中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
首页 机构 成果 学者
  
  1. CAS IR Grid
  2. 合肥物质科学研究院
  3. 中国科学院合肥物质科学研究院
Introducing Novel, Multiple Cd Coordination Modes into Gold Nanoclusters by Combined Doping for Enhancing Electrocatalytic Performance

文献类型：期刊论文

作者Liu, Zhen3,4,5; Meng, Xiangfu1,2; Gu, Wanmiao3,5; Zha, Jun3,4,5; Yan, Nan3,5; You, Qing3,5; Xia, Nan3,5; Wang, Hui1,2; Wu, Zhikun3,5
刊名ACTA PHYSICO-CHIMICA SINICA
出版日期2023-07-31
卷号39
关键词Metal Nanocluster Combined doping Cd-coordination mode Structure-property correlation Electrocatalytic reduction of CO2
ISSN号1000-6818
DOI10.3866/PKU.WHXB202212064
通讯作者Wang, Hui(hw39@hmfl.ac.cn) ; Wu, Zhikun(zkwu@issp.ac.cn)
英文摘要In recent years, gold nanoclusters have been widely used in catalysis, and alloying has become one of the most important methods for improving the catalytic performance of gold nanoclusters. As for the electrocatalytic reduction of CO2 (CO2RR), although many gold nanoclusters show fairly good Faraday efficiencies through Cd-doping, they still exhibit low current density. Furthermore, as an increasing number of Au-Cd alloy nanoclusters are reported, there is a growing interest in understanding the correlation between Cd coordination and catalysis performance. In most cases, Cd atoms are typically doped in the outer staples and connect with Au atoms through S coordinations. Are there any other unreported Cd coordination modes? Can novel or numerous Cd coordination modes be introduced into gold nanoclusters to increase the current density in the CO2RR? This study investigates these questions.Inspired by our previous work on surface sulfur doping, we employed a combined doping (S + Cd doping) strategy, developed a two-step synthesis method, and successfully synthesized a novel Au-Cd nanocluster-Au41Cd6S2(SCH2Ph)33. Precise formula and structure were determined by electrospray ionization mass spectrometry (ESI-MS), thermalgravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS), and single-crystal X-ray crystallography (SCXC). SCXC shows that the nanocluster contains a biicosahedral Au23 kernel, and all the Cd atoms are doped in the outer staples, providing a variety of coordination environments for Cd atoms. In addition to two common Au3(SR)4 trimers in the outer staples, two unusual Au5Cd2(SR)9S long staples were discovered cross-covering the top of the kernel, and a (S-Au-S)2(CdS-S-CdS) tetramer staple with two Cd atoms directly linked through S was also discovered for the first time. This alloy cluster shows robust stability in both high-temperature and oxidation environments. Compared with the "homo-kernel-hetero-staples" nanocluster Au38(SCH2Ph)24, Au41Cd6S2(SCH2Ph)33 exhibits distinct UV-Vis/NIR absorption and differential pulse voltammetry (DPV) results, indicating that the differences in the outer staples have a significant effect on the optical and electronic properties of gold nanoclusters. When used as an electrocatalyst, the Au41Cd6S2(SCH2Ph)33 exhibits a higher Faradaic efficiency for the CO2RR (99.3% at -0.7 V) and a higher CO partial current density (120 mA & BULL;cm-2 at -0.9 V) than Au38(SCH2Ph)24, providing an ideal platform for investigating the roles of different Cd coordination modes in outer staples on CO2RR. DFT calculations interpret the experimental finding that Cd doping improves the catalytic performance and reveal that the Cd-Cd site is the most active site and the Au-Cd site furthest away from the kernel is the best-performing catalytic site given the consideration of both selectivity and activity.This work introduces a novel strategy to enhance the catalytic performance of gold nanoclusters, having important implications for future research on the syntheses and structural properties of metal nanoclusters, and is expected to inspire more work in related areas.
WOS关键词TOTAL-ENERGY CALCULATIONS ; CATALYSIS ; SURFACE
资助项目National Natural Science Foundation of China[21829501] ; National Natural Science Foundation of China[21925303] ; National Natural Science Foundation of China[22171267] ; National Natural Science Foundation of China[22171268] ; National Natural Science Foundation of China[21771186] ; National Natural Science Foundation of China[21222301] ; National Natural Science Foundation of China[21171170] ; National Natural Science Foundation of China[21528303] ; Anhui Provincial Natural Science Foundation[2008085MB31] ; Anhui Provincial Natural Science Foundation[2108085MB56] ; CASHIPS Director's Fund[BJPY2019A02] ; Collaborative Innovation Program of Hefei Science Center, CAS[2020HSC-CIP005] ; Collaborative Innovation Program of Hefei Science Center, CAS[2022HSC-CIP018]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001071574900002
出版者PEKING UNIV PRESS
资助机构National Natural Science Foundation of China ; Anhui Provincial Natural Science Foundation ; CASHIPS Director's Fund ; Collaborative Innovation Program of Hefei Science Center, CAS
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/132603]  
专题中国科学院合肥物质科学研究院
通讯作者Wang, Hui; Wu, Zhikun
作者单位1.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
2.Chinese Acad Sci, Hefei Inst Phys Sci, High Magnet Field Lab, Hefei 230031, Peoples R China
3.Anhui Univ, Inst Phys Sci & Informat Technol, Hefei 230601, Peoples R China
4.Univ Sci & Technol China, Sci Isl Branch, Grad Sch, Hefei 230026, Peoples R China
5.Chinese Acad Sci, Inst Solid State Phys, Anhui Key Lab Nanomat & Nanotechnol, CAS Ctr Excellence Nanosci,Key Lab Mat Phys,Hefei, Hefei 230031, Peoples R China
推荐引用方式
GB/T 7714		 Liu, Zhen,Meng, Xiangfu,Gu, Wanmiao,et al. Introducing Novel, Multiple Cd Coordination Modes into Gold Nanoclusters by Combined Doping for Enhancing Electrocatalytic Performance[J]. ACTA PHYSICO-CHIMICA SINICA,2023,39.
APA Liu, Zhen.,Meng, Xiangfu.,Gu, Wanmiao.,Zha, Jun.,Yan, Nan.,...&Wu, Zhikun.(2023).Introducing Novel, Multiple Cd Coordination Modes into Gold Nanoclusters by Combined Doping for Enhancing Electrocatalytic Performance.ACTA PHYSICO-CHIMICA SINICA,39.
MLA Liu, Zhen,et al."Introducing Novel, Multiple Cd Coordination Modes into Gold Nanoclusters by Combined Doping for Enhancing Electrocatalytic Performance".ACTA PHYSICO-CHIMICA SINICA 39(2023).

入库方式： OAI收割

来源：合肥物质科学研究院

浏览0
下载0
收藏0
其他版本

除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。