Dajin Oh, Minji Kim, Wontae Lee, Jeongwoo Lee, Minsun Kong, Jiyeon Kim, Dae Beom Lee, Won-Sub Yoon
{"title":"Bifunctional Role of Surface Cobalt Doping as a Lithium-Residue Scavenger and Surface Stabilizer in Single-Crystalline Ultrahigh-Ni Cathodes","authors":"Dajin Oh, Minji Kim, Wontae Lee, Jeongwoo Lee, Minsun Kong, Jiyeon Kim, Dae Beom Lee, Won-Sub Yoon","doi":"10.1002/eem2.70343","DOIUrl":"https://doi.org/10.1002/eem2.70343","url":null,"abstract":"<p>Ultrahigh-Ni layered cathodes are among the most promising materials for next-generation lithium-ion batteries due to their high energy density, but their practical use is often limited by severe surface instability and structural degradation. In this work, surface Co doping of LiNi<sub>0.93</sub>Co<sub>0.05</sub>Al<sub>0.02</sub>O<sub>2</sub> (NCA) is demonstrated to enhance both electrochemical performance and structural stability. The introduction of Co at the surface promotes the formation of stable spinel phases, such as Co<sub>3</sub>O<sub>4</sub> and Li<sub><i>x</i></sub>CoO<sub>2</sub>, which simultaneously remove residual lithium species and suppress the evolution of detrimental NiO-like rock-salt phases and resistive interfacial layers. Comprehensive analyses, including electrochemical testing, synchrotron-based X-ray techniques, and high-resolution electron microscopy, confirm that Co-doped NCA exhibits improved interfacial stability and lithium-ion transport compared to undoped NCA. These findings highlight surface Co doping as a surface reconstruction stabilizer to mitigate degradation pathways, thereby enabling ultrahigh-Ni cathodes to achieve greater durability and performance in advanced lithium-ion battery applications.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70343","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149029113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pengyu Tan, Jianwei Lu, Yimin Chen, Kaiwen Yang, Kun Luo, Dan Liu, Weiwei Lei
{"title":"Electronic Synergy in NiCo-Embedded Nitrogen-Doped Hollow Mesoporous Carbon Spheres for Bifunctional Oxygen Catalysis and Zinc–Air Batteries","authors":"Pengyu Tan, Jianwei Lu, Yimin Chen, Kaiwen Yang, Kun Luo, Dan Liu, Weiwei Lei","doi":"10.1002/eem2.70318","DOIUrl":"https://doi.org/10.1002/eem2.70318","url":null,"abstract":"<p>Rechargeable zinc–air batteries (ZABs) are promising candidates for sustainable energy storage; however, their performance is severely limited by sluggish oxygen reduction and evolution (ORR/OER) kinetics. Here, a hard-templating etching strategy was employed to construct nitrogen-doped hollow mesoporous carbon spheres embedded with NiCo nanoparticles (NiCo@N-HMCS). The hollow nanostructure, together with a strong electronic coupling between NiCo alloys and N-doped carbon, provides abundant accessible active sites, optimized charge transfer, and robust structural stability. As a result, NiCo@N-HMCS delivers remarkable bifunctional electrocatalytic activity in alkaline media, with a half-wave potential of 0.84 V for the oxygen reduction reaction and an overpotential of 330 mV at 10 mA cm<sup>−2</sup> for the oxygen evolution reaction. When applied in ZABs, the catalyst delivers a high open-circuit voltage of 1.56 V, a peak power density of 185.53 mW cm<sup>−2</sup>, and durable cycling over 300 h. The flexible ZAB configuration also delivers a power density of 79.06 mW cm<sup>−2</sup> and stable operation of 120 h. This study demonstrates a robust platinum-group-metal-free strategy for advancing next-generation rechargeable and flexible energy storage systems.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70318","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149029077","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Cellulose Fiber-Engineered Gradient Interfacial Channels as Ion-Highways for High-Loading, Long-Life Lithium-Ion Batteries","authors":"Wenhao Jia, Haiwei Wu, Ruihua Li, Yuting Wang, Zhixiong Zhang, Hanbin Liu, Zhijian Li, Chuanyin Xiong, Yonghao Ni, Qiang Zhang, Li Wang, Xiangming He","doi":"10.1002/eem2.70325","DOIUrl":"https://doi.org/10.1002/eem2.70325","url":null,"abstract":"<p>Developing thick electrodes with high active material content is crucial to achieving high-energy-density lithium-ion batteries; yet it remains challenging due to the conflicting requirements of mechanical