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

doi:10.1021/acscatal.0c00459

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 journal › Article › peer-review

201 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 language	English
Pages (from-to)	6176-6187
Number of pages	12
Journal	ACS Catalysis
Volume	10
Issue number	11
DOIs	https://doi.org/10.1021/acscatal.0c00459
State	Published - Jun 5 2020

Bibliographical note

Publisher Copyright:
Copyright © 2020 American Chemical Society.

Funding

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).

Funders	Funder number
National Natural Science Foundation of P.R. China	21577013, 21707015, 21872014, 21932002
National Natural Science Foundation of P.R. China
Natural Science Foundation of Liaoning Province	2019-ZD-0023
Natural Science Foundation of Liaoning Province
National Key Basic Research and Development Program of China	2017YFA0700103
National Key Basic Research and Development Program of China
Fundamental Research Funds for the Central Universities	DUT19LK04
Fundamental Research Funds for the Central Universities

Keywords

CHand HCHO
MVK mechanism
catalytic oxidation
manganese oxides
oxygen species

ASJC Scopus subject areas

Catalysis
General Chemistry

Access to Document

10.1021/acscatal.0c00459

Cite this

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

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.",

keywords = "CHand HCHO, MVK mechanism, catalytic oxidation, manganese oxides, oxygen species",

author = "Bingbing Chen and Bo Wu and Limei Yu and Mark Crocker and Chuan Shi",

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year = "2020",

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doi = "10.1021/acscatal.0c00459",

language = "English",

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T1 - Investigation into the Catalytic Roles of Various Oxygen Species over Different Crystal Phases of MnO2for C6H6and HCHO Oxidation

AU - Chen, Bingbing

AU - Wu, Bo

AU - Yu, Limei

AU - Crocker, Mark

AU - Shi, Chuan

PY - 2020/6/5

Y1 - 2020/6/5

N2 - 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.

AB - 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.

KW - CHand HCHO

KW - MVK mechanism

KW - catalytic oxidation

KW - manganese oxides

KW - oxygen species

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