Hu Qinyuan, Li Mengqian, Zhu Juncheng, Zhang Zhixing, He Dongpo, Zheng Kai, Wu Yang, Fan Minghui, Zhu Shan, Yan Wensheng, Hu Jun, Zhu Junfa, Chen Qingxia, Jiao Xingchen, Xie Yi
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China.
Hefei National Research Center for Physical Sciences at Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China.
Nano Lett. 2024 Apr 17;24(15):4610-4617. doi: 10.1021/acs.nanolett.4c00748. Epub 2024 Apr 2.
The intricate protonation process in carbon dioxide reduction usually makes the product unpredictable. Thus, it is significant to control the reactive intermediates to manipulate the reaction steps. Here, we propose that the synergistic La-Ti active sites in the N-LaTiO nanosheets enable the highly selective carbon dioxide photoreduction into methane. In the photoreduction of CO over N-LaTiO nanosheets, Fourier transform infrared spectra are utilized to monitor the *CHO intermediate, pivotal for methane production, whereas such monitoring is not conducted for LaTiO nanosheets. Also, theoretical calculations testify to the increased charge densities on the Ti and La atoms and the regulated formation energy barrier of *CO and *CHO intermediates by the constructed synergistic active sites. Accordingly, the methane formation rate of 7.97 μL h exhibited by the N-LaTiO nanosheets, along with an electron selectivity of 96.6%, exceeds that of most previously reported catalysts under similar conditions.
