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Room-temperature cylindrical lithium battery enabled by sulfide solid electrolyte tube 硫化物固体电解质管实现的室温圆柱形锂电池
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-20 DOI: 10.1016/j.ensm.2025.104338
Lei Zhu , Dengxu Wu , Chang Guo , Jian Peng , Zhiwen Jiang , Guangtao Ma , Chang Xu , Weitao He , Liquan Chen , Fan Wu
{"title":"Room-temperature cylindrical lithium battery enabled by sulfide solid electrolyte tube","authors":"Lei Zhu ,&nbsp;Dengxu Wu ,&nbsp;Chang Guo ,&nbsp;Jian Peng ,&nbsp;Zhiwen Jiang ,&nbsp;Guangtao Ma ,&nbsp;Chang Xu ,&nbsp;Weitao He ,&nbsp;Liquan Chen ,&nbsp;Fan Wu","doi":"10.1016/j.ensm.2025.104338","DOIUrl":"10.1016/j.ensm.2025.104338","url":null,"abstract":"<div><div>Cylindrical batteries have been explored as promising grid energy storage device, due to their high safety margin and low capital/maintenance costs. <em>However</em>, the practical application of cylindrical batteries is hindered by their high operational temperatures (above 240 °C). <em>Herein</em>, we report a sulfide-based cylindrical battery with a significantly reduced operating temperature of 30 °C, enabled by a sulfide solid electrolyte tube, a liquid lithium anode, and an in-situ polymerized gel layer. The battery demonstrates stable performance over a temperature range of 20–55 °C, maintaining 98 % of its capacity after 50 cycles at 30 °C and achieving 80 % energy efficiency. Additionally, the battery recovers stable electrochemical performance after freezing at -70 °C for 6 h. The symmetric battery also exhibits stable cycling for 500 h at 1 mA cm<sup>-</sup>², with a 33.01 % increase in critical current density to 4.07 mA cm<sup>-</sup>², attributed to optimized ceramic sintering that reduces grain boundaries. This work addresses a century-old challenge in cylindrical batteries by incorporating room-temperature superionic-conductivity sulfide electrolyte tubes, significantly lowering operating temperature, costs, and associated risks.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"79 ","pages":"Article 104338"},"PeriodicalIF":18.9,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097527","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
Interplays between TM migration, cation mixing and oxygen defects and their impacts on degradation of layer-structured oxide cathode materials TM迁移、阳离子混合和氧缺陷的相互作用及其对层状结构氧化物正极材料降解的影响
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-20 DOI: 10.1016/j.ensm.2025.104337
Shuwei Li , Yixin Li , Zhenjie Zhang , Xi Shen , Hongxiang Ji , Zepeng Liu , Zilin Hu , Haibo Wang , Hao Yu , Zhiwei Hu , Shu-Chih Haw , Chien-Te Chen , Qingyu Kong , Yurui Gao , Xuefeng Wang , Richeng Yu , Zhaoxiang Wang , Liquan Chen
{"title":"Interplays between TM migration, cation mixing and oxygen defects and their impacts on degradation of layer-structured oxide cathode materials","authors":"Shuwei Li ,&nbsp;Yixin Li ,&nbsp;Zhenjie Zhang ,&nbsp;Xi Shen ,&nbsp;Hongxiang Ji ,&nbsp;Zepeng Liu ,&nbsp;Zilin Hu ,&nbsp;Haibo Wang ,&nbsp;Hao Yu ,&nbsp;Zhiwei Hu ,&nbsp;Shu-Chih Haw ,&nbsp;Chien-Te Chen ,&nbsp;Qingyu Kong ,&nbsp;Yurui Gao ,&nbsp;Xuefeng Wang ,&nbsp;Richeng Yu ,&nbsp;Zhaoxiang Wang ,&nbsp;Liquan Chen","doi":"10.1016/j.ensm.2025.104337","DOIUrl":"10.1016/j.ensm.2025.104337","url":null,"abstract":"<div><div>The Li-rich and Ni-rich layer-structured transition metal (TM) oxide cathode materials have attracted extensive attention due to their high energy densities. However, they suffer from rapid structural and performance degradations due to TM migration and oxygen loss during cycling. Herein, the <span><math><mrow><mi>R</mi><mover><mn>3</mn><mo>¯</mo></mover><mi>m</mi></mrow></math></span> structured LiNiO<sub>2</sub> was investigated as a model of the layered oxides to reveal their structural