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

{"title":"Selective light-driven methane oxidation to ethanol","authors":"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","doi":"10.1038/s41467-024-54835-5","DOIUrl":null,"url":null,"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.","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"77 1","pages":""},"PeriodicalIF":14.7000,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-024-54835-5","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}

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.

Abstract Image

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

求助全文

约1分钟内获得全文去求助

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.

期刊最新文献

Ants integrate proprioception as well as visual context and efference copies to make robust predictions Probabilistic photonic computing with chaotic light Dynamic anti-correlations of water hydrogen bonds Holistic numerical simulation of a quenching process on a real-size multifilamentary superconducting coil Selective light-driven methane oxidation to ethanol