Ziming Su, Xiangyu Chen, Mingke Sun, Xiuyi Yang, Jianxin Kang, Zhi Cai, Lin Guo
{"title":"用于高效电催化氨生产的非晶纳米颗粒。","authors":"Ziming Su, Xiangyu Chen, Mingke Sun, Xiuyi Yang, Jianxin Kang, Zhi Cai, Lin Guo","doi":"10.1002/anie.202416878","DOIUrl":null,"url":null,"abstract":"<p><p>One-dimensional (1D) amorphous nanomaterials combine the advantages of high active site concentration of amorphous structure, high specific surface area and efficient charge transfer of 1D materials, so they present promising opportunities for catalysis. However, how to achievie the balance between the high orientation of 1D morphology and the isotropy of amorphous structure is a significant challenge, which severely obstructs the controllable preparation of 1D amorphous materials. Guided by the hard-soft acids-bases theory, here we develop a general strategy for preparing 1D amorphous nanomaterials through the precise modulation of bond strength between metal ions and organic ligands for a moderated fastness. The soft base dodecanethiol (DT) is multifunctionally served as both structure-regulating agent and morphology-directing agent. Compared with the borderline acids (e.g. Fe<sup>2+</sup>, Co<sup>2+</sup>, Ni<sup>2+</sup>) to construct amorphous structure, soft acid of Cu<sup>+</sup> which produced crystalline nanobelts can still be amorphized by reducing the hardness of Cu ions through redox reaction to weak Cu-SR bond. Due to the combined advantages of amorphous structure and one-dimensional morphology, amorphous CuDT nanobelts exhibited excellent electrocatalytic activity in electrochemical nitrate reduction, outperformed most of the reported Cu-based catalysts. This work will effectively bridge the gap between traditional 1D crystalline nanomaterials synthesis and their amorphization preparation.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416878"},"PeriodicalIF":16.1000,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Amorphous Nanobelts for Efficient Electrocatalytic Ammonia Production.\",\"authors\":\"Ziming Su, Xiangyu Chen, Mingke Sun, Xiuyi Yang, Jianxin Kang, Zhi Cai, Lin Guo\",\"doi\":\"10.1002/anie.202416878\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>One-dimensional (1D) amorphous nanomaterials combine the advantages of high active site concentration of amorphous structure, high specific surface area and efficient charge transfer of 1D materials, so they present promising opportunities for catalysis. However, how to achievie the balance between the high orientation of 1D morphology and the isotropy of amorphous structure is a significant challenge, which severely obstructs the controllable preparation of 1D amorphous materials. Guided by the hard-soft acids-bases theory, here we develop a general strategy for preparing 1D amorphous nanomaterials through the precise modulation of bond strength between metal ions and organic ligands for a moderated fastness. The soft base dodecanethiol (DT) is multifunctionally served as both structure-regulating agent and morphology-directing agent. Compared with the borderline acids (e.g. Fe<sup>2+</sup>, Co<sup>2+</sup>, Ni<sup>2+</sup>) to construct amorphous structure, soft acid of Cu<sup>+</sup> which produced crystalline nanobelts can still be amorphized by reducing the hardness of Cu ions through redox reaction to weak Cu-SR bond. Due to the combined advantages of amorphous structure and one-dimensional morphology, amorphous CuDT nanobelts exhibited excellent electrocatalytic activity in electrochemical nitrate reduction, outperformed most of the reported Cu-based catalysts. This work will effectively bridge the gap between traditional 1D crystalline nanomaterials synthesis and their amorphization preparation.</p>\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":\" \",\"pages\":\"e202416878\"},\"PeriodicalIF\":16.1000,\"publicationDate\":\"2025-01-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie International Edition\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202416878\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/11/6 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202416878","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/11/6 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
一维(1D)非晶纳米材料兼具非晶结构的高活性位点浓度、高比表面积以及一维材料的高效电荷转移和质量传输等优点,因此在催化领域大有可为。然而,如何在一维形态的高取向性和非晶结构的各向同性之间实现平衡是一个重大挑战,这严重阻碍了一维非晶材料的可控制备。在软硬酸碱理论的指导下,我们通过精确调节金属离子与有机配体之间的结合强度,开发出了一种制备一维非晶纳米材料的通用策略,以达到适度的牢度。软基十二硫醇(DT)兼具结构调节剂和形态引导剂的多重功能。与边界酸(如 Fe2+、Co2+、Ni2+)构建非晶态结构相比,产生结晶纳米颗粒的 Cu+ 软酸仍可通过氧化还原反应降低 Cu 离子的硬度,使 Cu-SR 键变弱,从而实现非晶化。由于非晶态结构和一维形貌的综合优势,非晶态 CuDT 纳米颗粒在电化学硝酸盐还原中表现出优异的电催化活性,优于大多数已报道的铜基催化剂。这项工作将有效弥补传统一维晶体纳米材料与非晶态制备之间的差距。
Amorphous Nanobelts for Efficient Electrocatalytic Ammonia Production.
One-dimensional (1D) amorphous nanomaterials combine the advantages of high active site concentration of amorphous structure, high specific surface area and efficient charge transfer of 1D materials, so they present promising opportunities for catalysis. However, how to achievie the balance between the high orientation of 1D morphology and the isotropy of amorphous structure is a significant challenge, which severely obstructs the controllable preparation of 1D amorphous materials. Guided by the hard-soft acids-bases theory, here we develop a general strategy for preparing 1D amorphous nanomaterials through the precise modulation of bond strength between metal ions and organic ligands for a moderated fastness. The soft base dodecanethiol (DT) is multifunctionally served as both structure-regulating agent and morphology-directing agent. Compared with the borderline acids (e.g. Fe2+, Co2+, Ni2+) to construct amorphous structure, soft acid of Cu+ which produced crystalline nanobelts can still be amorphized by reducing the hardness of Cu ions through redox reaction to weak Cu-SR bond. Due to the combined advantages of amorphous structure and one-dimensional morphology, amorphous CuDT nanobelts exhibited excellent electrocatalytic activity in electrochemical nitrate reduction, outperformed most of the reported Cu-based catalysts. This work will effectively bridge the gap between traditional 1D crystalline nanomaterials synthesis and their amorphization preparation.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.