Ligand-Shell Engineering of a Au28 Nanocluster Boosts Electrocatalytic CO2 Reduction.
Ligand-Shell Engineering of a Au28 Nanocluster Boosts Electrocatalytic CO2 Reduction.
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Au28 纳米团簇的配体壳工程可促进电催化 CO2 还原。
DOI：
10.1002/anie.202207492
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发表时间：
2022
影响因子：
--
通讯作者：
T. Mak
中科院分区：
文献类型：
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作者：
Jie Wang;F. Xu;Zhao;Shuangquan Zang;T. Mak
金纳米团簇（NC）的细微剪裁可以显着赋予其物理化学性质。然而，直接比较的催化性能的金NC具有相同的金属核，但不同的配体壳很少阐明。本工作采用自还原法合成了一种新的金NC，即Au 28（C2 B H11 S）12（tht）4 Cl 4（Au 28 -S）. Au 28 -S采用与已报道的炔基保护的Au 28 -C相同的Au 28金属骨架。不同的保护层导致其电子结构和光学性质的差异。此外，Au 28 -S对CO2电化学还原为CO具有更好的催化活性，理论计算确定了催化剂的活性中心，并阐明了不同催化剂的催化机理.该工作为研究金纳米粒子的保护层与活性关系提供了一个理想的平台，也可为金属纳米粒子基催化剂的设计提供指导。
Subtle tailoring of gold nanoclusters (NCs) could significantly impart their physicochemical properties. However, direct comparison of the catalytic performance of gold NCs with identical metal core but distinct ligand shells is rarely elucidated. In this work, a novel gold NC, Au 28 (C 2 B 10 H 11 S) 12 (tht) 4 Cl 4 ( Au 28 -S ), was isolated by a facile self-reducing synthesis. Au 28 -S adopts an identical Au 28 metal framework with the reported alkynyl-protected Au 28 -C . The different protective layers lead to distinctions in their electronic structure and optical properties. Furthermore, Au 28 -S shows more excellent catalytic activity for the electrochemical reduction of CO 2 to CO. Theoretical calculations identified the active sites and shed light on the catalytic mechanism to elucidate the different catalytic performances. This work provides an ideal platform to study the protective layer-activity relationship of gold NCs, and may also provide guidance in the design of metal NC-based catalysts.