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Catalytic Conversion of C_(1) Molecules on atomically precise Metal Nanoclusters

CCS Chemistry 2022年第1期4卷 66-94页

作者： Dan Yang Yongnan Sun Xiao Cai Weigang Hu Yihu Dai Yan Zhu Yanhui Yang Institute of Advanced Synthesis School of Chemistry and Molecular EngineeringNanjing Tech UniversityNanjing 211816 School of Chemistry and Chemical Engineering Nanjing UniversityNanjing 210093

Metal nanoclusters with accurate compositions and precise crystalline structures hold remarkable attention in serving as a unique model catalyst for well-defined correlations between structure and catalytic activity.More importantly,these metal nanoclusters exhibit strong quantum confinement effects,which differ from their larger nanoparticles in a number of catalytic reactions.This review focuses on recent advances of atomically precise metal nanoclusters for C_(1) compound conversion(C_(O),CO_(2),CH_(4),and HCOOH),including thermally-driven catalysis,photocatalysis,and electrocatalysis.The reaction mechanisms are discussed at an atomic-or even electron-level.It is anticipated that the progress in this research area could be extended to catalytic applications of metal nanoclusters in C_(1) chemistry.

关键词： metal nanocluster atomically precise structure C_(1)molecule catalysis reactivity

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Bulky Thiolate-Protected Silver Nanocluster Ag_(213)(Adm-S)_(44)Cl_(33)with Excellent Electrocatalytic Performance toward Oxygen Reduction

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CCS Chemistry 2023年第5期5卷 1154-1162页

作者： Chen-Guang Shi Jian-Hua Jia Yaling Jia Guangqin Li Ming-Liang Tong Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education School of ChemistrySun Yat-sen UniversityGuangzhouGuangdong 510006

atomically precise gold and/or silver nanoclusters play a key role in crystallography and coordination chemistry.Compared with gold nanoclusters,silver nanoclusters become unstable and difficult to crystallize due to the high reactivity ofmetal silver.Herein,we report a silver nanocluster Ag_(213)(Adm-S)_(44)Cl_(33)(Ag_(213))coprotected by bulky thiolates and chlorides.The low surface thiolate coverage(about 45%)endows Ag_(213)with high catalytic activity.Supported on activated carbon,Ag_(213)nanoclusters exhibit excellent electrocatalytic oxygen reduction performance with Eonset and E_(1/2)values of 0.89 and 0.72 V,respectively,close to the values of commercial Pt/C catalyst.This is the first report on the electrocatalytic oxygen reduction reaction of nanoclusters with more than 100 silver atoms.Ag_(213)with the diameter of 2.75 nm comprises a core–shell structure Ag_(7)@Ag_(32)@Ag_(77)@Ag_(97).The strong plasmonic absorption band at 454 nm reveals the metallic nature of Ag_(213).Interestingly,halide is of importance.Chloride facilitates the formation of Ag_(213)and Ag_(56)(Adm-S)_(33)Cl_(16)(Ag_(56)^(Cl))while bromide can promote the formation of Ag_(56)(Adm-S)_(33)Br_(16)(Ag_(56)Br).This work provides an example for the study of largesized metal nanoclusters and nanocluster-based electrocatalysts.

关键词： silver nanoclusters atomically precise structure oxygen reduction reaction electrocatalysis

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