integrity and rapid ion transport. Here, we propose a scalable papermaking strategy to address this dilemma by constructing a minimal mass fraction (~3 wt%) of cellulose fibers into a three-dimensional scaffold. This scaffold not only ensures the mechanical robustness of electrodes with ultra-high active material content (96 wt%) but, more importantly, creates well-defined gradient interfacial channels. These channels function as efficient “ion highways,” which significantly enhance electrolyte wettability and minimize ion-diffusion resistance. When paired in a full cell (lithium manganese iron phosphate//lithium titanate), this design enables exceptional cycling stability and rate capability, maintaining 95.3% capacity after 500 cycles at 0.5 C and 72.3% over 1000 cycles at 2 C, substantially outperforming conventional counterparts. Post-cycling analysis reveals that performance degradation primarily stems from the active materials, while the cellulose framework exhibits excellent electrochemical inertness and interfacial stability. This work provides a practical and sustainable paradigm for engineering efficient ion transport pathways, breaking the coupling constraints between mechanics and ionics in high-loading electrodes.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70325","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wencheng Su, Chao Wang, Huiyan Zeng, Jianwen Wang, Long Gu, Mengxian Li, Liting Deng, Chi-Ying Vanessa Li, Chunzhen Yang
{"title":"Recycling Ni-Rich NCM Cathode Materials From Spent Li-Ion Batteries as Efficient Electrocatalyst for Urea Oxidation","authors":"Wencheng Su, Chao Wang, Huiyan Zeng, Jianwen Wang, Long Gu, Mengxian Li, Liting Deng, Chi-Ying Vanessa Li, Chunzhen Yang","doi":"10.1002/eem2.70314","DOIUrl":"https://doi.org/10.1002/eem2.70314","url":null,"abstract":"<p>The burgeoning electric vehicle industry has intensified the demand for high-energy Ni-Co-Mn (NCM) cathodes, yet their end-of-life management remains a critical environmental challenge. Here, we show that spent high-Ni NCM (LiNi<sub>0.92</sub>Co<sub>0.05</sub>Mn<sub>0.03</sub>O<sub>2</sub>) cathode materials can be directly upcycled into robust urea oxidation (UOR) catalysts. A facile solvent-only delamination converts discarded cathodes into printable inks; drop-casting onto carbon paper yields electrodes delivering ~10 mA mg<sup>−1</sup> at 1.50 V versus RHE. Operando synchrotron X-ray diffraction reveals that K<sup>+</sup> ions spontaneously intercalate into Li-deficient interlayers, expanding the (003) interplanar spacing from 4.7 to 7.1 Å. An electrochemical–chemical (E–C) reaction mechanism is proposed, in which Ni<sup>3+</sup> species are electrochemically generated on the catalyst surface and are then chemically reduced during urea oxidation, a process promoted by K<sup>+</sup> intercalation. This lattice-engineered redox process stabilizes the layered framework and suppresses metal dissolution, ensuring >24 h of continuous urea electrolysis. The work offers a circular economy solution for battery waste treatment while providing atomistic design principles for next-generation, earth-abundant environmental catalysts.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70314","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gunyoung Heo, Giyeok Lee, Ki-Tae Lee, Aloysius Soon, Taehun Lee
{"title":"Mechanistic Origins of Structural Failure in Deeply-Lithiated LixMoS2","authors":"Gunyoung Heo, Giyeok Lee, Ki-Tae Lee, Aloysius Soon, Taehun Lee","doi":"10.1002/eem2.70328","DOIUrl":"https://doi.org/10.1002/eem2.70328","url":null,"abstract":"<p>MoS<sub>2</sub> is a promising high-capacity anode for Li-ion batteries due to its layered structure and theoretical capacity of ∼670 mAh g<sup>−1</sup>, but its practical performance is limited by structural degradation under deep lithiation. Here, we employ a combination of global optimization and ab initio molecular dynamics (aiMD) to investigate the phase stability and structural failure mechanisms of Li-intercalated MoS<sub>2</sub> over a wide range of Li concentrations. Our results reveal that upon lithiation, MoS<sub>2</sub> undergoes a phase transformation from the 2H phase to a distorted 1T′ phase, with 1T′ Li<sub><i>x</i></sub>MoS<sub>2</sub> emerging as the most stable polymorph for <i>x</i> > 0.4. We further clarify