{"title":"Revealing Capacitive Slope Capacity of Open Pore Carbon for Ultrahigh-Rate Sodium-Ion Storage.","authors":"Sicheng Fan,Zerui Yan,Dafu Tang,Yuting Song,Jie Lin,Guiming Zhong,Dong-Liang Peng,Qiulong Wei","doi":"10.1002/adma.202513223","DOIUrl":null,"url":null,"abstract":"Disordered carbon materials exhibit slope and plateau Na+ storage capacities. Compared with the well-investigated plateau capacities from the intercalation/filling mechanism, the \"capacitive\" slope storage remains relatively unidentified. Herein, the effects of open pore sizes and solid electrolyte interface (SEI) layers are investigated on slope capacity and thus categorize the \"capacitive\" behaviors into three distinct scenarios. Conventionally, the complete desolvation and pseudocapacitive Na+ slope capacities arise from the sieving of ethylene carbonate (EC)-SEI layers. Differently, an electric double-layer (EDL) capacitive adsorption of partially desolvated Na+ ions is revealed in large open pores of 0.5-2 nm in the diethylene glycol dimethyl ether (DGDE) electrolyte in a large potential window of 3-0.01 V vs Na+/Na. Remarkably, DGDE-SEI does not block open pores or sieve solvation shells, resulting in an exceptionally high initial coulombic efficiency of 92.4% and ultrahigh-rate capabilities. When the open pore size decreases to <0.5 nm (accessible to CO2 but inaccessible to Ar) or becomes closed pores in DGDE electrolyte, the narrow pores themselves sieve solvation shells and subsequent pseudocapacitive Na+ storage for slope capacity. The EDL capacitive slope capacity of open porous carbon highlights the ultrafast (dis)charging abilities and stable cycles, which are highly promising for high-power sodium-ion storage devices.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"62 1","pages":"e13223"},"PeriodicalIF":26.8000,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.202513223","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Disordered carbon materials exhibit slope and plateau Na+ storage capacities. Compared with the well-investigated plateau capacities from the intercalation/filling mechanism, the "capacitive" slope storage remains relatively unidentified. Herein, the effects of open pore sizes and solid electrolyte interface (SEI) layers are investigated on slope capacity and thus categorize the "capacitive" behaviors into three distinct scenarios. Conventionally, the complete desolvation and pseudocapacitive Na+ slope capacities arise from the sieving of ethylene carbonate (EC)-SEI layers. Differently, an electric double-layer (EDL) capacitive adsorption of partially desolvated Na+ ions is revealed in large open pores of 0.5-2 nm in the diethylene glycol dimethyl ether (DGDE) electrolyte in a large potential window of 3-0.01 V vs Na+/Na. Remarkably, DGDE-SEI does not block open pores or sieve solvation shells, resulting in an exceptionally high initial coulombic efficiency of 92.4% and ultrahigh-rate capabilities. When the open pore size decreases to <0.5 nm (accessible to CO2 but inaccessible to Ar) or becomes closed pores in DGDE electrolyte, the narrow pores themselves sieve solvation shells and subsequent pseudocapacitive Na+ storage for slope capacity. The EDL capacitive slope capacity of open porous carbon highlights the ultrafast (dis)charging abilities and stable cycles, which are highly promising for high-power sodium-ion storage devices.
无序碳材料表现出斜坡式和高原式的Na+储存能力。与已得到充分研究的嵌入/填充机制的高原容量相比,“电容式”斜坡蓄能仍相对不明。本文研究了开放孔径和固体电解质界面(SEI)层对斜坡容量的影响,并将“电容”行为分为三种不同的情况。通常,完全脱溶和假电容性Na+斜率容量来自于乙烯碳酸酯(EC)-SEI层的筛分。在3-0.01 V vs Na+/Na的大电位窗口中,二甘醇二甲醚(DGDE)电解质在0.5-2 nm的大开孔中对部分脱溶的Na+离子进行了双电层(EDL)电容吸附。值得注意的是,DGDE-SEI不会堵塞开放的孔隙或过滤溶剂化壳,因此具有92.4%的超高初始库仑效率和超高速率能力。在DGDE电解质中,当开放孔径减小到<0.5 nm (CO2可达,Ar不可达)或成为封闭孔时,狭窄的孔本身会过滤溶剂化壳和随后的假电容性Na+存储以获得斜率容量。开放多孔碳的EDL电容斜率容量突出了其超快(非)充电能力和稳定的循环,在大功率钠离子存储器件中具有很大的应用前景。
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.