Selective light-driven methane oxidation to ethanol

Fei Xue, Chunyang Zhang, Cheng Cheng, Xueli Yan, Feng Liu, Xiaozhi Liu, Biao Jiang, Qiuyue Zhang, Lin Sun, Huiping Peng, Wei-Hsiang Huang, Chih-Wen Pao, Zhiwei Hu, Mingshu Chen, Dong Su, Maochang Liu (), Xiaoqing Huang () and Yong Xu ()
Additional contact information
Fei Xue: Chinese Academy of Sciences (CAS)
Chunyang Zhang: Xi’an Jiaotong University
Cheng Cheng: Xi’an Jiaotong University
Xueli Yan: Xi’an Jiaotong University
Feng Liu: Xi’an Jiaotong University
Xiaozhi Liu: Chinese Academy of Sciences
Biao Jiang: Xi’an Jiaotong University
Qiuyue Zhang: Xiamen University
Lin Sun: Xiamen University
Huiping Peng: Xiamen University
Wei-Hsiang Huang: National Synchrotron Radiation Research Center
Chih-Wen Pao: National Synchrotron Radiation Research Center
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids
Mingshu Chen: Xiamen University
Dong Su: Chinese Academy of Sciences
Maochang Liu: Xi’an Jiaotong University
Xiaoqing Huang: Xiamen University
Yong Xu: Chinese Academy of Sciences (CAS)

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Methane (CH4) photocatalytic upgrading to value-added chemicals, especially C2 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 CH4 oxidation to ethanol (C2H5OH) on crystalline carbon nitride (CCN) modified with Cu9S5 and Cu single atoms (Cu9S5/Cu-CCN). The integration of photothermal effect and photocatalysis overcomes CH4-to-C2H5OH conversion bottlenecks, with Cu9S5 as a hotspot to convert solar-energy to heat. In-situ characterizations demonstrate that Cu single atoms play as electron acceptor for O2 reduction to ·OOH/ · OH, while Cu9S5 acts as hole acceptor and site for CH4 adsorption, C − H activation, and C − C coupling. Theoretical calculations demonstrate that Cu9S5/Cu-CCN reduces C − C coupling energy barrier by stabilizing ·CH3 and ·CH2O. Impressively, C2H5OH productivity reaches 549.7 μmol g–1 h–1, with selectivity of 94.8% and apparent quantum efficiency of 0.9% (420 nm). This work provides a sustainable avenue for CH4 conversion to value-added chemcials.

Date: 2024
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DOI: 10.1038/s41467-024-54835-5

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