Selective light-driven methane oxidation to ethanol

Methane (CH<sub>4</sub>) photocatalytic upgrading to value-added chemicals, especially C<sub>2</sub> products, is significant yet challenging due to sluggish energy/mass transfer and insufficient chemical driven-force in single photochemical process. Herein, we realize solar-driven CH<sub>4</sub> oxidation to ethanol (C<sub>2</sub>H<sub>5</sub>OH) on crystalline carbon nitride (CCN) modified with Cu<sub>9</sub>S<sub>5</sub> and Cu single atoms (Cu<sub>9</sub>S<sub>5</sub>/Cu-CCN). The integration of photothermal effect and photocatalysis overcomes CH<sub>4</sub>-to-C<sub>2</sub>H<sub>5</sub>OH conversion bottlenecks, with Cu<sub>9</sub>S<sub>5</sub> as a hotspot to convert solar-energy to heat. In-situ characterizations demonstrate that Cu single atoms play as electron acceptor for O<sub>2</sub> reduction to ·OOH/ · OH, while Cu<sub>9</sub>S<sub>5</sub> acts as hole acceptor and site for CH<sub>4</sub> adsorption, C - H activation, and C - C coupling. Theoretical calculations demonstrate that Cu<sub>9</sub>S<sub>5</sub>/Cu-CCN reduces C - C coupling energy barrier by stabilizing ·CH<sub>3</sub> and ·CH<sub>2</sub>O. Impressively, C<sub>2</sub>H<sub>5</sub>OH productivity reaches 549.7 μmol g<sup>-1</sup> h<sup>-1</sup>, with selectivity of 94.8% and apparent quantum efficiency of 0.9% (420 nm). This work provides a sustainable avenue for CH<sub>4</sub> conversion to value-added chemcials.

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Publication Details

Journal
Nature Communications
Published
2024-12-01
DOI
https://doi.org/10.1038/s41467-024-54835-5
Citations
29
Primary Topic
Advanced Photocatalysis Techniques
Type
article
Field-Weighted Citation Impact
2.97

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article

Selective light-driven methane oxidation to ethanol

Zhiwei Hu, Feng Liu, Fei Xue, Huiping Peng et al.
29 citations
Nature Communications
Advanced Photocatalysis Techniques
2.97
article

Selective light-driven methane oxidation to ethanol

Zhiwei Hu, Feng Liu, Fei Xue, Huiping Peng, Chih‐Wen Pao, Xiaoqing Huang, Wei‐Hsiang Huang, Lin Sun, Maochang Liu, Cheng Cheng, Mingshu Chen, Xueli Yan, Chun‐yang Zhang, Yong Xu, Dong Su, Qiuyue Zhang, Xiaozhi Liu, Biao Jiang
article en
29 citations

Abstract

Methane (CH<sub>4</sub>) photocatalytic upgrading to value-added chemicals, especially C<sub>2</sub> products, is significant yet challenging due to sluggish energy/mass transfer and insufficient chemical driven-force in single photochemical process. Herein, we realize solar-driven CH<sub>4</sub> oxidation to ethanol (C<sub>2</sub>H<sub>5</sub>OH) on crystalline carbon nitride (CCN) modified with Cu<sub>9</sub>S<sub>5</sub> and Cu single atoms (Cu<sub>9</sub>S<sub>5</sub>/Cu-CCN). The integration of photothermal effect and photocatalysis overcomes CH<sub>4</sub>-to-C<sub>2</sub>H<sub>5</sub>OH conversion bottlenecks, with Cu<sub>9</sub>S<sub>5</sub> as a hotspot to convert solar-energy to heat. In-situ characterizations demonstrate that Cu single atoms play as electron acceptor for O<sub>2</sub> reduction to ·OOH/ · OH, while Cu<sub>9</sub>S<sub>5</sub> acts as hole acceptor and site for CH<sub>4</sub> adsorption, C - H activation, and C - C coupling. Theoretical calculations demonstrate that Cu<sub>9</sub>S<sub>5</sub>/Cu-CCN reduces C - C coupling energy barrier by stabilizing ·CH<sub>3</sub> and ·CH<sub>2</sub>O. Impressively, C<sub>2</sub>H<sub>5</sub>OH productivity reaches 549.7 μmol g<sup>-1</sup> h<sup>-1</sup>, with selectivity of 94.8% and apparent quantum efficiency of 0.9% (420 nm). This work provides a sustainable avenue for CH<sub>4</sub> conversion to value-added chemcials.

Nature CommunicationsVol. 15(1)
Xiamen University (CN), Chinese Academy of Sciences (CN), Suzhou Institute of Nano-tech and Nano-bionics (CN), National Synchrotron Radiation Research Center (TW), Max Planck Institute for Chemical Physics of Solids (DE), Tan Kah Kee Innovation Laboratory (CN), Institute of Physics (CN), Xi'an Jiaotong University (CN)
National Natural Science Foundation of China, Pohang University of Science and Technology, Natural Science Foundation of Guangdong Province, Xiamen University, Suzhou Institute of Nanotechnology, Chinese Academy of Sciences
Openalex Percentile: Top 8%
Advanced Photocatalysis Techniques
2.97
DOIOpen Access PDFOpenAlex
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