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Longitudinal Spatial Charge Transfer Optimization in Composite Cathode Enables Ultra-Stable All-Solid-State Batteries 复合阴极纵向空间电荷转移优化实现超稳定全固态电池
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-29 DOI: 10.1039/d5ee03407h
Junwei Liang, Kun Qian, Caijin Xiao, Yuhang Li, Zhichun Si, Lin Zeng, Songbai Han, Feiyu Kang, Yan-Bing He, Ming Liu
{"title":"Longitudinal Spatial Charge Transfer Optimization in Composite Cathode Enables Ultra-Stable All-Solid-State Batteries","authors":"Junwei Liang, Kun Qian, Caijin Xiao, Yuhang Li, Zhichun Si, Lin Zeng, Songbai Han, Feiyu Kang, Yan-Bing He, Ming Liu","doi":"10.1039/d5ee03407h","DOIUrl":"https://doi.org/10.1039/d5ee03407h","url":null,"abstract":"All-solid-state batteries (ASSBs) promise high energy density and inherent safety but face critical challenges in complex charge transfer process across the longitudinal cathode. Here, through multiphysics simulation, it is firstly revealed that charge transfer critically governs electrochemical reaction heterogeneity, dictating where reactions initiate preferentially along the lengthways of cathode. Building on this insight, a charge-transfer-optimized cathode (CTOC) is proposed to conceptually validate the effectiveness of charge-transfer regulation in homogenizing the longitudinal Li concentration. The CTOC features a double-layer architecture: a carbon-free layer with large-sized catholytes near separator to enhance Li-ion transfer while reduce electron conduction and a carbon-containing layer near current collector to ensure efficient electronic conductivity, thus tandem modulating the spatial ion and electron transfer dynamics longitudinally. Through graded ionic and electronic conduction to achieve decoupled but synchronized ion and electron transfer pathways, the CTOC enables longitudinally homogeneous Li distribution throughout the cathode. As a result, CTOC exhibits excellent cycling performance, retaining 82.7% capacity after 2000 cycles at 2C, a 27.4% durability improvement over conventional single-layer designs. This work establishes electrode-level charge transfer optimization as a design principle for heterogeneous reaction control, offering fundamental insights and practical strategies for high-performance ASSBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"21 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144719861","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
Origin and mitigation of premature dead Li formation at the current collector interface in high energy batteries 高能电池集流界面过早死锂形成的成因与缓解
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-29 DOI: 10.1039/d5ee02275d
Keyue Liang, Xintong Yuan, Bo Liu, Hayoung Park, Kaixi Chen, Tian-yu Wang, Haoyang Wu, Jung Tae Kim, Kaiyan Liang, Yuzhang Li
{"title":"Origin and mitigation of premature dead Li formation at the current collector interface in high energy batteries","authors":"Keyue Liang, Xintong Yuan, Bo Liu, Hayoung Park, Kaixi Chen, Tian-yu Wang, Haoyang Wu, Jung Tae Kim, Kaiyan Liang, Yuzhang Li","doi":"10.1039/d5ee02275d","DOIUrl":"https://doi.org/10.1039/d5ee02275d","url":null,"abstract":"Lithium metal battery (LMB) performance is strongly influenced by both Li deposition and stripping processes, which are closely related to the properties of the solid-electrolyte interphase (SEI). While most research focuses on optimizing Li deposition morphology, the stripping process and factors impacting its efficiency are often overlooked. In this study, we use cryo-electron microscopy (cryo-EM) and energy-dispersive X-ray spectroscopy (EDS) to analyze the structural and compositional properties of SEI films formed on both Li and Cu, investigating their respective roles in the stripping process. Our findings reveal that low-performing electrolytes exhibit dissimilar Li and Cu SEI compositions, which promote severe pinching near the base of the deposited Li metal, resulting in incomplete stripping and reduced Coulombic efficiency. In contrast, high-performing electrolytes display similar Li and Cu SEI compositions, which support uniform stripping and improve battery performance. This work highlights the critical role of achieving Li and Cu SEI compositional similarity to enhance stripping efficiency, offering valuable insights for future electrolyte design.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"26 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144736728","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 compactable Na2.5PS3.5F0.5 electrolyte for solid-state sodium batteries 一种用于固态钠电池的紧凑的Na2.5PS3.5F0.5电解质
