TY - JOUR
AU1 - Liu, Chengyuan
AU2 - Qian, Bing
AU3 - Xiao, Tianci
AU4 - Lv, Chunchun
AU5 - Luo, Jinsong
AU6 - Bao, Jun
AU7 - Pan, Yang
AB - Photocatalysis has emerged as an ideal method for the direct activation and conversion of methane under mild conditions. In this reaction, methyl radical (⋅CH3) was deemed a key intermediate that affected the yields and selectivity of the products. However, direct observation of ⋅CH3 and other intermediates is still challenging. Here, a rectangular photocatalytic reactor coupled with in situ synchrotron radiation photoionization mass spectrometry (SR‐PIMS) was developed to detect reactive intermediates within several hundred microseconds during photocatalytic methane oxidation over Ag−ZnO. Gas phase ⋅CH3 generated by photogenerated holes (O−) was directly observed, and its formation was demonstrated to be significantly enhanced by coadsorbed oxygen molecules. Methoxy radical (CH3O⋅) and formaldehyde (HCHO) were confirmed to be key C1 intermediates in photocatalytic methane overoxidation to CO2. The gas‐phase self‐coupling reaction of ⋅CH3 contributes to the formation of ethane, which indicates the key role of ⋅CH3 desorption in the highly selective synthesis of ethane. Based on the observed intermediates, the reaction network initiated from ⋅CH3 of photocatalytic methane oxidation could be clearly illustrated, which is helpful for studying the photocatalytic methane conversion processes.
TI - Illustrating the Fate of Methyl Radical in Photocatalytic Methane Oxidation over Ag−ZnO by in situ Synchrotron Radiation Photoionization Mass Spectrometry
JF - Angewandte Chemie
DO - 10.1002/ange.202304352
DA - 2023-08-07
UR - https://www.deepdyve.com/lp/wiley/illustrating-the-fate-of-methyl-radical-in-photocatalytic-methane-Rcn0zOJQia
VL - 135
IS - 32
DP - DeepDyve
ER -