Jia Henglei, Dou Yanrong, Yang Yuanyuan, Li Fan, Zhang Chun-Yang
College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals, Shandong Normal University, Jinan 250014, China.
Nanoscale. 2021 Dec 13;13(47):20289-20298. doi: 10.1039/d1nr05801k.
Photocatalytic conversion of carbon dioxide (CO) to liquid product acetaldehyde (CHCHO) remains a great challenge due to the involvement of a complex 10-electron reduction process and a sluggish C-C coupling reaction. Herein, we report the synthesis of Janus silver/ternary silver halide (Ag/AgClBr) nanostructures through precisely manipulating the growth kinetics and its function as a plasmonic photocatalyst to boost the conversion of CO to CHCHO. The obtained Janus nanostructures featuring both spatially separated architecture and broad light-harvesting capability facilitate the photocatalytic reduction of CO under solar illumination. The photocatalytic CO reduction with the characteristics of high activity and good selectivity can generate a 10-electron reduction product CHCHO with a generation rate of 209.3 ± 9.5 μmol h g and a selectivity of 96.9%, which are rarely achieved in previously reported photocatalytic CO reduction systems. The excellent photocatalytic performance can be ascribed to the plasmonic effect of Ag nanocrystals and the favorable active sites on the catalyst surface. This research demonstrates for the first time the utilization of the Janus Ag/AgClBr nanostructures to generate the value-added C liquid product through photocatalytic CO reduction, paving the way for the design and construction of novel plasmonic photocatalysts.
将二氧化碳（CO₂）光催化转化为液体产物乙醛（CH₃CHO）仍然是一个巨大的挑战，这是由于涉及复杂的10电子还原过程以及缓慢的C-C偶联反应。在此，我们报道了通过精确控制生长动力学合成Janus银/三元卤化银（Ag/AgClBr）纳米结构及其作为等离子体光催化剂促进CO₂转化为CH₃CHO的功能。所获得的Janus纳米结构具有空间分离的结构和广泛的光捕获能力，有利于在太阳光照射下光催化还原CO₂。具有高活性和良好选择性的光催化CO₂还原能够生成10电子还原产物CH₃CHO，生成速率为209.3±9.5 μmol h⁻¹ g⁻¹，选择性为96.9%，这在先前报道的光催化CO₂还原系统中很少实现。优异的光催化性能可归因于Ag纳米晶体的等离子体效应和催化剂表面有利的活性位点。本研究首次证明了利用Janus Ag/AgClBr纳米结构通过光催化CO₂还原生成增值C液体产物，为新型等离子体光催化剂的设计和构建铺平了道路。