features and structural degradation mechanisms. On the basis of comprehensive characterizations, we attributed the lowering of the TM oxidation potential to the deteriorated Li/TM cation mixing and the resultant change of the phase transition pathways. Notably, the cation mixing was found deteriorated even at a very low dosage of Li extraction and is enhanced with generation of extra oxygen vacancies at high potentials. Density functional theory (DFT) calculations explain the self-restriction of the Ni migration as well as these observations. Our findings clarify the mutual reinforcement between the TM migration, cation mixing and oxygen redox: the intrinsic and extrinsic Li/TM cation mixings result in the formation of Li-O-Li and/or Li-O-Vac<sub>TM</sub> configuration(s) (Vac<sub>TM</sub> for TM vacancy) and induce the oxygen oxidation, while the formation of oxygen vacancies further facilitate Ni migration by lowering its oxygen coordination. Clarification the relationship of TM migration, oxygen redox and structural degradation of LiNiO<sub>2</sub> and the Ni-rich materials provides a new insight for the development of other layer-structured oxide cathode materials.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"79 ","pages":"Article 104337"},"PeriodicalIF":18.9,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097530","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
Synergizing Catalytic Activity and Electronic Structure Adjustment by Dual-atomic Sites for High-Performance Lithium–sulfur Batteries 高性能锂硫电池双原子位的协同催化活性和电子结构调整
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-19 DOI: 10.1016/j.ensm.2025.104335
Longtao Ren, Chun-Wai Chang, Maoyu Wang, Abdul Hameed Pato, Zhenxing Feng, Hailiang Wang, Wen Liu
{"title":"Synergizing Catalytic Activity and Electronic Structure Adjustment by Dual-atomic Sites for High-Performance Lithium–sulfur Batteries","authors":"Longtao Ren, Chun-Wai Chang, Maoyu Wang, Abdul Hameed Pato, Zhenxing Feng, Hailiang Wang, Wen Liu","doi":"10.1016/j.ensm.2025.104335","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104335","url":null,"abstract":"The slow redox kinetics of lithium polysulfides (LiPSs) and the high energy barrier for Li<sub>2</sub>S deposition/dissociation are considered two significant challenges impeding the implementation of lithium–sulfur (Li–S) batteries. In this study, we have screened and successfully synthesized Fe-Cu and Co-Cu dual-atomic catalytic materials supported on reduced graphene oxide (rGO), which exhibits synergistic catalytic activity towards LiPSs and facilitates the adjustment of the electronic structure of Li<sub>2</sub>S. Consequently, the sulfur cathode with Fe-Cu dual-atomic catalyst sites exhibits remarkable electrochemical performance, including a high initial capacity of 1164 mAh g<sup>−1</sup> at 0.2 C, an exceptional rate capacity of 625.2 mAh g<sup>−1</sup> at 5 C, and excellent cycle stability with a low capacity fading rate of 0.045% per cycle over 500 cycles at 1 C. Notably, even with a high sulfur loading (8.5 mg cm<sup>−2</sup>) and a low E/S ratio (6 μL mg<sup>−1</sup>), an impressive initial capacity of 7.33 mAh cm<sup>−2</sup> is achieved. Furthermore, the Li–S pouch cell demonstrates a high discharge capacity of 5.5 mAh cm<sup>−2</sup> at 0.2 C, along with a capacity retention of 82% after 100 cycles. These results highlight the importance of elemental choice and synergy of dual-atomic catalytic materials in substantially propelling the sulfur redox kinetics in Li–S batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"87 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097529","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
Cascade effect of bioinspired slow-release protective layer enables stable Zn metal batteries 生物激发缓释保护层的级联效应使锌金属电池稳定
