Controllable Conversion of CO2 on Non-metallic Gold Clusters.
Controllable Conversion of CO2 on Non-metallic Gold Clusters.
复制标题
DOI：
10.1002/anie.201913635
复制
发表时间：
2019-11
影响因子：
--
通讯作者：
Dan Yang;Wei Pei;Si Zhou;Jijun Zhao;Weiping Ding;Yan Zhu
中科院分区：
文献类型：
--
作者：
Dan Yang;Wei Pei;Si Zhou;Jijun Zhao;Weiping Ding;Yan Zhu
金属或等离子体状态的金纳米粒子被广泛用于催化均相和非均相反应。然而，非金属或激子状态下的金催化剂的催化行为仍然难以捉摸。原子精确的AuN原子团簇(n=金原子数)弥合了非金属和金属催化剂之间的差距，为揭示金催化剂在金属、过渡区和非金属状态下的隐藏性质提供了新的机会。本文报道了在Au_9、Au_(11)和Au_(36)三种非金属An团簇上，CO_2转化为不同的目标产物：在Au_9上生成的甲烷、在Au_(11)上生成的乙醇和在Au_(36)上生成的甲酸。非金属原子团簇中编码的结构信息允许原子结构与催化性能的精确关联，从而提供了分子水平的洞察在三种非金属Au催化剂上CO2加氢的不同反应通道。
Gold nanoparticles in metallic or plasmonic state have been widely used to catalyze the homogeneous and heterogeneous reactions. However, the catalytic behaviours of gold catalysts in non-metallic or excitonic state remain elusive. Atomically precise Aun clusters (n = number of gold atoms) bridge the gap between non-metallic and metallic catalysts and offer new opportunities for unveiling the hidden properties of gold catalysts in the metallic, transition regime, and non-metallic states, respectively. Here we report the controllable conversion of CO2 over three non-metallic Aun clusters including Au9, Au11, and Au36, towards different target products: methane produced on Au9, ethanol on Au11, and formic acid on Au36. Structural information encoded in the non-metallic clusters permits a precise correlation of atomic structure with catalytic properties and hence provides molecular-level insight into distinct reaction channels of CO2 hydrogenation over the three non-metallic Au catalysts.