{"title":"单原子活化多级活性位点,实现钠的彻底利用。","authors":"Shengyong Gao,Yibo Zhu,Ke Shi,Peng Liu,Yiming Zhang,Junping Hu,Zhenhai Wen,Lina Wang,Wen Tan,Lianzhou Wang,Bin Luo,Jisheng Zhou","doi":"10.1038/s41467-025-64351-9","DOIUrl":null,"url":null,"abstract":"Atomically dispersed metals offer advantages in guiding sodium deposition, yet the effects of single atoms on their surrounding structures and the precise tuning of coordination-governed single-atom activity remain underexplored. Herein, carbon nanofiber films with tin single atoms anchored via a dynamic coordination mode (shifting from coordination with three nitrogen atoms and one oxygen atom to coordination with one nitrogen atom and three oxygen atoms) are developed to address these challenges. The tin atoms not only enhance the sodium-ion adsorption activity of their directly coordinated nitrogen and oxygen atoms but also activate remote carbon atoms. The activation capability is strongly dependent on coordination environment, with tin atoms coordinated to more nitrogen atoms exhibiting higher activity. As a result, the optimized tin-carbon host enables uniform sodium deposition and complete stripping, allowing symmetric cells to cycle stably for 1200 h at 100 mA cm-2 and 100 mAh cm-2 with 100% depth of discharge. Anode-free full cells pairing the tin-carbon host with a sodium vanadate phosphate cathode achieve 94% capacity retention after 700 cycles at 10 C (6 min).","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"39 1","pages":"9269"},"PeriodicalIF":15.7000,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Single atom activated multi-stage active sites for thoroughgoing sodium utilization.\",\"authors\":\"Shengyong Gao,Yibo Zhu,Ke Shi,Peng Liu,Yiming Zhang,Junping Hu,Zhenhai Wen,Lina Wang,Wen Tan,Lianzhou Wang,Bin Luo,Jisheng Zhou\",\"doi\":\"10.1038/s41467-025-64351-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Atomically dispersed metals offer advantages in guiding sodium deposition, yet the effects of single atoms on their surrounding structures and the precise tuning of coordination-governed single-atom activity remain underexplored. Herein, carbon nanofiber films with tin single atoms anchored via a dynamic coordination mode (shifting from coordination with three nitrogen atoms and one oxygen atom to coordination with one nitrogen atom and three oxygen atoms) are developed to address these challenges. The tin atoms not only enhance the sodium-ion adsorption activity of their directly coordinated nitrogen and oxygen atoms but also activate remote carbon atoms. The activation capability is strongly dependent on coordination environment, with tin atoms coordinated to more nitrogen atoms exhibiting higher activity. As a result, the optimized tin-carbon host enables uniform sodium deposition and complete stripping, allowing symmetric cells to cycle stably for 1200 h at 100 mA cm-2 and 100 mAh cm-2 with 100% depth of discharge. Anode-free full cells pairing the tin-carbon host with a sodium vanadate phosphate cathode achieve 94% capacity retention after 700 cycles at 10 C (6 min).\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":\"39 1\",\"pages\":\"9269\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2025-10-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-025-64351-9\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-64351-9","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
摘要
原子分散的金属在引导钠沉积方面具有优势,但单原子对其周围结构的影响以及配位控制的单原子活性的精确调谐仍有待探索。为此,通过动态配位模式(从三个氮原子和一个氧原子的配位转变为一个氮原子和三个氧原子的配位),开发了锡单原子纳米纤维薄膜来解决这些挑战。锡原子不仅能增强其直接配位的氮、氧原子对钠离子的吸附活性,还能活化远端碳原子。其活化能力与配位环境密切相关,锡原子与氮原子配位越多,活性越高。因此,优化后的锡碳基质可以实现均匀的钠沉积和完全剥离,使对称电池在100 mA cm-2和100 mAh cm-2的放电深度下稳定循环1200小时。无阳极全电池将锡碳主体与钒酸钠磷酸盐阴极配对,在10℃(6分钟)下循环700次后,容量保持率达到94%。
Single atom activated multi-stage active sites for thoroughgoing sodium utilization.
Atomically dispersed metals offer advantages in guiding sodium deposition, yet the effects of single atoms on their surrounding structures and the precise tuning of coordination-governed single-atom activity remain underexplored. Herein, carbon nanofiber films with tin single atoms anchored via a dynamic coordination mode (shifting from coordination with three nitrogen atoms and one oxygen atom to coordination with one nitrogen atom and three oxygen atoms) are developed to address these challenges. The tin atoms not only enhance the sodium-ion adsorption activity of their directly coordinated nitrogen and oxygen atoms but also activate remote carbon atoms. The activation capability is strongly dependent on coordination environment, with tin atoms coordinated to more nitrogen atoms exhibiting higher activity. As a result, the optimized tin-carbon host enables uniform sodium deposition and complete stripping, allowing symmetric cells to cycle stably for 1200 h at 100 mA cm-2 and 100 mAh cm-2 with 100% depth of discharge. Anode-free full cells pairing the tin-carbon host with a sodium vanadate phosphate cathode achieve 94% capacity retention after 700 cycles at 10 C (6 min).
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.