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-19 DOI: 10.1016/j.ensm.2025.104336
Zihan Liu , Yuliang Gao , Shifeng Huang , Yaodong Huo , Mengjing Li , Yanjiao Cao , Penghui Tian , Chenhui Han , Xiaojun Gu , Limin Wu
{"title":"Cascade effect of bioinspired slow-release protective layer enables stable Zn metal batteries","authors":"Zihan Liu ,&nbsp;Yuliang Gao ,&nbsp;Shifeng Huang ,&nbsp;Yaodong Huo ,&nbsp;Mengjing Li ,&nbsp;Yanjiao Cao ,&nbsp;Penghui Tian ,&nbsp;Chenhui Han ,&nbsp;Xiaojun Gu ,&nbsp;Limin Wu","doi":"10.1016/j.ensm.2025.104336","DOIUrl":"10.1016/j.ensm.2025.104336","url":null,"abstract":"<div><div>Aqueous Zn metal batteries have shown promise for large-scale energy storage systems, yet are constrained by cathodic metal ion dissolution and anodic dendrite growth. Herein, inspired by controlled drug delivery systems, we pioneer a bioinspired slow-release protective layer (SPL) on the Zn anode surface. The results indicate that SPL exhibits a unique cascade effect, which not only guides spherical Zn deposition through the solid-liquid biphasic structure and sustained <em>K</em><sup>+</sup>, but also innovatively extends protection to NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub> (NVO) model cathode via Cl<sup>−</sup>/<em>I</em><sup>−</sup>/DMSO co-release. For the cathode, these released species in situ generate a ZnS/ZnF<sub>2</sub>-rich cathode electrolyte interphase (CEI) by reconstructing the Zn<sup>2+</sup> solvation structure, effectively suppressing vanadium dissolution on the cathode side. Consequently, the capacity retention of the NVO||Zn pouch cell increases from 2.7 % to 65.3 % after 300 cycles and exhibits a low gassing behavior. This work provides a novel insight for the protective layer design and cathode protection.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"79 ","pages":"Article 104336"},"PeriodicalIF":18.9,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097652","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
Improving intrinsic safety of Ni-rich layered oxide cathode by modulating its electronic surface state 通过调节富镍层状氧化物阴极的电子表面态来提高其本质安全性
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-18 DOI: 10.1016/j.ensm.2025.104332
Jiaoyang Cheng , Xiaoli Ma , Xiaoman Sun , Fang Lian , Xiang Liu , Languang Lu , Dingguo Xia
{"title":"Improving intrinsic safety of Ni-rich layered oxide cathode by modulating its electronic surface state","authors":"Jiaoyang Cheng ,&nbsp;Xiaoli Ma ,&nbsp;Xiaoman Sun ,&nbsp;Fang Lian ,&nbsp;Xiang Liu ,&nbsp;Languang Lu ,&nbsp;Dingguo Xia","doi":"10.1016/j.ensm.2025.104332","DOIUrl":"10.1016/j.ensm.2025.104332","url":null,"abstract":"<div><div>Safety risks and severe capacity degradation at elevated temperature of Ni-rich layered oxides hamper their application in power batteries for electric vehicles. In this work, the polymethacrylate-<em>N</em>-dibenzenesulfonimide ester (PM-NDIE) is proposed to penetrate into the interstices of primary particles of LiNi<sub>0.85</sub>Co<sub>0.1</sub>Mn<sub>0.05</sub>O<sub>2</sub>. During in-situ polymerization, nucleophilic oxygen and electrophilic sulfur atoms chemically bond with undercoordinated Ni and oxygen on the surface, respectively, modulating the electronic surface state. The <em>in-situ</em> XRD/XAFS/TEM analyses and DFT calculations corroborate that PM-NDIE contributes to slowing down the covalency increase of TM-O bond and preserving atomic coordination integrity even under highly delithiated state, thereby maintaining the integral layered structure during cycling. NCM with the PM-NDIE-engineered surface (P-NCM) demonstrates a distinct thinner inorganics-dominant cathode/electrolyte interphase and enables exceptional interfacial stability. P-NCM delivers a 47 % reduction in voltage decay in self-discharge test at 55 °C, a 27.4 % improvement in capacity retention over 100 cycles at 1C/55 °C, and maintains 93.66 % capacity after 400 cycles under 1C in Ah-level pouch-cell. Moreover, a significantly inhibited thermal-induced phase transition and a delayed thermal runaway critical temperature of pouch-cells provide further evidence that a major driving force for heat-/oxygen- release spontaneous reaction of NCM has been cut off by stabilizing its electronic surface state.