how the initial Li distribution affects phase stability and structural fracture behavior. Through aiMD simulations, we find that pre-lithiated (ground-state) 1T′-Li<sub><i>x</i></sub>MoS<sub>2</sub> under the deep lithiation condition <i>x</i> > 1.0 exhibits enhanced structural integrity compared with a randomly-lithiated (high-energy) configuration. During aiMD simulation, the pre-lithiated Li<sub><i>x</i></sub>MoS<sub>2</sub> preserves the layered S–Mo–S framework up to higher Li concentrations (<i>x</i> ≃ 1.5), showing almost no S dislodgement while opening out-of-plane Li-ion diffusion channels via localized Mo–S bond cleavage. By contrast, dynamically-lithiated structures suffer from Mo–S bond breaking, early S dislodgement, and Li<sub><i>x</i></sub>S<sub><i>y</i></sub> cluster formation at the interfaces (notably around <i>x</i> in Li<sub><i>x</i></sub>MoS<sub>2</sub> ≃ 1.25). These findings suggest that controlling the initial Li intercalation geometry can significantly mitigate mechanical degradation in MoS<sub>2</sub> anodes, offering design guidelines for next-generation high-performance anodes with improved cycling stability and rate capability.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70328","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027985","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Unraveling Synergistic Regulation Mechanism in Nitrogen/Sulfur Co-Doped Biomass-Derived Hard Carbon Toward Durable Sodium-Ion Battery Anodes","authors":"Qian Long, Fangyuan Zhang, Jiayu Qu, Songtao Li, Renfei Cheng, Yaning Zhao, Di Guo, Zhengwang Zhu, Haifeng Zhang","doi":"10.1002/eem2.70276","DOIUrl":"https://doi.org/10.1002/eem2.70276","url":null,"abstract":"<p>Hard carbon (HC) materials featuring well-defined short-range ordered architectures have emerged as promising anode materials for sodium-ion batteries (SIBs). Nevertheless, due to the limited diffusion rate of sodium ions within the carbon structure, the rate capability of hard carbon at high current densities and long-term cycling stability remains a challenge. Herein, an innovative nitrogen/sulfur co-doping strategy is developed for loofah-derived hard carbon (LHC-N-S), synergistically regulating the electron defect and spatial structure. The synergistic charge regulation is attributed to the introduction of N atoms for ion adsorption and the improvement of electron conductivity. The spatial structure regulation mainly comes from the S doping to optimize the layer spacing and pore size, which facilitates the rapid ion diffusion kinetics. The obtained LHC-N-S anodes maintain a high reversible specific capacity (317.5 mAh g<sup>−1</sup> at 0.1 C) and ultralong lifespan (76% retention after 2000 cycles). Through the correlation analysis of the structural parameters and the Na<sup>+</sup> storage performance, the N/S co-doping mechanism is further clarified. This work provides deep insights into the design of high-performance biomass-derived hard carbon anodes for SIBs by leveraging the synergistic charge and space regulation through heteroatom doping, paving the way for the development of durable and sustainable sodium-ion battery technologies.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70276","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149029176","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Seulgi Kim, Kyoung Sun Kim, Young-Sang Yu, Ingyu Choi, Seungo Jeong, Eun-Jung Shin, Seung-Hyun Kim, Sung-Hak Jo, Seung-Ho Yu, Hyungsub Kim, Dongju Lee
{"title":"Redistributing Cobalt and Tungsten From WC–Co Soft Scrap Toward Sustainable Cathode and Coating Materials for Lithium-Ion Batteries","authors":"Seulgi Kim, Kyoung Sun Kim, Young-Sang Yu, Ingyu Choi, Seungo Jeong, Eun-Jung Shin, Seung-Hyun Kim, Sung-Hak Jo, Seung-Ho Yu, Hyungsub Kim, Dongju Lee","doi":"10.1002/eem2.70320","DOIUrl":"https://doi.org/10.1002/eem2.70320","url":null,"abstract":"<p>The scarcity of cobalt and tungsten causes unstable supply and sharp price fluctuations, emphasizing the urgent need for recycling and redistribution strategies. Herein, we develop an efficient upcycling route for recovering high-purity tungsten carbide and cobalt from cemented carbide (tungsten carbide–cobalt) soft scrap via mechanochemical ball milling and solvent extraction, and resynthesizing it into lithium-ion battery cathode