The development of excellent catalyst to achieve photocatalytic syngas production from CO_(2) and H_(2)O is a prospective and sustainable strategy to alleviate environment and energy crisis. In this study, a unique Ja...The development of excellent catalyst to achieve photocatalytic syngas production from CO_(2) and H_(2)O is a prospective and sustainable strategy to alleviate environment and energy crisis. In this study, a unique Janus PdZn-Co catalyst is prepared by annealed the Pd/IRMOF-3(Co, Zn) precursor. Due to the strong interaction, the electron transfers from PdZn terminal to Co terminal in the Janus structure. The electron-received Co terminal facilitates Co sites coordinate with the electrophilic C atom of CO_(2) and the electron-donated PdZn center is easier to coordinate with nucleophilic O atoms of H_(2)O or C=O bonds.The charge redistribution enhances the absorption of CO_(2) and H2O, which promotes H_(2) evolution and CO production. In addition, the carbon shell effectively suppresses the metal core agglomeration and facilitates the electron transmission from photosensitizer to metallic active sites. Meanwhile, the ratio of CO/H_(2) can be regulated(~3:1 to 2:1) by adjusting the proportion of Co and PdZn. The Janus structure and graphite carbon synergistically play a profound impact on improving the photocatalytic performance.The optimized PdZn-Co catalyst exhibits a superior photocatalytic CO production rate(20.03 μmol/h) and the H_(2) generation rate(9.90 μmol/h) with a ratio of CO/H_(2)= 2.02.展开更多
基金supported by the National Natural Science Foundation of China (No. 51872025)the National Key R&D Program of China (No. 2021YFB3802200)+4 种基金Natural Science Foundation of Guangdong Province (No. 2220XCC061)the National Defense Basic Scientific Research (No. JCKY2021110B206)Scientific and Technological Innovation Foundation of Foshan (No. BK21BE008)Zibo Key Research and Development Program (No. 2020XCCG0036)supported by USTB MatCom of Beijing Advanced Innovation Center for Materials Genome Engineering。
文摘The development of excellent catalyst to achieve photocatalytic syngas production from CO_(2) and H_(2)O is a prospective and sustainable strategy to alleviate environment and energy crisis. In this study, a unique Janus PdZn-Co catalyst is prepared by annealed the Pd/IRMOF-3(Co, Zn) precursor. Due to the strong interaction, the electron transfers from PdZn terminal to Co terminal in the Janus structure. The electron-received Co terminal facilitates Co sites coordinate with the electrophilic C atom of CO_(2) and the electron-donated PdZn center is easier to coordinate with nucleophilic O atoms of H_(2)O or C=O bonds.The charge redistribution enhances the absorption of CO_(2) and H2O, which promotes H_(2) evolution and CO production. In addition, the carbon shell effectively suppresses the metal core agglomeration and facilitates the electron transmission from photosensitizer to metallic active sites. Meanwhile, the ratio of CO/H_(2) can be regulated(~3:1 to 2:1) by adjusting the proportion of Co and PdZn. The Janus structure and graphite carbon synergistically play a profound impact on improving the photocatalytic performance.The optimized PdZn-Co catalyst exhibits a superior photocatalytic CO production rate(20.03 μmol/h) and the H_(2) generation rate(9.90 μmol/h) with a ratio of CO/H_(2)= 2.02.
