文献类型：期刊文献

英文题名：Operando NMR spectroscopic analysis of proton transfer in heterogeneous photocatalytic reactions

作者：Wang, Xue Lu[1];Liu, Wenqing[2];Yu, Yan-Yan[3];Song, Yanhong[2];Fang, Wen Qi[1];Wei, Daxiu[2];Gong, Xue-Qing[3];Yao, Ye-Feng[2,4];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Normal Univ, Shanghai Key Lab Magnet Resonance, Dept Phys, Shanghai 200062, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]NYU Shanghai, NYU ECNU Inst Phys, 3663 Zhongshan Rd North, Shanghai 200062, Peoples R China

年份：2016

卷号：7

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000379081600001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (21373083, 21421004, 21322307 and 21574043), the Fundamental Research Funds for the Central Universities (WD1313009 and WD1514303), SRF for ROCS, SEM, SRFDP, Program of Shanghai Subject Chief Scientist (15XD1501300), National High-tech R&D Program of China (863 Program; 2014AA123400, 2014AA123401).

语种：英文

摘要：Proton transfer (PT) processes in solid-liquid phases play central roles throughout chemistry, biology and materials science. Identification of PT routes deep into the realistic catalytic process is experimentally challenging, thus leaving a gap in our understanding. Here we demonstrate an approach using operando nuclear magnetic resonance (NMR) spectroscopy that allows to quantitatively describe the complex species dynamics of generated H-2/HD gases and liquid intermediates in pmol resolution during photocatalytic hydrogen evolution reaction (HER). In this system, the effective protons for HER are mainly from H2O, and CH3OH evidently serves as an outstanding sacrificial agent reacting with holes, further supported by our density functional theory calculations. This results rule out controversy about the complicated proton sources for HER. The operando NMR method provides a direct molecular-level insight with the methodology offering exciting possibilities for the quantitative studies of mechanisms of proton-involved catalytic reactions in solid-liquid phases.