Issue 7, 2019

Cathodized copper porphyrin metal–organic framework nanosheets for selective formate and acetate production from CO2 electroreduction

Abstract

An efficient and selective Cu catalyst for CO2 electroreduction is highly desirable since current catalysts suffer from poor selectivity towards a series of products, such as alkenes, alcohols, and carboxylic acids. Here, we used copper(II) paddle wheel cluster-based porphyrinic metal–organic framework (MOF) nanosheets for electrocatalytic CO2 reduction and compared them with CuO, Cu2O, Cu, a porphyrin–Cu(II) complex and a CuO/complex composite. Among them, the cathodized Cu-MOF nanosheets exhibit significant activity for formate production with a faradaic efficiency (FE) of 68.4% at a potential of −1.55 V versus Ag/Ag+. Moreover, the C–C coupling product acetate is generated from the same catalyst together with formate at a wide voltage range of −1.40 V to −1.65 V with the total liquid product FE from 38.8% to 85.2%. High selectivity and activity are closely related to the cathodized restructuring of Cu-MOF nanosheets. With the combination of X-ray diffraction, X-ray photoelectron spectroscopy, high resolution transmission electron microscopy and Fourier transform infrared spectroscopy, we find that Cu(II) carboxylate nodes possibly change to CuO, Cu2O and Cu4O3, which significantly catalyze CO2 to formate and acetate with synergistic enhancement from the porphyrin–Cu(II) complex. This intriguing phenomenon provides a new opportunity for the rational design of high-performance Cu catalysts from pre-designed MOFs.

Graphical abstract: Cathodized copper porphyrin metal–organic framework nanosheets for selective formate and acetate production from CO2 electroreduction

Supplementary files

Article information

Article type
Edge Article
Submitted
30 Sept. 2018
Accepted
14 Dec. 2018
First published
14 Dec. 2018
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2019,10, 2199-2205

Cathodized copper porphyrin metal–organic framework nanosheets for selective formate and acetate production from CO2 electroreduction

J. Wu, S. Hou, X. Zhang, M. Xu, H. Yang, P. Cao and Z. Gu, Chem. Sci., 2019, 10, 2199 DOI: 10.1039/C8SC04344B

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