Investigation into the Catalytic Roles of Various Oxygen Species over Different Crystal Phases of MnO2for C6H6and HCHO Oxidation

Bingbing Chen, Bo Wu, Limei Yu, Mark Crocker, Chuan Shi

Research output: Contribution to journalArticlepeer-review

107 Scopus citations

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 α-, β-, γ-, and δ-MnO2 were synthesized, and their catalytic properties in HCHO and C6H6 oxidation were studied. α- and γ-MnO2 were found to possess much better activity for C6H6 oxidation than δ- and β-MnO2 catalysts, whereas δ-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.

Original languageEnglish
Pages (from-to)6176-6187
Number of pages12
JournalACS Catalysis
Volume10
Issue number11
DOIs
StatePublished - Jun 5 2020

Bibliographical note

Funding Information:
The work was supported by the National Key R&D Program of China (no. 2017YFA0700103), and National Natural Science Foundation of China (nos. 21932002, 21872014, 21707015, and 21577013), the Fundamental Research Funds for the Central Universities (DUT19LK04) and the Natural Science Foundation of Liaoning Province (2019-ZD-0023).

Publisher Copyright:
Copyright © 2020 American Chemical Society.

Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.

Keywords

  • CHand HCHO
  • MVK mechanism
  • catalytic oxidation
  • manganese oxides
  • oxygen species

ASJC Scopus subject areas

  • Catalysis
  • Chemistry (all)

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