电化学二氧化碳还原乙烯:从机理认识到催化剂表面工程

IF 31.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Nano-Micro Letters Pub Date : 2023-07-11 DOI:10.1007/s40820-023-01146-x
Junpeng Qu, Xianjun Cao, Li Gao, Jiayi Li, Lu Li, Yuhan Xie, Yufei Zhao, Jinqiang Zhang, Minghong Wu, Hao Liu
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引用次数: 1

摘要

电化学二氧化碳还原反应(CO2RR)是一种很有前途的将二氧化碳转化为化学物质的方法。多碳(C2+)产品,特别是乙烯,由于其广泛的工业应用而引起了人们的极大兴趣。然而,选择性地将CO2还原为乙烯仍然具有挑战性,因为C-C耦合步骤所需的额外能量会导致过大的过电位和许多竞争产物。尽管如此,对关键步骤和首选反应途径/条件的机理理解,以及合理设计用于乙烯生产的新型催化剂,被认为是实现高效和选择性CO2RR的有希望的方法。在这篇综述中,我们首先阐述了CO2RR制乙烯的关键步骤(如CO2吸附/活化,*CO中间体的形成,C-C偶联步骤),提供了CO2RR制乙烯的机理认识。然后研究了乙烯和竞争产物(C1和其他C2+产物)生成的替代反应途径和条件,指导进一步设计和开发乙烯生成的优选条件。进一步总结了cu基co2rr -乙烯催化剂的工程策略,并阐述了反应机理/途径、工程策略与选择性之间的关系。最后,对CO2RR研究领域的未来发展和实际应用提出了主要挑战和展望。
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Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Electrochemical carbon dioxide reduction reaction (CO2RR) provides a promising way to convert CO2 to chemicals. The multicarbon (C2+) products, especially ethylene, are of great interest due to their versatile industrial applications. However, selectively reducing CO2 to ethylene is still challenging as the additional energy required for the C–C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding of the key steps and preferred reaction pathways/conditions, as well as rational design of novel catalysts for ethylene production have been regarded as promising approaches to achieving the highly efficient and selective CO2RR. In this review, we first illustrate the key steps for CO2RR to ethylene (e.g., CO2 adsorption/activation, formation of *CO intermediate, C–C coupling step), offering mechanistic understanding of CO2RR conversion to ethylene. Then the alternative reaction pathways and conditions for the formation of ethylene and competitive products (C1 and other C2+ products) are investigated, guiding the further design and development of preferred conditions for ethylene generation. Engineering strategies of Cu-based catalysts for CO2RR-ethylene are further summarized, and the correlations of reaction mechanism/pathways, engineering strategies and selectivity are elaborated. Finally, major challenges and perspectives in the research area of CO2RR are proposed for future development and practical applications.

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来源期刊
Nano-Micro Letters
Nano-Micro Letters NANOSCIENCE & NANOTECHNOLOGY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
42.40
自引率
4.90%
发文量
715
审稿时长
13 weeks
期刊介绍: Nano-Micro Letters is a peer-reviewed, international, interdisciplinary and open-access journal that focus on science, experiments, engineering, technologies and applications of nano- or microscale structure and system in physics, chemistry, biology, material science, pharmacy and their expanding interfaces with at least one dimension ranging from a few sub-nanometers to a few hundreds of micrometers. Especially, emphasize the bottom-up approach in the length scale from nano to micro since the key for nanotechnology to reach industrial applications is to assemble, to modify, and to control nanostructure in micro scale. The aim is to provide a publishing platform crossing the boundaries, from nano to micro, and from science to technologies.
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