Highly Selective CO<sub>2</sub> Electroreduction to C<sub>2+</sub> Products over Cu<sub>2</sub>O-Decorated 2D Metal-Organic Frameworks with Rich Heterogeneous Interfaces.

Liu, Chang; Wang, Mingmin; Ye, Jinyu; Liu, Liangbin; Li, Leigang; Li, Yunhua; Huang, Xiaoqing · Nano Lett · 2023

basic_science · Level V

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Abstract

The electroreduction of carbon dioxide into high-value-added products is an effective approach to alleviating the energy crisis and pollution issues. However, there are still significant challenges for multicarbon (C<sub>2+</sub>) product production due to the lack of efficient catalysts with high selectivity. Herein, a Cu-rich electrocatalyst, where Cu<sub>2</sub>O nanoparticles are decorated on two-dimensional (2D) Cu-BDC metal-organic frameworks (MOFs) with abundant heterogeneous interfaces, is synthesized for highly selective CO<sub>2</sub> electroreduction into C<sub>2+</sub> products. A high C<sub>2+</sub> Faradaic efficiency of 72.1% in an H-type cell and 58.2% in a flow cell are obtained, respectively. The heterogeneous interfaces of Cu<sub>2</sub>O/Cu-BDC can optimize the adsorption energy of reaction intermediates during CO<sub>2</sub> electroreduction. An in situ infrared spectroscopy study indicates that the constructed interfaces can maintain the particular distribution of Cu valence states, where the C-C coupling is promoted to efficiently produce C<sub>2+</sub> products owing to the stabilization of *CHO and *COH intermediates.