materials. In this process, the residual nickel impurity is repurposed as a stabilizing dopant, reinforcing the layered framework at the cobalt sites of LiCoO<sub>2</sub> and suppressing lattice collapse even under high-voltage cycling. Benefiting from nickel incorporation at cobalt sites, the resynthesized LiCoO<sub>2</sub> exhibits markedly reduced c-lattice shrinkage and suppressed phase transitions at high voltages, evidenced by in situ X-ray diffraction. Such dopant-induced stabilization enables remarkable electrochemical durability, as resynthesized LiCoO<sub>2</sub> preserves over 60% of its capacity after 1000 cycles at 4.3 V (1 C) and retains 86.78% after 200 cycles at 4.5 V (0.2 C). Simultaneously, the tungsten carbide fraction is converted into tungsten trioxide and employed to modify nickel-rich layered oxides, mitigating interfacial degradation and improving durability. This cross-sectoral upcycling strategy exemplifies a circular economy approach by converting cemented carbide soft scrap from hard-metal applications into cathodes, directly linking industrial waste streams to the lithium-ion battery supply chain.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70320","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149029119","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jae Hyeon Choi, Yeon Oh Lee, Kyoung Sun Kim, Yun Chan Kang, Jung Sang Cho, Hyungsub Kim, Sang Mun Jeong, Gi Dae Park
{"title":"One-Pot Spray Pyrolysis Fabrication of Multi-Phase Lithium Manganese Oxide Microsphere Cathodes for Enhanced Lithium-Ion Battery Performance","authors":"Jae Hyeon Choi, Yeon Oh Lee, Kyoung Sun Kim, Yun Chan Kang, Jung Sang Cho, Hyungsub Kim, Sang Mun Jeong, Gi Dae Park","doi":"10.1002/eem2.70249","DOIUrl":"https://doi.org/10.1002/eem2.70249","url":null,"abstract":"<p>Spinel-type lithium manganese oxide (LMO) cathodes offer low cost, environmental benignity, and strong thermal safety, making them attractive for fast-charge lithium-ion batteries. Their widespread adoption, however, has been hindered by structural degradation associated with the Jahn–Teller distortion of Mn<sup>3+</sup>. Here, we report for the first time a rapid, single-step spray pyrolysis route that produces multi-phase microspheres comprising Sr-doped LiMn<sub>2</sub>O<sub>4</sub> spinel, a minor Sr<sub>2</sub>Mn<sub>2</sub>O<sub>5</sub> phase, and a C2/m layered Li<sub>2</sub>MnO<sub>3</sub>-like structure, all crystallized directly from a single precursor solution without post-treatment. This continuous aerosol process enables uniform Sr incorporation, precise morphological control, and manufacturing scalability. The synergistic coexistence of these phases provides multiple benefits: Sr doping lowers the Mn<sup>3+</sup> fraction, suppresses lattice distortion, and stabilizes the spinel framework; the Sr<sub>2</sub>Mn<sub>2</sub>O<sub>5</sub> phase refines particle morphology and mitigates mechanical stress during cycling; and the layered Li<sub>2</sub>MnO<sub>3</sub>-like domains enhance structural stability, diversify Li<sup>+</sup> diffusion pathways, and suppress Mn dissolution and electrolyte side reactions. As a result, the composite cathode delivers improved electrochemical performance, retaining 81.72 mA h g<sup>−1</sup> after 400 cycles at 1 C and 76.78 mA h g<sup>−1</sup> at 5 C, demonstrating that rapid, single-step spray pyrolysis is an effective and scalable strategy for robust, high-voltage spinel cathodes.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70249","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027733","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"On the Sustainability of Lithium-Ion Battery-Powered Electric Vehicles: Critical Review, Analysis, and Perspectives","authors":"Wanru Chen, Hangqi Yang, Nuoya Yue, Xiaoyu Yan, Tao Wu, Chuang Peng","doi":"10.1002/eem2.70345","DOIUrl":"https://doi.org/10.1002/eem2.70345","url":null,"abstract":"<p>With the rapid growth of the global lithium-ion battery-powered electric vehicle (EV) market, their overall sustainability becomes an emerging concern. This work reviews the most up-to-date literature and provides our own critical analysis and perspectives. The topics covered by this study include resource sustainability and greener manufacturing of lithium-ion batteries, greenhouse gas and air pollutant emissions of