Synergistic electroreduction of carbon dioxide to carbon monoxide on bimetallic layered conjugated metal-organic frameworks

Zhong H, Ghorbani-Asl M, Ly KH, Zhang J, Ge J, Wang M, Liao Z, Makarov D, Zschech E, Brunner E, Weidinger IM, Zhang J, Krasheninnikov AV, Kaskel S, Dong R, Feng X (2020)

Publication Type: Journal article

Publication year: 2020

Journal

Nature Communications Nature Publishing Group: Nature Communications

Book Volume: 11

Article Number: 1409

Journal Issue: 1

DOI: 10.1038/s41467-020-15141-y

Abstract

Highly effective electrocatalysts promoting CO2 reduction reaction (CO2RR) is extremely desirable to produce value-added chemicals/fuels while addressing current environmental challenges. Herein, we develop a layer-stacked, bimetallic two-dimensional conjugated metal-organic framework (2D c-MOF) with copper-phthalocyanine as ligand (CuN4) and zinc-bis(dihydroxy) complex (ZnO4) as linkage (PcCu-O8-Zn). The PcCu-O8-Zn exhibits high CO selectivity of 88%, turnover frequency of 0.39 s−1 and long-term durability (>10 h), surpassing thus by far reported MOF-based electrocatalysts. The molar H2/CO ratio (1:7 to 4:1) can be tuned by varying metal centers and applied potential, making 2D c-MOFs highly relevant for syngas industry applications. The contrast experiments combined with operando spectroelectrochemistry and theoretical calculation unveil a synergistic catalytic mechanism; ZnO4 complexes act as CO2RR catalytic sites while CuN4 centers promote the protonation of adsorbed CO2 during CO2RR. This work offers a strategy on developing bimetallic MOF electrocatalysts for synergistically catalyzing CO2RR toward syngas synthesis.

Involved external institutions

Technische Universität Dresden DE Germany (DE) Helmholtz-Zentrum Dresden-Rossendorf (HZDR) DE Germany (DE) Chinese Academy of Sciences (CAS) / 中国科学院 CN China (CN) Fraunhofer-Institut für Keramische Technologien und Systeme (IKTS) DE Germany (DE)

How to cite

APA:

Zhong, H., Ghorbani-Asl, M., Ly, K.H., Zhang, J., Ge, J., Wang, M.,... Feng, X. (2020). Synergistic electroreduction of carbon dioxide to carbon monoxide on bimetallic layered conjugated metal-organic frameworks. Nature Communications, 11(1). https://doi.org/10.1038/s41467-020-15141-y

MLA:

Zhong, Haixia, et al. "Synergistic electroreduction of carbon dioxide to carbon monoxide on bimetallic layered conjugated metal-organic frameworks." Nature Communications 11.1 (2020).

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