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Interfacial hydrogen bond modulation of dynamic catalysts for nitrate electroreduction to ammonia 硝酸电还原制氨动力学催化剂的界面氢键调节
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-11 DOI: 10.1039/d5ee00597c
Yuchi Wan, Yixiang Tang, Yinze Zuo, Kaian Sun, Zewen Zhuang, Yun Zheng, Wei Yan, Jiujun Zhang, Ruitao Lv
{"title":"Interfacial hydrogen bond modulation of dynamic catalysts for nitrate electroreduction to ammonia","authors":"Yuchi Wan, Yixiang Tang, Yinze Zuo, Kaian Sun, Zewen Zhuang, Yun Zheng, Wei Yan, Jiujun Zhang, Ruitao Lv","doi":"10.1039/d5ee00597c","DOIUrl":"https://doi.org/10.1039/d5ee00597c","url":null,"abstract":"Electrocatalytic nitrate reduction (NO3−RR) shows potentials in clean NH3 synthesis and industrial effluent disposal, turning waste into treasure. However, the catalyst reconstruction mechanism is still ambiguous, and the influence of interfacial hydrogen bond on NO3−RR performance remains unexplored. Herein, a Cr doping strategy is developed to regulate interfacial hydrogen-bonded interactions on the Co-based dynamic electrocatalyst for improving electrocatalytic NO3−RR activity. In-situ XRD, in-situ Raman and theoretical calculations indicate that doping Cr can modulate the reconstruction process of the Co-based material, achieving the dynamic balance of Co(OH)2 and Co. Moreover, molecular dynamics simulations, density functional theory calculations combined with in-situ infrared spectra reveal that strong hydrogen-bonded interactions between interfacial H2O and the Cr doped Co(OH)2 surface can drag more free H2O from rigid H2O network and facilitate the H2O dissociation with the formation of active hydrogen for accelerating the NO3−RR pathway on metallic Co site. As a result, the Cr doped Co-based dynamic electrocatalyst can display a superior NH3 Faradaic efficiency of 97.36% and a high NH3 yield rate of 58.92 mg h-1 cm-2, outperforming the state-of-art electrocatalysts. This work can further inspire the dynamic electrocatalyst design and interfacial microenvironment modulation for electrochemical hydrogenation reactions.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"25 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819130","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}
引用次数: 0
A Universal Surface Fixed Charge Reconstruction Strategy to Minimize Contact Loss of Wide Bandgap Perovskite Photovoltaics 一种减少宽禁带钙钛矿光伏电池接触损耗的通用表面固定电荷重建策略
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-11 DOI: 10.1039/d4ee05855k
Yaxiong Guo, Fang Yao, Yunchen Zhang, Guoyi Chen, Shengjie Du, Zhixi Yu, Hai Zhou, Weijun Ke, Chun Li, Guojia Fang
{"title":"A Universal Surface Fixed Charge Reconstruction Strategy to Minimize Contact Loss of Wide Bandgap Perovskite Photovoltaics","authors":"Yaxiong Guo, Fang Yao, Yunchen Zhang, Guoyi Chen, Shengjie Du, Zhixi Yu, Hai Zhou, Weijun Ke, Chun Li, Guojia Fang","doi":"10.1039/d4ee05855k","DOIUrl":"https://doi.org/10.1039/d4ee05855k","url":null,"abstract":"It is widely accepted that non-radiative recombination losses in the wide-bandgap (WBG) subcell dominate carrier recombination processes in perovskite tandem photovoltaics. We demonstrate that healing the perovskite top-surface with an additive potassium thioglycolate (PT) inhibits Pb-Pb dimer formation at the top surface, which is especially urgent in ultra-WBG perovskite CsxFA1-xPb(I1-yBry)3 (y>0.6). Concurrently, field effect passivation, induced by the ordered arrangement of linear diamine 1,3-diammonium (PDA2+) and associated adequate surface fixed charge, are reconstituted. This “healing-reconstruction” strategy suppresses cross-interface recombination and boosts open circuit voltage (VOC), delivering the highest VOC value reported to date for 1.91 eV perovskite. The strategy allows us to approach the potential of VOC (VOC losses<10% of the SQ limit) in single-junction applications employing band gaps in the range from 1.6 to 1.9 eV, that is critical for tandem solar cells.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"6 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819131","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}
引用次数: 0
Deciphering the Interplay between Tin Vacancies and Free Carriers in the Ion Transport of Tin-Based Perovskites 解析锡基钙钛矿离子输运中锡空位与自由载流子的相互作用
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-11 DOI: 10.1039/d5ee00632e
Luis Huerta Hernandez, Luis Lanzetta, Anna M. Kotowska, Ilhan Yavuz, Nikhil Kalasariya, Badri Vishal, Martí Gibert-Roca, Matthew Piggott, David J Scurr, Stefaan De Wolf, Martin Stolterfoht, Derya Baran
