphite, prelithiated silicon suboxide (SiO<sub>x</sub>), and lithium-metal anodes. Voltage curves and differential capacity analysis show that all cells experience polarization growth throughout cycling. A combination of electrochemical techniques, such as operando galvanostatic electrochemical impedance spectroscopy (GEIS), and surface analyses, such as scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS), reveal that cycling against more reactive anodes promotes the formation of a thicker, organic-rich cathode electrolyte interphase (CEI), which suffers from impedance growth and large irreversible capacity loss. Post-mortem characterization with XPS and SEM confirms compositional and morphological changes at the cathode surface and the cycled separator. The findings provide insights into the role of anode-driven degradation of high-Ni cathodes, promoting further understanding of two-way crossover in LIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"2 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145141105","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}