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-28 DOI: 10.1039/d5ee00427f
Xianguang Miao, Yifan Wu, Huirong Jing, Yuchuang Cao, Yichao Wang, Junyeob Moon, Xin Li
{"title":"A compactable Na2.5PS3.5F0.5 electrolyte for solid-state sodium batteries","authors":"Xianguang Miao, Yifan Wu, Huirong Jing, Yuchuang Cao, Yichao Wang, Junyeob Moon, Xin Li","doi":"10.1039/d5ee00427f","DOIUrl":"https://doi.org/10.1039/d5ee00427f","url":null,"abstract":"Solid-state sodium batteries (NaSSBs) hold great promise due to their large-scale energy storage properties. However, the widely used sulfide electrolyte, Na<small><sub>3</sub></small>PS<small><sub>4</sub></small>, shows severe interface reaction with the anode and can be easily penetrated by Na dendrites during cycling. Here we propose a new type of Na<small><sub>2.5</sub></small>PS<small><sub>3.5</sub></small>F<small><sub>0.5</sub></small> (NPSF) electrolyte with comprehensive advantages over Na<small><sub>3</sub></small>PS<small><sub>4</sub></small>. It demonstrates a Na<small><sup>+</sup></small> conductivity of 0.27 mS cm<small><sup>−1</sup></small> and a low electronic conductivity of 3.9 × 10<small><sup>−6</sup></small> mS cm<small><sup>−1</sup></small> at room temperature. Benefiting from F-doping, NPSF demonstrates superior mechanical compactability, thus obtaining a dense electrolyte pellet with minimal defects, through a simple cold-pressing process. The assembled symmetric battery with Na<small><sub>15</sub></small>Sn<small><sub>4</sub></small> electrodes shows highly improved dendrite-resistant capability. Moreover, NPSF also exhibits increased electrochemical stability with Na<small><sub>15</sub></small>Sn<small><sub>4</sub></small>, enabling it to be a comprehensive upgrade over Na<small><sub>3</sub></small>PS<small><sub>4</sub></small>. A robust Na<small><sub>15</sub></small>Sn<small><sub>4</sub></small>/hard carbon composite electrode is further developed to pair with an NPSF electrolyte, where the assembled symmetric battery can demonstrate a high critical current density of 4.5 mA cm<small><sup>−2</sup></small>. Integrated full batteries of NaSSBs with a series of oxide cathodes of the high-performance 4 V class are achieved with high specific energy and power densities, as well as a long cycle life of over 1000 cycles.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"26 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144719862","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
Photon-coupled-proton buffers: reshaping solar-driven hydrogen and formic acid production with biomass 光子耦合质子缓冲:重塑太阳能驱动的氢和甲酸生产与生物质
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-28 DOI: 10.1039/d5ee01744k
Lei Gan, Yuyang Liu, Shiqi Huang, Yang Liu, Wei Liu, Kuang Sheng, Chenyu Zhang, Mingjun Han, Wenhao He, Jie Li, Xiong Li, Tao Jiang
{"title":"Photon-coupled-proton buffers: reshaping solar-driven hydrogen and formic acid production with biomass","authors":"Lei Gan, Yuyang Liu, Shiqi Huang, Yang Liu, Wei Liu, Kuang Sheng, Chenyu Zhang, Mingjun Han, Wenhao He, Jie Li, Xiong Li, Tao Jiang","doi":"10.1039/d5ee01744k","DOIUrl":"https://doi.org/10.1039/d5ee01744k","url":null,"abstract":"Solar-driven selective biomass conversion presents a promising pathway for green hydrogen production. However, conventional approaches are hindered by solar intermittency and the challenge of balancing conversion efficiency with over-oxidation. Here, we design photon-coupled-proton buffers (PCPBs) based on heteropolyacids, integrating photosensitivity, proton storage, and redox modulation. Under illumination, the PCPB material H<small><sub>5</sub></small>SiVMo<small><sub>2</sub></small>W<small><sub>9</sub></small>O<small><sub>40</sub></small>·10H<small><sub>2</sub></small>O catalyzes glucose oxidation to formic acid while capturing protons <em>via</em> self-reduction to heteropolyblue. This proton-rich species can be electrolyzed at ultralow potentials (0.58/0.62 V <em>vs.