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"79 ","pages":"Article 104332"},"PeriodicalIF":18.9,"publicationDate":"2025-05-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144083400","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
Corrigendum to ’Dynamic Iron Migration Triggers Single-to-Dual Electron Redox Conversion in Hexacyanoferrates for Stable Aqueous Potassium Ion Batteries’,Energy Storage Materials 79 (2025) 104296 “动态铁迁移触发Hexacyanoferrates中单到双电子氧化还原转换,用于稳定的钾离子电池”,储能材料79(2025)104296的更正
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-17 DOI: 10.1016/j.ensm.2025.104331
Usman Ali, Maoyu Sun, Muhammad Sajid, Zeeshan Ali, Talal Ahmad, Yuehan Hao, Fuping Min, Lu Li, Chungang Wang, Bingqiu Liu
{"title":"Corrigendum to ’Dynamic Iron Migration Triggers Single-to-Dual Electron Redox Conversion in Hexacyanoferrates for Stable Aqueous Potassium Ion Batteries’,Energy Storage Materials 79 (2025) 104296","authors":"Usman Ali, Maoyu Sun, Muhammad Sajid, Zeeshan Ali, Talal Ahmad, Yuehan Hao, Fuping Min, Lu Li, Chungang Wang, Bingqiu Liu","doi":"10.1016/j.ensm.2025.104331","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104331","url":null,"abstract":"The authors regret The authors regret that there was an error in the author list of the original article. The correct author’s name should read as “[<strong>Usman Ali, Muhammad Sajid, Zeeshan Ali, Talal Ahmad</strong>]” instead of “[<strong>Ali Usman, Sajid Muhammad, Ali Zeeshan, Ahmad Talal</strong>].” The authors apologize for this oversight and any inconvenience it may have caused.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"29 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144067464","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
Nitrile-based solid polymer electrolytes for novel energy storage systems: A perspective from ion transport mechanism to applications in solid-state batteries 用于新型储能系统的腈基固体聚合物电解质:从离子传输机制到固态电池应用的视角
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-17 DOI: 10.1016/j.ensm.2025.104317
Rui Yan , Keyu Zhang , Binbin Li , Feng Liang , Shaoze Zhang , Bin Yang , Yaochun Yao , Yong Lei
{"title":"Nitrile-based solid polymer electrolytes for novel energy storage systems: A perspective from ion transport mechanism to applications in solid-state batteries","authors":"Rui Yan ,&nbsp;Keyu Zhang ,&nbsp;Binbin Li ,&nbsp;Feng Liang ,&nbsp;Shaoze Zhang ,&nbsp;Bin Yang ,&nbsp;Yaochun Yao ,&nbsp;Yong Lei","doi":"10.1016/j.ensm.2025.104317","DOIUrl":"10.1016/j.ensm.2025.104317","url":null,"abstract":"<div><div>Considering several challenges for traditional liquid batteries and liquid electrolytes, solid-state batteries (SSBs) and solid-state electrolytes (SSEs) offer a means to significantly improve the safety and energy density of energy storage devices. The utilization of SSEs in lithium metal batteries (LMBs) is widely recognized as a crucial step in designing next-generation high-performance energy storage devices. Nitrile-based solid polymer electrolytes (SPEs), exemplified by polyacrylonitrile (PAN), have gained prominence due to its exceptional mechanical strength, effective lithium salt dissociation capabilities and excellent interfacial contact. Exploration and modification of intrinsic active functional groups of polymers are emerging as pivotal strategies for advanced SSBs, simultaneously providing