Turning Au Nanoclusters Catalytically Active for Visible-Light-Driven CO2 Reduction through Bridging Ligands
Turning Au Nanoclusters Catalytically Active for Visible-Light-Driven CO2 Reduction through Bridging Ligands
复制标题
通过桥连配体使金纳米团簇具有催化活性，实现可见光驱动的二氧化碳还原
DOI：
10.1021/jacs.8b06723
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发表时间：
2018-12-05
影响因子：
15
通讯作者：
Xiong, Yujie
中科院分区：
文献类型：
--
作者：
Cui, Xiaofeng;Wang, Jin;Xiong, Yujie
可见光催化材料的开发是太阳能驱动CO2转化的最终目标。Au纳米团簇（NC）可以潜在地用作用于收集可见光的组件，但是由于缺乏催化位点而几乎不能执行太阳能驱动的CO2还原。在本文中，我们报告了一种有效的策略，使Au纳米团簇对可见光CO 2还原具有催化活性，其中金属阳离子（Fe 2+，Co 2+，Ni 2+和Cu 2+）使用L-半胱氨酸作为桥接配体接枝到Au NCs上。金属-S键桥促进了电子从Au NCs到金属阳离子的转移，使得接枝的金属阳离子可以接收光生电子并作为CO 2还原的催化位点。对于不同的金属阳离子，不同的d带中心和与CO的结合能允许调节电子转移效率和CO活化能。此外，通过金属有机骨架的包覆，可以显著提高Au NCs基催化剂的光稳定性。该工作为基于金属簇的光催化剂设计打开了一扇新的大门，并为金属簇的表面工程提供了具体的应用。
Development of visible-light photocatalytic materials is an ultimate goal for solar-driven CO, conversion. Au nanoclusters (NCs) may potentially serve as components for harvesting visible light but can hardly perform solar-driven CO, reduction due to the lack of catalytic sites. Herein, we report an effective strategy for turning Au nanoclusters catalytically active for visible-light CO, reduction, in which metal cations (Fe2+, Co2+, Ni2+, and Cu2+) are grafted to the Au NCs using L-cysteine as a bridging ligand. The metal-S bonding bridge facilitates the electron transfer from Au NCs to metal cations so that the grafted metal cations can receive photoinduced electrons and work as catalytic sites for CO, reduction. The varied d-band centers and binding energies with CO, for different metal cations allow tuning electron transfer efficiency and CO, activation energy. Furthermore, the photostability of Au NCs-based catalyst can be significantly enhanced through the encapsulation with metal organic frameworks. This work opens a new door for the photocatalyst design based on metal clusters and sheds light on the surface engineering of metal clusters toward specific applications.