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揭示石墨相氮化碳与氧化铜对CO电还原为CH的协同效应。

Unveiling the Synergistic Effect between Graphitic Carbon Nitride and Cu O toward CO Electroreduction to C H.

作者信息

Zhang Jiguang, Guo Yuting, Shang Bin, Fan Tingting, Lian Xinyi, Huang Pingping, Dong Yunyun, Chen Zhou, Yi Xiaodong

机构信息

National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, College of Materials, Xiamen University, Xiamen, 361005, P. R. China.

College of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng, 252059, P. R. China.

出版信息

ChemSusChem. 2021 Feb 5;14(3):929-937. doi: 10.1002/cssc.202002427. Epub 2020 Dec 18.

Abstract

Electrochemically reducing carbon dioxide (CO RR) to ethylene is one of the most promising strategies to reduce carbon dioxide emissions and simultaneously produce high value-added chemicals. However, the lack of catalysts with excellent activity and stability limits the large-scale application of this technology. In this work, a graphitic carbon nitride (g-C N )-supported Cu O composite was fabricated, which exhibited a 32.2 % faradaic efficiency of C H with a partial current density of -4.3 mA cm at -1.1 V vs. reversible hydrogen electrode in 0.1 m KHCO electrolyte. The introduction of g-C N support not only enhanced the uniform dispersion of Cu O nanocubes, but also stabilized the important *CO intermediates. Moreover, the g-C N itself had a good activity of reducing CO to form *CO, which enriched the key intermediates of C-C coupling around cuprous oxide. The findings highlight the importance of the g-C N support, a unique two-dimensional material, including not only the strong CO adsorption and activation capacity but also its synergistic effect with the cuprous oxide in CO RR selectivity.

摘要

将二氧化碳电化学还原为乙烯是减少二氧化碳排放并同时生产高附加值化学品最具前景的策略之一。然而,缺乏具有优异活性和稳定性的催化剂限制了该技术的大规模应用。在这项工作中,制备了一种石墨相氮化碳(g-C₃N₄)负载的Cu₂O复合材料,在0.1 m KHCO₃电解液中,相对于可逆氢电极在-1.1 V时,该复合材料表现出32.2%的C₂H₄法拉第效率,其分电流密度为-4.3 mA cm⁻²。g-C₃N₄载体的引入不仅增强了Cu₂O纳米立方体的均匀分散性,还稳定了重要的CO中间体。此外,g-C₃N₄本身具有将CO还原形成CO的良好活性,这在氧化亚铜周围富集了C-C偶联的关键中间体。这些发现突出了g-C₃N₄载体这种独特二维材料的重要性,它不仅具有强大的CO吸附和活化能力,还在CO₂RR选择性方面与氧化亚铜具有协同效应。

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