Huang Ning-Yu, Li Bai, Wu Duojie, Chen Zhen-Yu, Shao Bing, Chen Di, Zheng Yu-Tao, Wang Wenjuan, Yang Chunzhen, Gu Meng, Li Lei, Xu Qiang
Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials (SKLPM), SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory (SKAEM-JIL), Department of Chemistry and Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China.
Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials (SKLPM), Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China.
Angew Chem Int Ed Engl. 2024 May 21;63(21):e202319177. doi: 10.1002/anie.202319177. Epub 2024 Apr 9.
Considering that CO reduction is mostly a multielectron reaction, it is necessary for the photocatalysts to integrate multiple catalytic sites and cooperate synergistically to achieve efficient photocatalytic CO reduction to various products, such as C hydrocarbons. Herein, through crystal engineering, we designed and constructed a metal-organic framework-derived Zr/Ti bimetallic oxide solid solution support, which was confirmed by X-ray diffraction, electron microscopy and X-ray absorption spectroscopy. After anchoring Au nanoparticles, the composite photocatalyst exhibited excellent performances toward photocatalytic CO reduction to syngas (H and CO production rates of 271.6 and 260.6 μmol g h) and even C hydrocarbons (CH and CH production rates of 6.80 and 4.05 μmol g h). According to the control experiments and theoretical calculations, the strong interaction between bimetallic oxide solid solution support and Au nanoparticles was found to be beneficial for binding intermediates and reducing CO reduction, highlighting the synergy effect of the catalytic system with multiple active sites.
考虑到CO还原大多是多电子反应,光催化剂有必要整合多个催化位点并协同作用,以实现将CO高效光催化还原为各种产物,如碳氢化合物。在此,通过晶体工程,我们设计并构建了一种金属有机框架衍生的Zr/Ti双金属氧化物固溶体载体,这通过X射线衍射、电子显微镜和X射线吸收光谱得到证实。在锚定Au纳米颗粒后,复合光催化剂在将CO光催化还原为合成气(H和CO的产率分别为271.6和260.6 μmol g h)甚至碳氢化合物(CH和CH的产率分别为6.80和4.05 μmol g h)方面表现出优异的性能。根据对照实验和理论计算,发现双金属氧化物固溶体载体与Au纳米颗粒之间的强相互作用有利于结合中间体并降低CO还原,突出了具有多个活性位点的催化体系的协同效应。