Indexed by:Journal Papers

First Author:Chen, Bingbing

Correspondence Author:Shi, C (reprint author), Dalian Univ Technol, State Key Lab Fine Chem, Sch Chem Engn, Dalian 116024, Peoples R China.

Co-author:Wu, Bo,Yu, Limei,Crocker, Mark,Shi, Chuan

Date of Publication:2020-06-05

Journal:ACS CATALYSIS

Included Journals:SCIE

Volume:10

Issue:11

Page Number:6176-6187

ISSN No.:2155-5435

Key Words:manganese oxides; oxygen species; C6H6 and HCHO; catalytic oxidation; MVK mechanism

Abstract:Although manganese oxide (MnO2) exhibits excellent activity in various oxidation reactions, especially for volatile organic compound oxidation, the origin of the catalytic activity remains ambiguous and controversial. In this study, four types of MnO2 catalysts with crystal phases corresponding to alpha-, beta-,gamma-, and delta-MnO2 were synthesized, and their catalytic properties in HCHO and C6H6 oxidation were studied. alpha- and gamma-MnO2 were found to possess much better activity for C6H6 oxidation than delta- and beta-MnO2 catalysts, whereas delta-MnO2 exhibited the best performance for HCHO oxidation as compared with other types of MnO2. Three kinds of oxygen species were discriminated based on their Mn-O bond strength and reducibility. By quantitatively correlating the amount of specific oxygen species with the reaction rates, the catalytic roles of different oxygen species in HCHO and C6H6 oxidation were clarified. With the assistance of isotopic labeling studies, the participation of oxygen species in C6H6 oxidation-which followed a Mars-van Krevelen mechanism-was illuminated.