Surface-Clean Au25 Nanoclusters in Modulated Microenvironment Enabled by Metal-Organic Frameworks for Enhanced Catalysis

doi:10.1021/jacs.2c09136

	Surface-Clean Au25 Nanoclusters in Modulated Microenvironment Enabled by Metal-Organic Frameworks for Enhanced Catalysis
	Wang, He 1; Liu, Xiyuan 1; Yang, Weijie 2; Mao, Guangyang 2; Meng, Zheng 1; Wu, Zhikun 3; Jiang, Hai-Long 1
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2022-11-21
ISSN号	0002-7863
DOI	10.1021/jacs.2c09136
通讯作者	Jiang, Hai-Long(jianglab@ustc.edu.cn)
英文摘要	Metal nanoclusters (NCs) with atomically precise structures have sparked interest in catalysis. Unfortunately, their high aggregation tendency and the spatial resistance of surface ligands pose significant challenges. Herein, Au25 NCs are encapsulated into isoreticular metal- organic frameworks (MOFs), namely UiO-66-X (X = H, NH2, OH, and NO2), followed by the removal of surface ligands on Au25 NCs. The resulting surface-clean Au25 NCs, protected by the MOF spatial confinement, exhibit much superior activity and stability with respect to pristine Au25 NCs in the oxidative esterification of furfural. Remarkably, experimental and theoretical results jointly demonstrate that diverse functional groups on UiO-66-X modulate the Au25 electronic state, giving rise to the discriminated substrate adsorption energy of Au25@UiO-66-X. As a result, the high electron density and suitable substrate adsorption ability dominate the activity trend: Au25@UiO-66-NH2 > Au25@UiO-66-OH > Au25@UiO-66 > Au25@UiO-66-NO2. This work develops a new strategy for the stabilization of surface-clean metal NCs in pore wall-engineered MOFs for enhanced catalysis.
资助项目	National Key Research and Development Program of China ; National Natural Science Foundation of China ; Collaborative Innovation Program of Hefei Science Center, CAS ; Fundamental Research Funds for the Central Universities ; [2021YFA1500402] ; [21725101] ; [22161142001] ; [21871244] ; [2020HSC-CIP005] ; [WK3450000007] ; [WK2060000038]
WOS关键词	AEROBIC ALCOHOL OXIDATION ; NANOPARTICLES ; GOLD ; PERFORMANCE ; STABILITY ; LIGANDS ; DESIGN
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000889686500001
资助机构	National Key Research and Development Program of China ; National Natural Science Foundation of China ; Collaborative Innovation Program of Hefei Science Center, CAS ; Fundamental Research Funds for the Central Universities
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/131709]
专题	中国科学院合肥物质科学研究院
通讯作者	Jiang, Hai-Long
作者单位	1.Univ Sci & Technol China, Dept Chem, Hefei 230026, Anhui, Peoples R China 2.North China Elect Power Univ, Sch Energy Power & Mech Engn, Dept Power Engn, Baoding 071003, Hebei, Peoples R China 3.Chinese Acad Sci, Inst Solid State Phys, CAS Ctr Excellence Nanosci, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotechn, Hefei 230031, Anhui, Peoples R China
推荐引用方式 GB/T 7714	Wang, He,Liu, Xiyuan,Yang, Weijie,et al. Surface-Clean Au25 Nanoclusters in Modulated Microenvironment Enabled by Metal-Organic Frameworks for Enhanced Catalysis[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2022.
APA	Wang, He.,Liu, Xiyuan.,Yang, Weijie.,Mao, Guangyang.,Meng, Zheng.,...&Jiang, Hai-Long.(2022).Surface-Clean Au25 Nanoclusters in Modulated Microenvironment Enabled by Metal-Organic Frameworks for Enhanced Catalysis.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY.
MLA	Wang, He,et al."Surface-Clean Au25 Nanoclusters in Modulated Microenvironment Enabled by Metal-Organic Frameworks for Enhanced Catalysis".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022).