Highly selective and low-overpotential electrocatalytic CO2 reduction to ethanol by Cu-single atoms decorated N-doped carbon dots

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-03 DOI:10.1016/j.apcatb.2024.123694

Rahul Purbia , Sung Yeol Choi , Chae Heon Woo , Jiho Jeon , Chulwan Lim , Dong Ki Lee , Jae Young Choi , Hyung-Suk Oh , Jeong Min Baik

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Abstract

Selective, low-overpotential and high Faradaic efficiency electroreduction of CO₂ to ethanol is in prominent global demand and lies in structuring, loading, and modulating the coordination states of Cu single atom catalysts (SACs) with support matrix. Here, the low-temperature (160 °C) synthesis of Cu–SACs–N-doped carbons dots (Cu–SACs–N–CQDs) is reported via Cu–dopamine complex process. The optimized Cu–SACs–N–CQDs electrocatalyst brings remarkably high Faraday efficiency (> 80%) and selectivity for ethanol with 50 h operation stability, which far exceeds previous results in terms of overpotential, stability, and Faraday efficiency. Surprisingly, the Faraday efficiency and selectivity of ethanol are highly sensitive to the coordination states of copper SACs with variation of Cu loadings. Operando X-ray absorption spectroscopy indicates in situ-generated neighboring metallic Cu–Cu atom coordination as real catalytic active sites from isolated single Cu atom during CO₂ reduction, which favors the ethanol selectivity.

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铜-单原子装饰的 N-掺杂碳点高选择性、低过电势电催化 CO2 还原成乙醇

将二氧化碳电还原成乙醇的选择性、低过电势和高法拉第效率是全球的突出需求，而这取决于铜单原子催化剂（SACs）与支撑基质的结构、负载和配位状态的调节。本文报告了通过铜-多巴胺复合物工艺低温（160°C）合成铜-SACs-N-掺杂碳点（Cu-SACs-N-CQDs）的过程。优化后的 Cu-SACs-N-CQDs 电催化剂具有极高的法拉第效率（80%）和对乙醇的选择性，并能稳定工作 50 小时，在过电位、稳定性和法拉第效率方面都远远超过了之前的研究成果。令人惊讶的是，随着铜负载量的变化，法拉第效率和对乙醇的选择性对铜 SAC 的配位状态非常敏感。操作X射线吸收光谱表明，在二氧化碳还原过程中，原位生成的邻近金属铜-铜原子配位是真正的催化活性位点，而不是孤立的单个铜原子，这有利于提高乙醇选择性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.