Direct evidence for hydrated protons as the active species in artificial photocatalytic water reduction into hydrogen  

作　　者：Feng Xiong Zhengming Wang Zongfang Wu Guanghui Sun Hong Xu Peng Chai Weixin Huang 

机构地区：[1]Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China

出　　处：《Science China Chemistry》2019年第2期199-204,共6页中国科学（化学英文版）

基　　金：supported by the National Key R & D Program of Ministry of Science and Technology of China (2017YFB0602205);the National Natural Science Foundation of China (21525313, 21761132005, 91745202);Chinese Academy of Sciences (KJZD-EW-M03);the Changjiang Scholars Program of Ministry of Education of China, the Fundamental Research Funds for the Central Universities of Ministry of Education of China (WK2060030017, WK2060030024);Collaborative Innovation Center of Suzhou Nano Science and Technology

摘　　要：Photocatalytic water reduction to hydrogen over oxide semiconductors is one of the most extensively investigated artificial photocatalytic reactions, but the nature of the active species has not yet been elucidated. Here, we successfully prepared Pt/rutile TiO_2(110) surfaces with hydrated proton species via co-adsorption of hydrogen and water and observed the photocatalytic reduction of hydrated protons to H_2 upon UV light illumination. These results provide experimental evidence to prove hydrated protons as the active species for photocatalytic water reduction to hydrogen and demonstrate the occurrence of photocatalytic reduction of hydrated protons to H_2 within the H-bonding network on the catalyst surface instead of directly on the catalyst surface. The Pt-TiO_2 interface is capable of dissociating water to form hydroxyl groups that facilitate the formation of H-bonding network on the catalyst surface to enhance the photocatalytic H_2 production. Our results greatly advance fundamental understanding of artificial photocatalytic water reduction.Photocatalytic water reduction to hydrogen over oxide semiconductors is one of the most extensively investigated artificial photocatalytic reactions, but the nature of the active species has not yet been elucidated. Here, we successfully prepared Pt/rutile TiO_2(110) surfaces with hydrated proton species via co-adsorption of hydrogen and water and observed the photocatalytic reduction of hydrated protons to H_2 upon UV light illumination. These results provide experimental evidence to prove hydrated protons as the active species for photocatalytic water reduction to hydrogen and demonstrate the occurrence of photocatalytic reduction of hydrated protons to H_2 within the H-bonding network on the catalyst surface instead of directly on the catalyst surface. The Pt-TiO_2 interface is capable of dissociating water to form hydroxyl groups that facilitate the formation of H-bonding network on the catalyst surface to enhance the photocatalytic H_2 production. Our results greatly advance fundamental understanding of artificial photocatalytic water reduction.

关 键 词：surface CHEMISTRY reaction mechanism PHOTOCATALYSIS PT/TIO2 H-BONDING network 

分 类 号：O6[理学—化学]