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.
Authors
- X Zhao (ORCID: https://orcid.org/0000-0001-6672-4720)
- Jie Zeng (ORCID: https://orcid.org/0000-0002-8812-0298)
- Hongfei Lin (ORCID: https://orcid.org/0000-0001-8198-1493)
- Jingwen Hu (ORCID: https://orcid.org/0000-0002-2560-9977)
- Wenlong Wu
- Haibin Yin
- Bo Wu (ORCID: https://orcid.org/0009-0007-0217-2331)
- Hepeng Luo
Institutions
- 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)
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
Funders
- 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