{"title":"Deciphering the Interplay between Tin Vacancies and Free Carriers in the Ion Transport of Tin-Based Perovskites","authors":"Luis Huerta Hernandez, Luis Lanzetta, Anna M. Kotowska, Ilhan Yavuz, Nikhil Kalasariya, Badri Vishal, Martí Gibert-Roca, Matthew Piggott, David J Scurr, Stefaan De Wolf, Martin Stolterfoht, Derya Baran","doi":"10.1039/d5ee00632e","DOIUrl":"https://doi.org/10.1039/d5ee00632e","url":null,"abstract":"Mixed ionic-electronic conduction is a prevalent phenomenon in metal halide perovskites, having a critical impact in multiple optoelectronic applications. In Sn-based halide perovskites, their higher hole density ([p]) owing to the facile formation of Sn vacancies (V<small><sub>Sn</sub></small><small><sup>-2</sup></small>) induces substantial electronic transport differences versus their Pb-based analogues. However, the influence of [p] and V<small><sub>Sn</sub></small><small><sup>-2</sup></small> on their ionic transport properties remains elusive. Herein, the link between electronic and ionic transport is unravelled in a compendium of Sn-based perovskite compositions. Specifically, ionic and electronic conductivities are found to concomitantly rise with higher Sn content. Using a combination of electrical characterization techniques, a rise in [p] and V<small><sub>Sn</sub></small><small><sup>-2</sup></small> is demonstrated to increase mobile ion density, enhancing lateral ion migration and ionic conductivity. First-principles simulations reveal that [p] and V<small><sub>Sn</sub></small><small><sup>-2</sup></small> jointly lower the energy barrier for iodide migration from 0.38 eV to 0.12 eV. Chemical mapping techniques support these observations by identifying the bias-induced migration of iodide and formamidinium ions in compositions with higher [p] and V<small><sub>Sn</sub></small><small><sup>-2</sup></small>. These fundamental insights on the ionic-electronic coupling will enable next-generation of Sn-based perovskite technologies with improved performance and stability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"66 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819187","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}
引用次数: 0
Recent Advances in Perovskite Air Electrode Materials for Protonic Solid Oxide Electrochemical Cells 质子固体氧化物电化学电池用钙钛矿空气电极材料的研究进展
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-10 DOI: 10.1039/d5ee00983a
Cancan Peng, xu han, Sebete S Mabaleha, Philip Kwong, Yao Zheng, Xiaoyong Xu
{"title":"Recent Advances in Perovskite Air Electrode Materials for Protonic Solid Oxide Electrochemical Cells","authors":"Cancan Peng, xu han, Sebete S Mabaleha, Philip Kwong, Yao Zheng, Xiaoyong Xu","doi":"10.1039/d5ee00983a","DOIUrl":"https://doi.org/10.1039/d5ee00983a","url":null,"abstract":"Intermediate-temperature proton-conducting solid oxide cells (P-SOCs) have emerged as a promising technology for power generation and hydrogen production. They have gained significant attention due to their lower operating temperature, higher efficiency, better safety and durability and simplified water management over conventional high-temperature oxygen-conducting solid oxide cells (O-SOCs). However, the performance of P-SOC air electrodes is hindered by the sluggish kinetics of oxygen reduction and evolution reactions, necessitating efficient conductivities of H+, O2−, and e−. Despite critical advancements, the search for optimal air electrode materials remains challenging. This review provides a comprehensive overview of recent advancements in perovskite materials for P-SOC air electrodes, covering from fundamental mechanisms, material development, theoretical modeling, and practical applications. It highlights key progress in reaction kinetics, structure–property relationships, and modification strategies across widely studied perovskite-based systems. Particular emphasis is placed on understanding the correlation between structural characteristics and the electrochemical activity and stability of electrodes, which is essential for the rational design of high-performance, durable P-SOC materials. Additionally, advanced methodologies and mechanistic insights into newly developed air electrode materials are explored, with a focus on the role of theoretical simulations, including artificial intelligence (AI)-driven machine learning (ML) techniques. Finally, perspectives are provided on the future development of high-performance P-SOC air electrodes for industrial applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"25 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813690","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}
