Heng Zhang, Youcun Bai*, Wei Sun, Xiaogang Yang, Ruguang Ma, Liming Dai* and Chang Ming Li*,
{"title":"实现二硫化钼界面与双缺陷工程协同作用,实现高效钠离子存储","authors":"Heng Zhang, Youcun Bai*, Wei Sun, Xiaogang Yang, Ruguang Ma, Liming Dai* and Chang Ming Li*, ","doi":"10.1021/acsnano.4c1796710.1021/acsnano.4c17967","DOIUrl":null,"url":null,"abstract":"<p >Engineering-rich electrocatalyst defects play a critical role in greatly promoting the charge storage/transfer capability of an energy storage/conversion system. Here, an ingenious and effective two-step strategy was used to synthesize a bimetallic sulfide/oxide composite with a coaxial carbon coating, starting from mixing well-dispersed MoO<sub>3</sub> nanobelts and Co-PAA compound, followed by a selective etching process. The simultaneous formation of dual defects of interlayer defect and sulfur-rich vacancies as well as MoO<sub>2</sub>/MoS<sub>2-<i>x</i></sub>/CoS heterojunctions noticeably enhances both electron transfer and ion diffusion kinetics. The ultrathin carbon protective layer on the surface of the composite ensures its high conductivity and excellent structural stability. The composite electrode shows a high reversible capacity (158.3 mAh g<sup>–1</sup> at 10 A g<sup>–1</sup> after 4000 cycles) and outstanding long-cycle stability (0.04% per cycle over 2100 cycles at 20 A g<sup>–1</sup>). A full cell based on MoO<sub>2</sub>/MoS<sub>2–<i>x</i></sub>/CoS@N, S–C anode, and Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode can maintain a reversible capacity of 128.1 mAh g<sup>–1</sup> after 600 cycles at 1 A g<sup>–1</sup>, surpassing that based on MoO<sub>2</sub>/MoS<sub>2</sub> and is very comparable in performance with the state-of-the-art Na-ion full cells. Moreover, density functional theory (DFT) calculations, electrochemical kinetics analysis, and <i>in situ</i> Raman and <i>ex-situ</i> X-ray diffraction characterization were carried out to elucidate the involved scientific mechanisms of sodium storage.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"19 9","pages":"9081–9095 9081–9095"},"PeriodicalIF":16.0000,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Realizing the Synergy of Interface and Dual-Defect Engineering for Molybdenum Disulfide Enables Efficient Sodium-Ion Storage\",\"authors\":\"Heng Zhang, Youcun Bai*, Wei Sun, Xiaogang Yang, Ruguang Ma, Liming Dai* and Chang Ming Li*, \",\"doi\":\"10.1021/acsnano.4c1796710.1021/acsnano.4c17967\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Engineering-rich electrocatalyst defects play a critical role in greatly promoting the charge storage/transfer capability of an energy storage/conversion system. Here, an ingenious and effective two-step strategy was used to synthesize a bimetallic sulfide/oxide composite with a coaxial carbon coating, starting from mixing well-dispersed MoO<sub>3</sub> nanobelts and Co-PAA compound, followed by a selective etching process. The simultaneous formation of dual defects of interlayer defect and sulfur-rich vacancies as well as MoO<sub>2</sub>/MoS<sub>2-<i>x</i></sub>/CoS heterojunctions noticeably enhances both electron transfer and ion diffusion kinetics. The ultrathin carbon protective layer on the surface of the composite ensures its high conductivity and excellent structural stability. The composite electrode shows a high reversible capacity (158.3 mAh g<sup>–1</sup> at 10 A g<sup>–1</sup> after 4000 cycles) and outstanding long-cycle stability (0.04% per cycle over 2100 cycles at 20 A g<sup>–1</sup>). A full cell based on MoO<sub>2</sub>/MoS<sub>2–<i>x</i></sub>/CoS@N, S–C anode, and Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode can maintain a reversible capacity of 128.1 mAh g<sup>–1</sup> after 600 cycles at 1 A g<sup>–1</sup>, surpassing that based on MoO<sub>2</sub>/MoS<sub>2</sub> and is very comparable in performance with the state-of-the-art Na-ion full cells. Moreover, density functional theory (DFT) calculations, electrochemical kinetics analysis, and <i>in situ</i> Raman and <i>ex-situ</i> X-ray diffraction characterization were carried out to elucidate the involved scientific mechanisms of sodium storage.</p>\",\"PeriodicalId\":21,\"journal\":{\"name\":\"ACS Nano\",\"volume\":\"19 9\",\"pages\":\"9081–9095 9081–9095\"},\"PeriodicalIF\":16.0000,\"publicationDate\":\"2025-02-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Nano\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsnano.4c17967\",\"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}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Nano","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsnano.4c17967","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
摘要
工程性质丰富的电催化剂缺陷在极大地提高储能/转换系统的电荷存储/传输能力方面起着至关重要的作用。本文采用了一种巧妙而有效的两步法,从混合分散良好的MoO3纳米带和Co-PAA化合物开始,然后进行选择性蚀刻工艺,合成了具有同轴碳涂层的双金属硫化物/氧化物复合材料。层间缺陷和富硫空位的双重缺陷以及MoO2/MoS2-x/CoS异质结的同时形成显著提高了电子转移和离子扩散动力学。复合材料表面的超薄碳保护层保证了其高导电性和优异的结构稳定性。复合电极显示出高可逆容量(10a g-1, 4000次循环后158.3 mAh g-1)和出色的长周期稳定性(20a g-1, 2100次循环,每周期0.04%)。基于MoO2/MoS2 - x/CoS@N, S-C阳极和Na3V2(PO4)3阴极的全电池在1 A g-1下循环600次后可以保持128.1 mAh g-1的可逆容量,超过了基于MoO2/MoS2的电池,并且在性能上与最先进的钠离子全电池相当。此外,通过密度泛函理论(DFT)计算、电化学动力学分析、原位拉曼和非原位x射线衍射表征,阐明了钠储存的科学机制。
Realizing the Synergy of Interface and Dual-Defect Engineering for Molybdenum Disulfide Enables Efficient Sodium-Ion Storage
Engineering-rich electrocatalyst defects play a critical role in greatly promoting the charge storage/transfer capability of an energy storage/conversion system. Here, an ingenious and effective two-step strategy was used to synthesize a bimetallic sulfide/oxide composite with a coaxial carbon coating, starting from mixing well-dispersed MoO3 nanobelts and Co-PAA compound, followed by a selective etching process. The simultaneous formation of dual defects of interlayer defect and sulfur-rich vacancies as well as MoO2/MoS2-x/CoS heterojunctions noticeably enhances both electron transfer and ion diffusion kinetics. The ultrathin carbon protective layer on the surface of the composite ensures its high conductivity and excellent structural stability. The composite electrode shows a high reversible capacity (158.3 mAh g–1 at 10 A g–1 after 4000 cycles) and outstanding long-cycle stability (0.04% per cycle over 2100 cycles at 20 A g–1). A full cell based on MoO2/MoS2–x/CoS@N, S–C anode, and Na3V2(PO4)3 cathode can maintain a reversible capacity of 128.1 mAh g–1 after 600 cycles at 1 A g–1, surpassing that based on MoO2/MoS2 and is very comparable in performance with the state-of-the-art Na-ion full cells. Moreover, density functional theory (DFT) calculations, electrochemical kinetics analysis, and in situ Raman and ex-situ X-ray diffraction characterization were carried out to elucidate the involved scientific mechanisms of sodium storage.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.