Efficient Selective Oxidation of Aromatic Alkanes by Double Cobalt Active Sites over Oxygen Vacancy‐rich Mesoporous Co3O4

Author:

Liu Yali12,Zheng Yuenan13,Feng Danyang4,Zhang Liangliang1,Zhang Ling5,Song Xiaowei1,Qiao Zhen‐An1ORCID

Affiliation:

1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University Changchun, Jilin 130012 China

2. Department of Chemical Engineering, School of Petrochemical Engineering & Environment Zhejiang Ocean University Zhoushan, Zhejiang 316022 China

3. State Key Laboratory of Fine Chemicals, School of Chemical Engineering Dalian University of Technology Dalian, Liaoning 116081 China

4. Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Northeast Normal University Jilin 130024 China

5. State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry Jilin University Changchun, Jilin 130012 China

Abstract

AbstractThe development of efficient catalyst for selective oxidation of hydrocarbon to functional compounds remains a challenge. Herein, mesoporous Co3O4 (mCo3O4‐350) showed excellent catalytic activity for selective oxidation of aromatic‐alkanes, especially for oxidation of ethylbenzene with a conversion of 42 % and selectivity of 90 % for acetophenone at 120 °C. Notably, mCo3O4 presented a unique catalytic path of direct oxidation of aromatic‐alkanes to aromatic ketones rather than the conventional stepwise oxidation to alcohols and then to ketones. Density functional theory calculations revealed that oxygen vacancies in mCo3O4 activate around Co atoms, causing electronic state change from Co3+(Oh)→Co2+(Oh). Co2+(Oh) has great attraction to ethylbenzene, and weak interaction with O2, which provide insufficient O2 for gradual oxidation of phenylethanol to acetophenone. Combined with high energy barrier for forming phenylethanol, the direct oxidation path from ethylbenzene to acetophenone is kinetically favorable on mCo3O4, sharply contrasted to non‐selective oxidation of ethylbenzene on commercial Co3O4.

Funder

National Natural Science Foundation of China

Publisher

Wiley

Subject

General Medicine

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