</em> RHE at 50/100 mA cm<small><sup>−2</sup></small>) for on-site H<small><sub>2</sub></small> production alongside PCPB self-regeneration. The system achieves 56.05% formic acid conversion from 0.1 M glucose and sustains H<small><sub>2</sub></small> evolution (≥91 mL H<small><sub>2</sub></small> per mmol glucose) over 14 cycles. Notably, the PCPB prototype delivers 82.44 g H<small><sub>2</sub></small> per kg of glucose in aqueous solution—23.78% higher than the theoretical H<small><sub>2</sub></small> output from aerobic glucose-to-formic acid conversion—surpassing conventional biomass photo-reforming. Furthermore, the PCPB is also effective for fructose, maltose, starch, and cellulose. Time-resolved spectroscopy and density functional theory (DFT) calculations reveal that Mo–O<small><sub>b</sub></small>–W sites enable photon-coupled-proton transfer under illumination, suppressing over-oxidation through dynamic proton buffering. By reshaping the photocatalytic biomass valorization pathway, this approach provides a proof-of-concept for stable, transportable, and energy-efficient solar-H<small><sub>2</sub></small> production.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"27 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144715640","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
Engineering ion-pumping solid electrolyte interphase for ultra-stable aqueous zinc-ion batteries under deep discharge conditions 深度放电条件下超稳定水锌离子电池的工程离子泵送固体电解质界面
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-26 DOI: 10.1039/d5ee01408e
Leixin Yang, Yujie Shen, Xintao Long, Qianyi Ma, Ziqing Ruan, Nuo Xu, Kaihua Li, Long Jiao, Yaping Kong, Jie Li, Lei Tang, Aiping Yu, Bowen Cheng
{"title":"Engineering ion-pumping solid electrolyte interphase for ultra-stable aqueous zinc-ion batteries under deep discharge conditions","authors":"Leixin Yang, Yujie Shen, Xintao Long, Qianyi Ma, Ziqing Ruan, Nuo Xu, Kaihua Li, Long Jiao, Yaping Kong, Jie Li, Lei Tang, Aiping Yu, Bowen Cheng","doi":"10.1039/d5ee01408e","DOIUrl":"https://doi.org/10.1039/d5ee01408e","url":null,"abstract":"Meeting the global terawatt-scale energy demands necessitates innovative solutions to overcome the critical challenges facing aqueous Zn-ion batteries, particularly the poor reversibility and unstable plating/stripping of Zn anodes under high depths of discharge (DOD). In this work, we introduce a novel composite artificial solid-electrolyte interphase (SEI), termed P-G, which combines a poly(ether-block-amide) matrix with graphene oxide (GO). By leveraging the functional groups of the polymer (C=O, C–O–C) and the electronegativity of GO, the P-G SEI layer acts as a highly efficient Zn2+ ion pump, achieving a remarkable Zn2+ transfer number of 0.77 and fast ion transport kinetics. Comprehensive theoretical and experimental analyses demonstrate that the P-G SEI layer regulates Zn2+ coordination and forms rapid ion transport pathways, leading to a highly stable and reversible Zn anode. As a result, P-G@Zn symmetric cells achieve ultra-stable cycling for 6500 hours at 1 mA·cm-2 and a record-breaking lifespan exceeding 5000 hours at 54.7% DOD. Furthermore, a high-specific-energy P-G@Zn||I2 pouch cell delivers exceptional performance, retaining 82.8% capacity after 400 cycles with an N/P ratio of 2. This study offers a compelling framework for designing advanced composite SEI layer, paving the way for highly reversible Zn-ion batteries in practical energy storage applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"21 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144710743","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
Correction: Ultrathin cellulosic gel electrolytes with a gradient hydropenic interface for stable, high-energy and flexible zinc batteries 更正:超薄纤维素凝胶电解质,具有梯度疏水界面,用于稳定,高能量和柔性锌电池
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-25 DOI: 10.1039/d5ee90076j
Jichao Zhai, Wang Zhao, Lei Wang, Jianbo Shuai, Ruwei Chen, Wenjiao Ge, Yu Zong, Guanjie He, Xiaohui Wang
{"title":"Correction: Ultrathin cellulosic gel electrolytes with a gradient hydropenic interface for stable, high-energy and flexible zinc batteries","authors":"Jichao Zhai, Wang Zhao, Lei Wang, Jianbo Shuai, Ruwei Chen, Wenjiao Ge, Yu Zong, Guanjie He, Xiaohui Wang","doi":"10.1039/d5ee90076j","DOIUrl":"https://doi.org/10.1039/d5ee90076j","url":null,"abstract":"Correction for ‘Ultrathin cellulosic gel electrolytes with a gradient hydropenic interface for stable, high-energy and flexible zinc batteries’ by Jichao Zhai <em>et al.</em>, <em>Energy Environ. Sci.</em>, 2025, <strong>18</strong>, 4241–4250, https://doi.org/10.1039/D5EE00158G.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"214 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701565","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
