Surface-Clean Au25 Nanoclusters in Modulated Microenvironment Enabled by Metal-Organic Frameworks for Enhanced Catalysis
文献类型:期刊论文
作者 | Wang, He2; Liu, Xiyuan2; Yang, Weijie1; Mao, Guangyang1; Meng, Zheng2; Wu, Zhikun3; Jiang, Hai-Long2 |
刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY |
出版日期 | 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. |
WOS关键词 | AEROBIC ALCOHOL OXIDATION ; NANOPARTICLES ; GOLD ; PERFORMANCE ; STABILITY ; LIGANDS ; DESIGN |
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 |
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.North China Elect Power Univ, Sch Energy Power & Mech Engn, Dept Power Engn, Baoding 071003, Hebei, Peoples R China 2.Univ Sci & Technol China, Dept Chem, Hefei 230026, Anhui, 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). |
入库方式: OAI收割
来源:合肥物质科学研究院
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