引用次数: 0
Fluorine-Free Electrolytes in Batteries: Principles, Strategies, and Advances 电池中的无氟电解质:原理、策略和进展
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-10 DOI: 10.1039/d4ee04820b
Boligarla Vinay, Yosef Nikodimos, Tripti Agnihotri, Shadab Ali Ahmed, Teklay Mezgebe Hagos, Rehbar Hasan, Elango Balaji Tamilarasan, Wei-Nien Su, Bing Joe Hwang
{"title":"Fluorine-Free Electrolytes in Batteries: Principles, Strategies, and Advances","authors":"Boligarla Vinay, Yosef Nikodimos, Tripti Agnihotri, Shadab Ali Ahmed, Teklay Mezgebe Hagos, Rehbar Hasan, Elango Balaji Tamilarasan, Wei-Nien Su, Bing Joe Hwang","doi":"10.1039/d4ee04820b","DOIUrl":"https://doi.org/10.1039/d4ee04820b","url":null,"abstract":"Electrolytes play a pivotal role in battery technologies, influencing performance and safety. However, electrolytes containing fluorine present adverse environmental risks due to their high greenhouse gas emissions and caution of global warming. Hence, developing fluorine-free alternatives is imperative to design net-zero fluorine electrolytes. This review addresses the need for sustainable, low-toxicity electrolytes by exploring strategies for eliminating fluorine in the electrolytes system. Studies on the choice of electrolyte ingredients, such as fluorine-free salts, green solvents, safe additives, and fluorine-free binders, effectively enhance battery performance and safety. Recent progress highlights significant improvements in the environmental impact and functionality of fluorine-free electrolytes (FFEs), demonstrating their potential for practical applications. Despite these advancements, challenges remain in matching the performance and stability of traditional fluorinated electrolytes. Future research encourages to focus on developing fluorine-free materials, understanding functional degradation processes, and ensuring commercial scalability. This review provides an in-depth look at recent innovations and promotes design principles for complete fluorine elimination strategies. It guides future pathways for creating high-performance, non-flammable, low-cost, environmentally sustainable FFEs for advanced rechargeable batteries. The summary and perspectives emphasize the importance and future directions of a sustainable circular economy in advancing sustainable electrolyte engineering.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"30 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813796","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}
引用次数: 0
High-Iodine-Loading Quasi-Solid-State Zinc-Iodine Batteries Enabled by a Continuous Ion-Transport Network 用连续离子传输网络实现高碘负载准固态锌碘电池
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-10 DOI: 10.1039/d5ee01170a
Xin Yang, Minghao Xie, Zhijie Yan, Hang Ruan, Chunpeng Yang, Zaiping Guo, Zi-Jian Zheng
{"title":"High-Iodine-Loading Quasi-Solid-State Zinc-Iodine Batteries Enabled by a Continuous Ion-Transport Network","authors":"Xin Yang, Minghao Xie, Zhijie Yan, Hang Ruan, Chunpeng Yang, Zaiping Guo, Zi-Jian Zheng","doi":"10.1039/d5ee01170a","DOIUrl":"https://doi.org/10.1039/d5ee01170a","url":null,"abstract":"Zinc-iodine (Zn–I₂) batteries are promising candidates for next-generation large-scale energy storage systems due to their inherent safety, environmental sustainability, and potential cost-effectiveness compared to lithium-ion batteries. Their applications, however, have been limited by the sluggish Zn2+ transfer kinetics, severe polyiodide shuttling, and relatively low mass loading of iodine cathodes. Herein, we report a design strategy for a quasi-solid-state Zn–I₂ battery with a continuous 3D ion-transport network by integrating a thick iodine cathode and a bacterial cellulose hydrogel electrolyte. The polar bacterial cellulose fibers formed an interconnected network that provided abundant ion pathways for inward Zn2+ transport and also limited iodine species dissolution. The continuous 3D ion-transport networks were formed throughout the entire thick iodine cathode, resulting in a 10-times higher Zn-ion conductivity compared with the conventional-structured cathode. The quasi-solid-state Zn–I2 battery based on the Zn anode and an integrated cathode delivered a reversible capacity of 176.6 mAh g−1 and achieved long-term cycling for 900 cycles at 1 C under a iodine loading of 20.0 mg cm−2. The iodine loading can be further increased to 39.3 mg cm−2 by adjusting the thickness of cathode. Under a practical condition of low negative/positive ratio (N/P) of 2.1, an energy density of 56.4 Wh kg−1 is achieved. This integrated electrode design provides guidelines for fabricating high-energy quasi-solid-state Zn ion batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"18 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813797","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}
