Integrating photochemical and photothermal effects for selective oxidative coupling of methane into C2+ hydrocarbons with multiple active sites
The direct photocatalytic oxidation of methane to value-added chemicals has garnered considerable interest in recent years. However, achieving high productivity while maintaining high selectivity at an appreciable methane conversion rate remains a formidable challenge. Here, we present photochemically-triggered and photothermally-enhanced oxidative coupling of methane to multi-carbon C<sub>2+</sub> alkanes over an Au and CeO<sub>2</sub> nanoparticle-decorated ZnO photocatalyst, which exhibits a record-breaking C<sub>2+</sub> production rate of 17,260 μmol g<sup>-1</sup> h<sup>-1</sup> with ~90% C<sub>2+</sub> selectivity under wide-spectrum light irradiation without a secondary source of heating. Comprehensive characterizations and computational studies reveal that CH<sub>4</sub> activation is a photochemical reaction initiated by ultraviolet light-excited ZnO, and the introduction of CeO<sub>2</sub> substantially enhances the activation of CH<sub>4</sub> and O<sub>2</sub> due to the cooperative interaction between Au and CeO<sub>2</sub>. Concurrently, Au nanoparticles capture visible and near-infrared light to generate localized heating, which greatly promotes the subsequent desorption of produced methyl radical for C-C coupling prior to undergoing further undesired overoxidation.
Authors
- Zhou‐jun Wang (ORCID: https://orcid.org/0000-0002-9196-8062)
- Hui Song (ORCID: https://orcid.org/0000-0001-6424-7959)
- Zhuan Wang (ORCID: https://orcid.org/0000-0001-7770-7192)
- Hengming Huang (ORCID: https://orcid.org/0000-0001-6154-9716)
- Yuxiang Weng (ORCID: https://orcid.org/0000-0003-0423-2266)
- Defa Wang
- Jinhua Ye (ORCID: https://orcid.org/0000-0002-8105-8903)
- Lequan Liu (ORCID: https://orcid.org/0000-0003-3837-6831)
- Shengyao Wang (ORCID: https://orcid.org/0000-0002-2748-483X)
- Kai Sun (ORCID: https://orcid.org/0000-0003-1745-9136)
- Yi Cui (ORCID: https://orcid.org/0000-0002-9182-9038)
- Shangbo Ning (ORCID: https://orcid.org/0000-0002-9278-7378)
- Yifan Li (ORCID: https://orcid.org/0000-0002-3249-1778)
- Xusheng Wang (ORCID: https://orcid.org/0000-0001-5872-8502)
Institutions
- Zhejiang Sci-Tech University (CN)
- Nanjing Tech University (CN)
- Tianjin University (CN)
- Chinese Academy of Sciences (CN)
- Huazhong Agricultural University (CN)
- Ningxia University (CN)
- Suzhou Institute of Nano-tech and Nano-bionics (CN)
- Catalytic Materials (United States) (US)
- Institute of Physics (CN)
- Hebei University (CN)
- Beijing University of Chemical Technology (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-03-22
- DOI
- https://doi.org/10.1038/s41467-025-58101-0
- Citations
- 27
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 13.98
Funders
- National Natural Science Foundation of China
- State Key Laboratory of Chemical Resource Engineering
- State Key Laboratory of Clean Energy Utilization