Carbon Nitride With Abundant Nitrogen Vacancies for Methane Oxidation Under Mild Conditions

ABSTRACT Direct methane oxidation to oxygenates under mild conditions is challenging due to the inert C─H bond in methane, especially for nonmetal catalytic systems. In this study, we report that nitrogen vacancy‐rich graphitic carbon nitride (g‐C 3 N 4 ) serves as an effective catalyst for methane oxidation using H 2 O 2 as the oxidant. Under optimized conditions (3 MPa CH 4 , 70°C, 1 h), the g‐C 3 N 4 catalyst with the highest nitrogen vacancy concentration ( V N ‐rich CN) achieved an oxygenates yield of 13.42 µmol. Comprehensive characterization and mechanistic studies revealed that nitrogen vacancies in g‐C 3 N 4 facilitate H 2 O 2 decomposition into hydroxyl radicals (·OH), which subsequently activate methane to form oxygenates. Notably, the catalytic activity exhibited a positive correlation with nitrogen vacancy concentration, demonstrating the critical role of these defects in the oxidation process.

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Publication Details

Journal
ChemCatChem
Published
2026-05-01
DOI
https://doi.org/10.1002/cctc.70756
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
0.00

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article

Carbon Nitride With Abundant Nitrogen Vacancies for Methane Oxidation Under Mild Conditions

X Zhao, Jie Zeng, Hongfei Lin, Jingwen Hu et al.
ChemCatChem
Catalytic Processes in Materials Science
article

Carbon Nitride With Abundant Nitrogen Vacancies for Methane Oxidation Under Mild Conditions

X Zhao, Jie Zeng, Hongfei Lin, Jingwen Hu, Wenlong Wu, Haibin Yin, Bo Wu, Hepeng Luo
article en

Abstract

ABSTRACT Direct methane oxidation to oxygenates under mild conditions is challenging due to the inert C─H bond in methane, especially for nonmetal catalytic systems. In this study, we report that nitrogen vacancy‐rich graphitic carbon nitride (g‐C 3 N 4 ) serves as an effective catalyst for methane oxidation using H 2 O 2 as the oxidant. Under optimized conditions (3 MPa CH 4 , 70°C, 1 h), the g‐C 3 N 4 catalyst with the highest nitrogen vacancy concentration ( V N ‐rich CN) achieved an oxygenates yield of 13.42 µmol. Comprehensive characterization and mechanistic studies revealed that nitrogen vacancies in g‐C 3 N 4 facilitate H 2 O 2 decomposition into hydroxyl radicals (·OH), which subsequently activate methane to form oxygenates. Notably, the catalytic activity exhibited a positive correlation with nitrogen vacancy concentration, demonstrating the critical role of these defects in the oxidation process.

ChemCatChemVol. 18(9)
Hefei National Center for Physical Sciences at Nanoscale (CN), Geological Exploration Technology Institute of Jiangsu Province (CN), King Abdullah University of Science and Technology (SA), Anhui University of Technology (CN)
Natural Science Foundation for Distinguished Young Scholars of Anhui Province, National Natural Science Foundation of China, Science and Technology Development Fund, State Key Laboratory of Catalysis, National Synchrotron Radiation Laboratory, National Key Research and Development Program of China, Fundamental Research Funds for the Central Universities
Openalex Percentile: Top 12%
Catalytic Processes in Materials Science
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Carbon Nitride With Abundant Nitrogen Vacancies for Methane Oxidation Under Mild Conditions — X Zhao, Jie Zeng, et al. · ChemCatChem (2026) | TGRS Research Map | TGRS