Decoupling Electrode Kinetics to Elucidate Reaction Mechanisms in Alkaline Water Electrolysis 解耦电极动力学研究碱水电解反应机理
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-25 DOI: 10.1039/d5ee03044g
Woo Yeong Noh, Samuel Joseph Kazmouz, Seong-hun Lee, Jui-Kun Peng, Tae Joo Shin, Meital Shviro
{"title":"Decoupling Electrode Kinetics to Elucidate Reaction Mechanisms in Alkaline Water Electrolysis","authors":"Woo Yeong Noh, Samuel Joseph Kazmouz, Seong-hun Lee, Jui-Kun Peng, Tae Joo Shin, Meital Shviro","doi":"10.1039/d5ee03044g","DOIUrl":"https://doi.org/10.1039/d5ee03044g","url":null,"abstract":"Alkaline water electrolysis (AWE) presents key advantages, including reduced material costs, enhanced operational stability, and compatibility with non-precious metal catalysts, positioning it as a scalable route for hydrogen production. In this study, we introduce a minimally invasive single-cell configuration incorporating a reference electrode via diaphragm extension to form an internal ion channel. This setup, combined with an interfaced potentiostat and auxiliary electrometer, enables real-time, independent monitoring of anode and cathode behavior, offering high-resolution electrochemical diagnostics. Contrary to conventional assumptions that hydrogen evolution reaction (HER) is kinetically more favorable than oxygen evolution reaction, we demonstrate that HER is significantly more sluggish in practical nickel-based AWE systems. This observation is supported by both experimental data and voltage breakdown modeling. Arrhenius-type analysis reveals that localized electric fields induced by catalysts shift the reaction kinetics from classical Butler–Volmer behavior toward a Marcus-like regime, where interfacial molecular dynamics and bimolecular charge transfer dominate. We propose a semi-empirical model and a surficial reaction mechanism to describe these dynamics. This work underscores the critical need for cathode innovation and provides a rational framework for designing advanced catalysts and electrode architectures to optimize AWE performance.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"21 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701636","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
Nanofluidic-enhanced high-mass-loading electrodes for energy-dense and high-rate lithium-sulfur batteries 用于能量密集和高倍率锂硫电池的纳米流体增强高质量负载电极
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-25 DOI: 10.1039/d5ee03001c
Chunlei Song, Lyuming Pan, Lu Chen, Yanxin Jiang, Hongji Pan, He Zhao, Nanshan Chen, Zhiqiang Yang, Liu Yang, Qing Yan, Xudong Peng, Xiaohua Ma, Yiju Li, Tianshou Zhao
{"title":"Nanofluidic-enhanced high-mass-loading electrodes for energy-dense and high-rate lithium-sulfur batteries","authors":"Chunlei Song, Lyuming Pan, Lu Chen, Yanxin Jiang, Hongji Pan, He Zhao, Nanshan Chen, Zhiqiang Yang, Liu Yang, Qing Yan, Xudong Peng, Xiaohua Ma, Yiju Li, Tianshou Zhao","doi":"10.1039/d5ee03001c","DOIUrl":"https://doi.org/10.1039/d5ee03001c","url":null,"abstract":"High-mass-loading sulfur cathodes with high areal capacity are critical for developing energy-dense lithium-sulfur (Li-S) batteries. However, facilitating efficient Li+ ion and electron transport in high-mass-loading sulfur electrodes remains a great challenge due to the extended pathways and inferior ion-electron transfer, especially at a high charge/discharge rate. To address the issue, we develop an ion-gated coating layer inspired by the nanofluidic effects in organisms (IGCL-NFE), which enhances the Li+ diffusion coefficient (D) and transference number (µ+) to enable ultrafast and selective Li+ transport in thick sulfur electrodes. The IGCL-NFE exhibits a characteristic biomimetic nanofluidic ion transport behavior, yielding a high µ+ (~2.1 times higher than that in the bulk solution) and a high D (~1012 times higher than that in the bulk solution) at a low Li salt concentration of 10-6 mol L-1. With selective and fast Li+ conduction, coupled with the high electrical conductivity of the IGCL-NFE, the IGCL-NFE-enhanced sulfur cathode demonstrates exceptional rate performance (757.8 mAh g-¹ after 300 cycles) at a high rate of 10.0 C. As a proof of concept, Li-S batteries utilizing the dry electrode with an ultrahigh sulfur loading of 18.7 mg cm-2 achieve an impressive energy density of 430.6 Wh kg-1. Furthermore, the Li-S full cell exhibits stable cycling performance over 100 cycles, retaining a high capacity of 1313.9 mAh g-¹ even at -20 °C. The nature-inspired, nanofluidic-enhanced electrode design presents a promising strategy for developing ultrahigh-mass-loading and high-rate Li-S batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"90 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701637","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
