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基于M-SACs/Cu催化剂的CO串联电还原为C2+产物

Tandem Electroreduction of CO to C2+ Products Based on M-SACs/Cu Catalysts.

作者信息

He Qizhe, Li Ting-Ting

机构信息

School of Materials Science and Chemical Engineering, Ningbo University, Ningbo, 315211, China.

Key Laboratory of Advanced Mass Spectrometry and Molecular Analysis of Zhejiang Province, Ningbo University, Ningbo, 315211, China.

出版信息

Chemistry. 2025 Jan 14;31(3):e202403297. doi: 10.1002/chem.202403297. Epub 2024 Dec 12.

Abstract

Electrochemical CO reduction reaction (ECORR) is considered a highly promising method to produce high-value chemicals and fuels, contributing significantly the artificial carbon balance. Plenty catalysts can facilitate the conversion of CO into mono-carbon (C1) products. Among these catalysts, Cu species exhibit a distinct role in the formation of multi-carbon (C2+) products characterized by enhanced energy density. However, the limited selectivity of C2+ products, along with the inferior stability, and high overpotential demonstrated by single-component Cu catalysts, hinders their applicability in industrial-scale production. The implementation of a tandem strategy, which involves coupling the CO-to-CO pathway using Ag, Au, metal single-atom catalysts (M-SACs), etc., with the CO-to-C2+ conversion on Cu, represents a novel approach for the efficient generation of C2+ products. Given the high cost and restricted availability of noble metals, M-SACs have attracted substantial interest in tandem systems due to their cost-effectiveness and efficient atom utilization. The systematic analysis of the design principles and structure-activity relationship is essential for the advancement of M-SACs/Cu-based tandem catalysts. Here we first introduce various prevalent design strategies of M-SACs/Cu-based tandem catalysts for ECORR and then systematically summarize the latest advancements of M-SACs/Cu-based tandem system, encompassing metal-organic frameworks/Cu (MOFs/Cu), covalent organic frameworks/Cu (COFs/Cu), and nitrogen-doped carbon support transition metal single atomic materials/Cu (M-N-C/Cu). Lastly, we discuss the challenges and opportunities with the design and construction of M-SACs/Cu-based tandem catalysis for ECORR.

摘要

电化学CO还原反应(ECORR)被认为是一种极具前景的生产高价值化学品和燃料的方法,对人工碳平衡有重要贡献。大量催化剂可促进CO转化为单碳(C1)产物。在这些催化剂中,Cu物种在形成以能量密度增强为特征的多碳(C2+)产物方面发挥着独特作用。然而,C2+产物的选择性有限,以及单组分Cu催化剂表现出的稳定性差和过电位高,阻碍了它们在工业规模生产中的应用。实施串联策略,即将使用Ag、Au、金属单原子催化剂(M-SACs)等的CO到CO途径与Cu上的CO到C2+转化相耦合,代表了一种高效生成C2+产物的新方法。鉴于贵金属成本高且可用性受限,M-SACs因其成本效益和高效的原子利用率而在串联系统中引起了广泛关注。对M-SACs/Cu基串联催化剂的设计原则和结构-活性关系进行系统分析,对于其发展至关重要。在此,我们首先介绍用于ECORR的M-SACs/Cu基串联催化剂的各种普遍设计策略,然后系统总结M-SACs/Cu基串联系统的最新进展,包括金属有机框架/Cu(MOFs/Cu)、共价有机框架/Cu(COFs/Cu)以及氮掺杂碳负载过渡金属单原子材料/Cu(M-N-C/Cu)。最后,我们讨论了设计和构建用于ECORR 的M-SACs/Cu基串联催化的挑战和机遇。

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