文献类型：期刊文献

英文题名：Unveiling the Nature of Room-Temperature O2 Activation and O2?- Enrichment on MgO-Loaded Porous Carbons with Efficient H2S Oxidation

作者：Pan, Yankai[1];Xu, Hai[1];Chen, Mingqi[1];Wu, Kede[1];Zhang, Yayun[1];Long, Donghui[1,2]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Key Lab Multiphase Mat Chem Engn, Shanghai 200237, Peoples R China

年份：2021

卷号：11

期号：10

起止页码：5974

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20212210427447);WOS:【SCI-EXPANDED(收录号:WOS:000656056200009)】；

基金：This work was financially supported by the National Natural Science Foundation of China (nos. 21576090, 21878091, and 22008073).

语种：英文

外文关键词：oxygen activation; O-2(center dot-); enrichment; radical reaction; heterogenous catalysis; desulfurization

摘要：The activation of O-2 into the dioxide radical (O-2(center dot-)) at room temperature serves as a critical chemical process implicated in environmental remediation and industrial chemical processes, but the involved mechanism remains unclear. Herein, we address this challenge by the radical detection method combined with DFT study and unveil that the O-2 activation reaction could take place merely in porous carbons (PCs) at room temperature. DFT calculations indicate that sp(2)-conjugated carbons can transfer a pi* electron to the outer orbit of the O-2 molecule derived by the space confinement in ultramicropores (similar to 0.4 nm), and the presence of edge site defects and heterogeneous atoms can facilitate the electron transfer due to increased quantity of free electrons. The produced O-2(center dot-) radicals could be further trapped and enriched on the surface of MgO as predicted by DFT calculations, which is subsequently confirmed by radical detection analysis of the designed MgO-loaded PCs. Furthermore, the O-2 activation and O-2(center dot-) enrichment on MgO-loaded PCs are applied in a probe reaction of room-temperature catalytic H2S oxidation, in which an outstanding catalytic performance is achieved. These findings provide valuable insight into the intrinsic origin of the O-2 activation at room temperature and open a fresh route to efficient formation and concentration of O-2(center dot-) for aerobic oxidization processes.