a foundational framework for analyzing the intricate relationship between microscopic mechanisms and macroscopic performance. This review initially focuses on the dissociation-coupling of ion behavior, kinetics, and various types of nitrile-based polymers. Specifically, focusing on the advantages of nitrile-containing functional groups, the key limiting factors and empirical formula ions transport in SSEs and are summarized. In addition, a brief introduction of numerous achievements related to the diverse applications of nitrile-based organic compounds in SSEs and electrolyte additives with a detailed exposition of current mainstream modification strategies are highlighted, designed to provide direction for optimization and development of nitrile-based SPEs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"79 ","pages":"Article 104317"},"PeriodicalIF":18.9,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144067463","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
Corrigendum to `Anionic flip induced gating effect enables high stability of zinc metal anode’ < [Energy Storage Materials Anionic flip induced gating effect enables high stability of zinc metal anode 79 (2025) 104035 /ENSM-D-25-01092]> “阴离子翻转诱导门效应使锌金属阳极具有高稳定性”的勘误表<[储能材料]阴离子翻转诱导门效应使锌金属阳极具有高稳定性79 (2025)104035 /ENSM-D-25-01092]>
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-16 DOI: 10.1016/j.ensm.2025.104329
Qiwen Zhao, Yesong Chen, Wen Liu, Changding Wang, Hanwei He, Bingang Xu, Gang Zhou, Yuejiao Chen, Libao Chen
{"title":"Corrigendum to `Anionic flip induced gating effect enables high stability of zinc metal anode’ < [Energy Storage Materials Anionic flip induced gating effect enables high stability of zinc metal anode 79 (2025) 104035 /ENSM-D-25-01092]>","authors":"Qiwen Zhao, Yesong Chen, Wen Liu, Changding Wang, Hanwei He, Bingang Xu, Gang Zhou, Yuejiao Chen, Libao Chen","doi":"10.1016/j.ensm.2025.104329","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104329","url":null,"abstract":"The authors regret the while the affiliations in our originally submitted manuscript were correct, current online publication erroneously shows second and third authors (<strong>Yesong Chen, Wen Liu</strong>) institutional affiliations as ''National Energy Metal Resources and New Materials Key Laboratory''. The correct affiliations should be ''State Key Laboratory of Powder Metallurgy, Central South University, Changsha, 410083, P. R. China'', as provided in our initial submission. We deeply regret this oversight occurred during the proofreading process due to an inadvertent error on our part.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"30 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066330","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
Molecular crowding effect synergies ice breaking: A Cryogenic revival prescription for aqueous Zn-ion batteries 分子拥挤效应协同破冰:水溶液锌离子电池的低温再生配方
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-15 DOI: 10.1016/j.ensm.2025.104326
Xinwen Rao , Yuying Han , Liang Luo , Linfang Hu , Lijin Yan , Bin Xiang , Yang Zhou , Xuefeng Zou
{"title":"Molecular crowding effect synergies ice breaking: A Cryogenic revival prescription for aqueous Zn-ion batteries","authors":"Xinwen Rao ,&nbsp;Yuying Han ,&nbsp;Liang Luo ,&nbsp;Linfang Hu ,&nbsp;Lijin Yan ,&nbsp;Bin Xiang ,&nbsp;Yang Zhou ,&nbsp;Xuefeng Zou","doi":"10.1016/j.ensm.2025.104326","DOIUrl":"10.1016/j.ensm.2025.104326","url":null,"abstract":"<div><div>Aqueous Zn-ion batteries have been widely concerned for their high ionic conductivity and intrinsic safety. However, solvated water easily induces HER to deteriorate Zn anode interface and has poor performance at low temperatures. Here, formamide (FA) and D-xylose (DX) synergically induce a molecular crowding effect that increases