具有原子精度单分散的负载型金基纳米催化剂在催化选择性氧化领域具有重要的意义和潜在应用价值。本课题首次提出以原子精度的单分散水溶性硫醇稳定金纳米簇为前体，通过修饰的浸渍吸附法可控制备水滑石（LDH）负载超细单分散原子精度的金纳米簇催化剂。其一，精细调控合成参数，控制动力学过程（低温、慢速搅拌）制备出原子精度的纯相谷胱甘肽和卡托普利稳定水溶性金纳米簇（Au25(SR)18或 Au38(SR)24）；其二，通过预分散小尺寸高结晶度LDH纳米片提供碱性介质抑制金纳米簇的自团聚，再利用二者间的静电作用将带负电的纳米簇吸附到LDH表面，经适度焙烧除去配体同时保持金簇的超小尺寸（< 2 nm）。系统表征纳米簇的组成、尺寸和电子结构，研究金纳米簇与不同组成LDH间的相互作用。通过实验研究与理论分析比较金纳米簇尺寸效应及Au25簇-LDH协同效应对负载型原子精度金簇的醇选择氧化活性与稳定性的本质影响规律。

Atomically precise monodispersed supported gold-based catalyst hold important interest and potential application in selectively catalytic oxidation areas. The project firstly aims at synthesizing hydrotalcite (layered double hydroxide: LDH) supported ultrafine gold-based nanocluster catalyst by atomically precise water-soluable thiol-protected Au nanocluster (Aun(SR)m). (1) Pure-phase glutathione- and captopril-stabilized gold clusters (Au25(SR)18 and Au38(SR)24) can be prepared by carefully tuning the reaction kinetics such as low temperature (zero degree or ambient temperature) and slow initial stirring rate, which is critical for subsequent growth of monodisperse gold clusters. (2) Ultrafine LDH-supported gold nanocluster catalyst can be synthesized by modified adsorption step of the as-prepared negatively charged Aun(SR)m clusters onto the predispersed LDH nanolayers via electrostatic attraction followed by proper calcination to remove the thiol ligands but remained ultrasmall size (< 2 nm) aiming at acquiring highly active and stable supported gold nanocluster/ superatom catalyst. Combinational characterizations can be employed to study the compositions, size and electron structure of Au nanoclusters and the effect of the interactions between Au25 cluster and LDH nanoplates with varied compositions on the selectively catalytic oxidation for alcohols. Based on experimental data and theory analysis, the key role of size effect of Au nanoclusters and gold-LDH synergetic function of the novel atomically precise gold cluster catalysts in alcohol oxidation can be compared and revealed.