Selective light-driven methane oxidation to ethanol

IF 14.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2024-12-01 DOI:10.1038/s41467-024-54835-5

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, Yong Xu

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引用次数: 0

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.

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.