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Single-Atom Catalysts through Pressure-Controlled Metal Diffusion

文献类型：期刊论文

作者AlHilfi, Samir H5,6; Jiang XK(蒋玺恺)4; Heuer, Julian5; Akula, Srinu3; Tammeveski, Kaido3; Hu, Guoqing2; Yang, Juan6; Wang, Hai I1,5; Bonn, Mischa5; Landfester, Katharina5
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
出版日期2024-07-11
卷号146期号:29页码:19886-19895
ISSN号0002-7863
DOI10.1021/jacs.4c03066
通讯作者Bonn, Mischa(bonn@mpip-mainz.mpg.de) ; Muellen, Klaus() ; Zhou, Yazhou(yazhou@ujs.edu.cn)
英文摘要Single-atom catalysts (SACs) open up new possibilities for advanced technologies. However, a major complication in preparing high-density single-atom sites is the aggregation of single atoms into clusters. This complication stems from the delicate balance between the diffusion and stabilization of metal atoms during pyrolysis. Here, we present pressure-controlled metal diffusion as a new concept for fabricating ultra-high-density SACs. Reducing the pressure inhibits aggregation substantially, resulting in almost three times higher single-atom loadings than those obtained at ambient pressure. Molecular dynamics and computational fluid dynamics simulations reveal the role of a metal hopping mechanism, maximizing the metal atom distribution through an increased probability of metal-ligand binding. The investigation of the active site density by electrocatalytic oxygen reduction validates the robustness of our approach. The first realization of Ullmann-type carbon-oxygen couplings catalyzed on single Cu sites demonstrates further options for efficient heterogeneous catalysis.
分类号一类
WOS关键词ARYL HALIDES ; IDENTIFICATION ; COMPLEXES ; AMINATION ; EFFICIENT ; SITES
资助项目Natural Science Foundation of China[51702129] ; Natural Science Foundation of China[51972150] ; DFG[514772236] ; Estonian Research Council[PRG723] ; EU through the European Regional Development Fund[MOBJD671] ; EU through the European Regional Development Fund[TK141]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001266684200001
资助机构Natural Science Foundation of China ; DFG ; Estonian Research Council ; EU through the European Regional Development Fund
其他责任者Bonn, Mischa ; Muellen, Klaus ; Zhou, Yazhou
源URL[http://dspace.imech.ac.cn/handle/311007/95977]  
专题力学研究所_非线性力学国家重点实验室
作者单位1.Univ Utrecht, Debye Inst Nanomat Sci, Nanophoton, NL-3584 CC Utrecht, Netherlands
2.Zhejiang Univ, Dept Engn Mech, State Key Lab Fluid Power & Mechatron Syst, Hangzhou 310027, Zhejiang, Peoples R China;
3.Univ Tartu, Inst Chem, EE-50411 Tartu, Estonia;
4.Chinese Acad Sci, Inst Mech, State Key Lab Nonlinear Mech, Beijing 100190, Peoples R China;
5.Max Planck Inst Polymer Res, D-55128 Mainz, Germany;
6.Jiangsu Univ, Sch Mat Sci & Engn, Zhenjiang 212013, Jiangsu, Peoples R China;
推荐引用方式
GB/T 7714		 AlHilfi, Samir H,Jiang XK,Heuer, Julian,et al. Single-Atom Catalysts through Pressure-Controlled Metal Diffusion[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146(29):19886-19895.
APA AlHilfi, Samir H.,蒋玺恺.,Heuer, Julian.,Akula, Srinu.,Tammeveski, Kaido.,...&Zhou, Yazhou.(2024).Single-Atom Catalysts through Pressure-Controlled Metal Diffusion.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(29),19886-19895.
MLA AlHilfi, Samir H,et al."Single-Atom Catalysts through Pressure-Controlled Metal Diffusion".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.29(2024):19886-19895.

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来源：力学研究所

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