Crystal Engineering of MOF‐Derived Bimetallic Oxide Solid Solution Anchored with Au Nanoparticles for Photocatalytic CO2 Reduction to Syngas and C2 Hydrocarbons

• Published in: Angewandte Chemie International Edition Vol. 63; no. 21; pp. e202319177 - n/a
• Main Authors: 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
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 21.05.2024
• Edition: International ed. in English
• Subjects: Absorption spectroscopy; Active sites; Bimetals; C2 hydrocarbons; Carbon dioxide; CO2 reduction; crystal engineering; Electron microscopy; Gold; Hydrocarbons; Intermediates; Metal-organic frameworks; MOF-derived catalysts; Nanoparticles; Photocatalysis; Photocatalysts; Solid solutions; Synthesis gas; X-ray diffraction; MOF-derived catalysts; Crystal Engineering; CO2 REDUCTION; C2 hydrocarbons; Photocatalysis
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202319177

Considering that CO2 reduction is mostly a multielectron reaction, it is necessary for the photocatalysts to integrate multiple catalytic sites and cooperate synergistically to achieve efficient photocatalytic CO2 reduction to various products, such as C2 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 CO2 reduction to syngas (H2 and CO production rates of 271.6 and 260.6 μmol g−1 h−1) and even C2 hydrocarbons (C2H4 and C2H6 production rates of 6.80 and 4.05 μmol g−1 h−1). 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 CO2 reduction, highlighting the synergy effect of the catalytic system with multiple active sites. Through crystal engineering and MOF derivation, the Zr/Ti bimetallic oxide solid solution anchored with Au nanoparticles can be elaborately designed and synthesized to integrate multiple active sites, achieving photocatalytic CO2 reduction to syngas and eventually C2 hydrocarbons under simulated solar light irradiation.