Correction: Carbon footprint of oil produced through enhanced oil recovery using carbon dioxide directly captured from air 更正:通过直接从空气中捕获二氧化碳提高采收率而产生的石油的碳足迹
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-24 DOI: 10.1039/d5ee90077h
Antonio Gasós, Ronny Pini, Viola Becattini, Marco Mazzotti
{"title":"Correction: Carbon footprint of oil produced through enhanced oil recovery using carbon dioxide directly captured from air","authors":"Antonio Gasós, Ronny Pini, Viola Becattini, Marco Mazzotti","doi":"10.1039/d5ee90077h","DOIUrl":"https://doi.org/10.1039/d5ee90077h","url":null,"abstract":"Correction for ‘Carbon footprint of oil produced through enhanced oil recovery using carbon dioxide directly captured from air’ by Antonio Gasós <em>et al.</em>, <em>Energy Environ. Sci.</em>, 2025, https://doi.org/10.1039/d5ee01752a.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"20 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693843","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
An Unwanted Guest in the Electrochemical Oxidation of High-Voltage Li-ion Battery Electrolytes: The Life of Highly Reactive Protons 高压锂离子电池电解液电化学氧化中的不速之客:高活性质子的寿命
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2025-07-24 DOI: 10.1039/d5ee02403j
Stefan Ilic, Milena Zorko, Haoyu Liu, Pedro Farinazzo Bergamo Dias Martins, Dominik Haering, Jingtian Yang, Toru Hatsukade, Bostjan Genorio, Stephen Weitzner, Liwen Wan, Zhengcheng Zhang, Justin G. Connell, Baris Key, Jordi Cabana, Dusan Strmcnik
{"title":"An Unwanted Guest in the Electrochemical Oxidation of High-Voltage Li-ion Battery Electrolytes: The Life of Highly Reactive Protons","authors":"Stefan Ilic, Milena Zorko, Haoyu Liu, Pedro Farinazzo Bergamo Dias Martins, Dominik Haering, Jingtian Yang, Toru Hatsukade, Bostjan Genorio, Stephen Weitzner, Liwen Wan, Zhengcheng Zhang, Justin G. Connell, Baris Key, Jordi Cabana, Dusan Strmcnik","doi":"10.1039/d5ee02403j","DOIUrl":"https://doi.org/10.1039/d5ee02403j","url":null,"abstract":"Lithium-ion batteries (LIBs) are central to the urgent societal need to decarbonize both transportation and energy storage on the grid. Unfortunately, despite their attractive energy/power density, as well as high Coulombic and energy efficiencies, further improvement of this technology – especially their durability – is desperately needed. To support these efforts, our study focuses on fundamental understanding of the decomposition pathways for LIB electrolytes at the cathode-electrolyte interface (CEI), as the nature of these reactions directly controls the extent to which cell capacity and voltage decays in these systems. In this study, we employ electrochemical methods, coupled with product analysis using NMR spectroscopy and mass spectrometry, to determine the decomposition mechanisms in both model and technologically relevant electrolytes. Remarkably, we discovered the electrochemical formation of protons with high chemical activity, comparable to known superacids, at potentials relevant to practical Li-ion batteries. Their reactivity toward every individual component of the CEI provides a unified thermochemical origin for a myriad of side reactions that are commonly associated with the electrochemical reaction. In particular, electrochemically generated protons react with intact EC molecules to form CO<small><sub>2</sub></small> and other short and long chain ethers. They also undergo an acid-base reaction with LiPF<small><sub>6</sub></small>, to form the weaker acid HF, and with the cathode active material, leaching transition metals into the electrolyte. Collectively, the results of this study all point to the urgent need to either mitigate this proton formation or introduce benign harvesting additives via new electrolyte design strategies.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"702 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693844","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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