引用次数: 0
Galvanic Corrosion Underlies Coulombic Efficiency Differences in High-Performing Lithium Metal Battery Electrolytes 电偶腐蚀是高性能锂金属电池电解质库仑效率差异的基础
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-10 DOI: 10.1039/d5ee00071h
Solomon T. Oyakhire, Sang Cheol Kim, Wenbo Zhang, Sanzeeda Baig Shuchi, Yi Cui, Stacey Bent
{"title":"Galvanic Corrosion Underlies Coulombic Efficiency Differences in High-Performing Lithium Metal Battery Electrolytes","authors":"Solomon T. Oyakhire, Sang Cheol Kim, Wenbo Zhang, Sanzeeda Baig Shuchi, Yi Cui, Stacey Bent","doi":"10.1039/d5ee00071h","DOIUrl":"https://doi.org/10.1039/d5ee00071h","url":null,"abstract":"Current guidelines for electrolyte engineering in lithium metal batteries are based on design metrics such as lithium morphology, electrolyte transport properties, solid electrolyte interphase (SEI) characteristics, and lithium-electrolyte reactivity. In our work, we show that those design metrics fail to account for performance differences in new high-performing electrolytes whereas galvanic corrosion does. This insight regarding the importance of galvanic corrosion is enabled by the combination of machine learning with rigorous experimental characterization. First, we partition our electrolyte data into low and high Coulombic efficiency (CE) segments to obtain an interpretable machine learning model which informs the design of high-performing (high CE) electrolytes. We design new model-guided, high-performing electrolytes and use spectroscopy and electroanalytical methods to demonstrate the weak correlation between common design metrics and performance in the high-performing electrolytes. Our work results in the design of a high-performing electrolyte with a Coulombic efficiency (CE) of 99.6%, a new understanding that common performance indicators are not sufficient for informing the development of high-performing electrolytes, and the identification of galvanic corrosion as an important performance driver in high-performing electrolytes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"12 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819190","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}
引用次数: 0
High-Conversion-Efficiency and Stable Six-Electron Zn-I2 Batteries Enabled by Organic Iodide/Thiazole-Linked Covalent Organic Frameworks 有机碘化物/噻唑共价有机框架实现高转换效率和稳定的六电子Zn-I2电池
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-09 DOI: 10.1039/d5ee00365b
Wenyan Du, Qi Huang, Xunwen Zheng, Yaokang Lv, Ling Miao, Ziyang Song, Lihua Gan, Mingxian Liu
{"title":"High-Conversion-Efficiency and Stable Six-Electron Zn-I2 Batteries Enabled by Organic Iodide/Thiazole-Linked Covalent Organic Frameworks","authors":"Wenyan Du, Qi Huang, Xunwen Zheng, Yaokang Lv, Ling Miao, Ziyang Song, Lihua Gan, Mingxian Liu","doi":"10.1039/d5ee00365b","DOIUrl":"https://doi.org/10.1039/d5ee00365b","url":null,"abstract":"Six-electron I−/I5+ redox chemistry gives a promising platform to propel high-capacity Zn-I2 batteries, but faces limited conversion efficiency and instability of IO3− species. Here we design a thiazole-linked covalent organic frameworks (TZ-COFs) hosted organic trimethylsulfonium iodide (C3H9IS/TZ-COFs) electrode in 1-methyl-3-propylimidazolium bromide (MPIBr)-containing electrolyte to stimulate I−/I0/I+/I5+ iodine conversion chemistry with better electrochemical efficiency and stability. Compared with inorganic symmetric I2 molecules, the more easily exposed I− center of polar C3H9IS combines with the oxygen in H2O to form HIO3, which initiates 6 e− I−/IO3− conversion through I+ activation of MPIBr, thus reducing the oxidation/reduction potential gap to achieve 97% iodine conversion efficiency. Meanwhile, thiazole units of TZ-COFs enable strong chemical adsorption with IO3− species to improve redox stability with high reversibility due to reduced energy barriers (−5.1 vs. −3.5 eV in activated carbon (AC) host) and upgraded conversion kinetics (activation energy: 0.21 vs. 0.38 eV in AC). Such a stable and high-efficiency 6 e− iodine conversion gives C3H9IS/TZ-COFs electrode record capacity (1296 mAh g−1) and energy density (1464 Wh kg−1), and superior cycling stability (1200 cycles). These findings constitute a major advance for the design of iodine redox chemistry towards state-of-the-art Zn-I2 batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"38 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806161","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}