electric vehicles, and the impact of electric vehicle charging on the power grid. Briefly, the raw materials face low supply risks as the cathodes switch to low cobalt scenarios. For the greenhouse gas emissions, we first derive the equations for calculation of emissions from vehicle production, lithium-ion battery production, and the electric vehicle use phase. Subsequently, a heuristic-based method is adopted to determine the parameters and coefficients, while an Excel spreadsheet is created for facile calculations of the GHG emissions. This spreadsheet is included in the Supporting Information for free download and use. The benefits of greenhouse gas and air pollutant emission reduction for electric vehicles are obvious compared to internal combustion engine vehicles. In the future, these benefits will be further augmented by grid electricity decarbonization and deployment of more effective end-of-pipe air pollutant control measures. The charging of electric vehicles poses negative impacts on the stability of the power grid. However, if managed properly, these impacts can be effectively mitigated; moreover, EVs can even promote renewable electricity incorporation. Furthermore, this study summarizes greener manufacturing practices in lithium-ion battery production, which are beneficial for both resource sustainability and life-cycle emission reduction of electric vehicles.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70345","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149027830","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuqiong He, Shengping Hou, Jie Liu, Shengbo Ge, Siqun Wang, Mashallah Rezakazemi, Feng Liang, Guanben Du, Kaimeng Xu
{"title":"Electrospun Biomass-Derived Flexible Anodes With Hierarchical Structure via Cobalt MOF Integration for Sodium-Ion Batteries","authors":"Yuqiong He, Shengping Hou, Jie Liu, Shengbo Ge, Siqun Wang, Mashallah Rezakazemi, Feng Liang, Guanben Du, Kaimeng Xu","doi":"10.1002/eem2.70355","DOIUrl":"10.1002/eem2.70355","url":null,"abstract":"<p>To develop a green, sustainable, and high-performance anode for sodium-ion batteries (SIBs), flexible biomass-based carbon nanofiber membranes as a self-standing and structurally stable anode for SIBs were designed and fabricated by incorporating cellulose (CE) and chitosan (CS) with a cobalt-based metal–organic framework (ZIF-67) through two facile strategies: blending electrospinning–carbonization (CBNFM/ZIF-67) and electrospinning in situ growth–carbonization (CISNFM/ZIF-67). Compared with CISNFM/ZIF-67, the CBNFM/ZIF-67 anode displayed superior specific capacity, rate performance, and cycling stability, corresponding to 384.2 mAh g<sup>−1</sup> at 20 mA g<sup>−1</sup>, and maintaining a discharge capacity of 336.1 mAh g<sup>−1</sup> with a high Coulombic efficiency of 95.5% after 700 cycles at 100 mA g<sup>−1</sup>. The specific discharge capacity at 100 mA g<sup>−1</sup> and cycling stability of CBNFM/ZIF-67 significantly improved by 65.95% and 69.49% than the control (CNFM), respectively. The enhanced mechanism of sodium-ion insertion and desertion through construction and design of hierarchical pore structure, nitrogen-doping, and sodium-cobalt alloy was revealed by combining in situ Raman spectroscopy with density functional theory (DFT) calculation. CBNFM/ZIF-67 exhibited significantly higher binding energy (−774 kcal mol<sup>−1</sup>) and diffusion coefficient (12.88 e<sup>−7</sup> cm<sup>2</sup> s<sup>−1</sup>) than those of CISNFM/ZIF-67, revealing its superior ion transport kinetics. In addition, life cycle assessment demonstrates that the synthesis route offers an eco-friendly and low-carbon pathway for producing biomass-derived anodes. This study provides fundamental insights into sodium-ion insertion and extraction mechanisms, establishes a structure–property relationship for biomass-based electrodes, and presents a sustainable strategy for the large-scale development of sodium-ion batteries. These findings highlight the environmental and technological potential of green electrode materials for next-generation energy storage systems.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 6","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70355","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967054","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}