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}
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}
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}
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}
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}
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}
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}
{"title":"Interface parallel dipole regulation in all-perovskite tandem solar cells","authors":"Yue Zhao, Tianshu Ma, Xinxing Yin, Luwei Zhou, Yuqi Zhang, Zhanghao Wu, Chen Chen, Yuhui Liu, Zhenhai Yang, Lin Hu, Zaifang Li, Cong Chen, Hao Tian, Chuanxiao Xiao, Zijun Chen, Bingsuo Zou, Long Jiang, Dewei Zhao, Xiaofeng Li, Changlei Wang","doi":"10.1039/d5ee02696b","DOIUrl":"https://doi.org/10.1039/d5ee02696b","url":null,"abstract":"The abstract should be a single paragraph that summarises the content of the article Constructing all-perovskite tandem solar cells (TSCs) provides an effective route to surpass the efficiency limit of single-junction devices. However, huge non-radiative recombination losses in wide-bandgap (WBG) subcells degrade their performance from theoretical predictions. Here, we propose a parallel dipole engineering strategy employing tailored phenoxyethylammonium halides (POEAX, X=I, Br, Cl) to simultaneously heal defects and modulate interfacial electric fileds. POEA+ forms parallel dipole moment at the perovskite/C60 interface, effectively binding with Pb2+ defects and enhancing the carrier transport. Synergistically, Cl- amplifies the dipole-bridged defect healing and optimizes the energy level alignment, leading to highly improved film homogeneity and suppressed recombination. These advantages lead to a power conversion efficiency (PCE) of 19.54% and a remarkable open-circuit voltage of 1.352 V in 1.77 eV WBG perovskite solar cells (PSCs). Furthermore, integrated with low-bandgap PSCs, all-perovskite TSCs with a champion PCE of 28.92% (certified 28.51%) and excellent stability are realized.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"52 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693949","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}
Yutong Zhai, Yimu Zhang, Ning Wang, Minghui Li, Mingjia Shen, Pingbo Xu, Maoyu Sun, Feilong Dong, Tian Zong Ma, Jun Ming, Lina Cong, Haiming Xie, Yulong Liu
{"title":"Dense Li deposition enabled by weakly coordinated Li and fast Li transport single-ion conducting gel-polymer electrolyte","authors":"Yutong Zhai, Yimu Zhang, Ning Wang, Minghui Li, Mingjia Shen, Pingbo Xu, Maoyu Sun, Feilong Dong, Tian Zong Ma, Jun Ming, Lina Cong, Haiming Xie, Yulong Liu","doi":"10.1039/d5ee02373d","DOIUrl":"https://doi.org/10.1039/d5ee02373d","url":null,"abstract":"Polymer electrolytes face fundamental challenges in simultaneously achieving rapid Li+ transport and weak Li+-anion/solvent bonding. To address this bottleneck, this study introduces a molecular-level stepwise regulation of solvation structures in a gel-polymer electrolyte (GPE). By weakening the strong Li+-solvent coordination via NO3-, immobilizing anions with PFPN, and utilizing the shielding effect of the NO3--TFSI--FSI- triplet anion in the solvated structure, the Li-coordination is sequentially reduced. The lithium-ion transport mechanism evolves from a vehicular transport mechanism of the entire primary solvation sheath (directional movement within the first solvation shell) to a Li⁺-hopping conduction mechanism (Li⁺ jumping between different coordination sites). Consequently, a single ion conducting GPE (SIC-GPE+PFPN+LiFSI) achieves a high lithium-ion transference number (0.92) and high conductivity of 2.58 mS cm-1. Due to the alleviation of space-charge effect at anode interface with higher tLi+, the Li nucleation over-potential and deposition over-potential are significantly reduced, while the critical current density (CCD) reaches 8 mA cm-2 for SIC-GPE+PFPN+LiFSI. Additionally, the exchange current density of SIC-GPE+PFPN+LiFSI is increased, which results in smooth and dense Li deposition morphology. With PFPN derived cathode interphase interlayer (CEI) on the NCM622 cathode, the high-voltage lithium metal battery (LMB) operates stably for over 300 cycles, which is 30 times higher than the GPE without PFPN. This research unveils the secrets of relationship between ultra-high lithium-ion transference number electrolytes with dense Li deposition and provides essential insights for the development of high-energy-density lithium metal batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"47 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693872","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}
Yue Chen, Wenye Xuan, Weijian Zhang, Mangayarkarasi Nagarathinam, Guiying Zhao, Jianming Tao, Jiaxin Li, Long Zhang, Yingbin Lin, Yubiao Niu, Hsin-Yi Tiffany Chen, Svetlana Menkin, Dominic S. Wright, Clare P. Grey, Oleg Victor Kolosov, Zhigao Huang
{"title":"Hidden Subsurface Molecular Bubbles in Graphite Anodes for LIBs","authors":"Yue Chen, Wenye Xuan, Weijian Zhang, Mangayarkarasi Nagarathinam, Guiying Zhao, Jianming Tao, Jiaxin Li, Long Zhang, Yingbin Lin, Yubiao Niu, Hsin-Yi Tiffany Chen, Svetlana Menkin, Dominic S. Wright, Clare P. Grey, Oleg Victor Kolosov, Zhigao Huang","doi":"10.1039/d5ee01076d","DOIUrl":"https://doi.org/10.1039/d5ee01076d","url":null,"abstract":"The interplay between solvent co-intercalation, solid-electrolyte interface (SEI) formation, and gas evolution at the graphite anode-electrolyte interface plays a critical role in battery performance, yet it remains poorly understood at the nanoscale. In this study, we introduce ultrasound-based operando atomic force microscopy (AFM), which breaks the spatial-resolution limitation of ultrasound-based techniques, to visualize the dynamics of solvent co-intercalation, SEI formation, and subsurface gas evolution in graphite anodes for lithium-ion batteries. Remarkably, we observe that gas evolution leads to the formation of “subsurface molecular bubbles”—gaseous pockets trapped between graphite layers—that compromise interfacial stability during battery formation cycles. AFM and Density Functional Theory calculations results revealed that these subsurface molecular bubbles are primarily induced by the co-intercalation and decomposition of Li+(EC)4 solvation complexes. We also found the solvent co-intercalation and interlayer decomposition effects can be fully suppressed by incorporating a low-permittivity, non-solvating diluent solvent (fluoride benzene) through optimizing the de-solvation energy and the interfacial molecular architectures. By applying this optimized electrolyte in both graphite/Li half-cells and lithium cobalt oxide (LCO)/graphite full-cells, we achieve stable cycling with negligible molecular bubble formation, compact SEI growth, and high coulombic efficiency (>93%) during high-rate (0.5 C) battery formation.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"6 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144684952","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}
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