Zn<sup>2+</sup> kinetics and decreases the freezing point. FA as a ‘chain’ is mainly used to regulate the solvation structure of Zn<sup>2+</sup> and DX as a ‘bridge’ is mainly used to destroy the hydrogen bond network of water. Therefore, the multiple Zn<sup>2+</sup> solvation configurations present in FD can effectively inhibit the side reactions and reduce its freezing point to -51 °C. The Zn∣∣Zn battery can operate for more than 3000 h at -35 °C (0.5 mA cm<sup>-2</sup>). The average CE of Zn∣∣Cu battery after 3000 cycles is close to 100 %. The capacity retention rate of Zn∣∣PANI battery is 80 % after 3000 cycles at 30 °C (3 A g<sup>-1</sup>) and 91 % after 750 cycles at -35 °C (0.1 A g<sup>-1</sup>). This study provides a three-in-one modification strategy of ‘solvation structure - deposition kinetics - interface stability’ and provides practical insights for the application of AZIBs at extremely low temperatures.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"79 ","pages":"Article 104326"},"PeriodicalIF":18.9,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143979869","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
Fast charge transfer of single metal atom coordinating p-phenylenediamine covalently pillared graphene cathode for high-rate lithium-ion capacitors 高倍率锂离子电容器单金属配位对苯二胺共价柱撑石墨烯阴极的快速电荷转移
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-05-15 DOI: 10.1016/j.ensm.2025.104328
Ziqin Xu , Guomeng Xie , Delai Qian , Ruiwu Li , Haitao Fang , Zhengjia Wang
{"title":"Fast charge transfer of single metal atom coordinating p-phenylenediamine covalently pillared graphene cathode for high-rate lithium-ion capacitors","authors":"Ziqin Xu ,&nbsp;Guomeng Xie ,&nbsp;Delai Qian ,&nbsp;Ruiwu Li ,&nbsp;Haitao Fang ,&nbsp;Zhengjia Wang","doi":"10.1016/j.ensm.2025.104328","DOIUrl":"10.1016/j.ensm.2025.104328","url":null,"abstract":"<div><div>P-type redox-active organic molecules (ROMs) exhibit higher redox potentials due to deeper highest occupied molecular orbital (HOMO) energy level, but the inherent higher charge transfer energy barrier limits their rate performance, which cannot be overcome by simply hybridizing with carbon materials (CMs). Herein, Co single atoms (SAs) are introduced into <em>p</em>-phenylenediamine (pPD) pillared graphene (rGO-pPD-Co), aiming to leverage their catalytic effect on the pseudocapacitive charge transfer process. Experimental results and density functional theory (DFT) calculations reveal that Co SAs alter the local charge distribution, activating their redox activity toward <span><math><msubsup><mtext>PF</mtext><mrow><mn>6</mn></mrow><mo>−</mo></msubsup></math></span> adsorption. Their electron-donating property disrupts the conjugation and elevates the Fermi level of rGO-pPD-Co, thus reducing the energy barrier for electron transfer. Additionally, the more positive electrostatic potential (ESP) of Co SAs coordination increases the affinity with <span><math><msubsup><mtext>PF</mtext><mrow><mn>6</mn></mrow><mo>−</mo></msubsup></math></span> anion, lowering the total Gibbs free energy change for the redox reaction of rGO-pPD-Co. Although exhibiting slightly reduced redox potentials, the catalytically accelerated rGO-pPD-Co cathode achieves excellent rate performance (128 mAh g<sup>-1</sup> at 20 A g<sup>-1</sup>). This work demonstrates the catalytic effect of coordinated single-atom metals (SAMs) on the charge transfer of p-type groups, providing a novel strategy to accelerate pseudocapacitive reaction kinetics and boost the rate capability of p-type ROMs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"79 ","pages":"Article 104328"},"PeriodicalIF":18.9,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066067","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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