引用次数: 0
Mitigating chemo-mechanical heterogeneity of Ni-rich layered cathodes through the regulated medium-range order by doping 通过掺杂调节中程有序性缓解富镍层状阴极的化学机械异质性
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-09 DOI: 10.1039/d5ee01180a
Junfeng Luo, Gi-Hyeok Lee, Jiliang Zhang, Seongkoo Kang, Chi Liang Chen, Chung-Kai Chang, Zheng-Yao Li, Ronghua Zeng, Hong Li, Jialu Li, Ruirui Zhao, Qifeng Zheng, Yong-Mook Kang
{"title":"Mitigating chemo-mechanical heterogeneity of Ni-rich layered cathodes through the regulated medium-range order by doping","authors":"Junfeng Luo, Gi-Hyeok Lee, Jiliang Zhang, Seongkoo Kang, Chi Liang Chen, Chung-Kai Chang, Zheng-Yao Li, Ronghua Zeng, Hong Li, Jialu Li, Ruirui Zhao, Qifeng Zheng, Yong-Mook Kang","doi":"10.1039/d5ee01180a","DOIUrl":"https://doi.org/10.1039/d5ee01180a","url":null,"abstract":"Structural heterogeneity-induced chemo-mechanical interplay has been identified as the primary reason for the capacity degradation of high-voltage Ni-rich layered cathodes. In the current study, two dopants known to have different site occupancies in Ni-rich layered cathodes, Mg and W, are revisited, revealing the relationship between dopant-induced local structure changes and electrochemical reversibility across a broad charge/discharge voltage range. Our results indicate that the introduced W induces Li-W-Li medium-range order (MRO), resulting in a lower electron concentration in O 2p orbitals. The MRO in a W-doped Ni-rich layered oxide (LNCW) triggers asymmetry in the NiO6 octahedra and weakens the surrounding hybridization, leading to a highly covalent Ni4+-O bond and activating charge transfer from the ligand. Although the contribution of oxygen oxidation was somewhat reduced in LNCW, the distorted NiO6 octahedra arising from deepened cationic oxidation worsened the electrochemical performance significantly. By contrast, Mg occupies the 3b site of Li and thereby forms MgO4 tetrahedra, inducing Ni-Mg-Ni MRO and a resulting charge redistribution that shrinks the Ni 3d orbital band, leading to a reversible Ni-redox process and suppressing oxygen oxidation. Hence, the Mg-doped Ni-rich layered oxide (LNCMg) maintains superior structural integrity to LNCW, avoiding the parasitic distortion of NiO6 octahedra and alleviating the chemo-mechanical heterogeneity. This work underscores the significance of medium-range order in the chemo-mechanical interplay in Ni-rich layered cathodes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"108 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806450","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}
引用次数: 0
Advanced Energy Harvesting from Low-Frequency Ocean Waves for Lithium-Ion Battery Applications 用于锂离子电池的低频海浪先进能量收集
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-04-09 DOI: 10.1039/d5ee01492a
Yingjin Luo, Wentao Lei, Pengfei Chen, Tao Jiang, Andeng Liu, Meidan Ye, Zijie Xu, Zhong Lin Wang, Wenxi Guo
{"title":"Advanced Energy Harvesting from Low-Frequency Ocean Waves for Lithium-Ion Battery Applications","authors":"Yingjin Luo, Wentao Lei, Pengfei Chen, Tao Jiang, Andeng Liu, Meidan Ye, Zijie Xu, Zhong Lin Wang, Wenxi Guo","doi":"10.1039/d5ee01492a","DOIUrl":"https://doi.org/10.1039/d5ee01492a","url":null,"abstract":"The low root mean square (RMS) current density generated by triboelectric nanogenerators (TENGs) has significantly hindered their effectiveness in charging lithium batteries. In response, we present a universal energy storage strategy for TENGs specifically designed for real marine environments, facilitating effective charging of lithium batteries for the first time. By integrating multiple grating electrodes and a ternary electrification architecture with an opposite-charge compensation mechanism, we increased the RMS current density of TENGs to 57.19±0.23 mA·m⁻²·Hz⁻¹. Additionally, we designed a lithium polymer charge management module that further boosts the RMS current density to 0.86±0.02 A·m⁻²·Hz⁻¹, a 14-fold improvement, enabling direct charging of 30 mAh and 40 mAh lithium batteries in 2.33±0.05 h and 3.73±0.14 h, respectively. Building on this foundation, we developed a self-powered remote (0.65 nautical miles) monitoring sensor network tailored for marine applications, enabling the initial use of Internet of Things technology in a marine environment.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"18 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806158","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}
引用次数: 0
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