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

Haixia Zhong, Mahdi Ghorbani-Asl, Khoa Hoang Ly, Jichao Zhang, Jin Ge, Mingchao Wang, Zhongquan Liao, Denys Makarov, Ehrenfried Zschech, Eike Brunner, Inez M. Weidinger, Jian Zhang, Arkady V. Krasheninnikov, Stefan Kaskel, Renhao Dong () and Xinliang Feng ()
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Haixia Zhong: Technische Universität Dresden
Mahdi Ghorbani-Asl: Institute of Ion Beam Physics and Materials Research
Khoa Hoang Ly: Technische Universität Dresden
Jichao Zhang: Chinese Academy of Sciences
Jin Ge: Institute of Ion Beam Physics and Materials Research
Mingchao Wang: Technische Universität Dresden
Zhongquan Liao: Fraunhofer Institute for Ceramic Technologies and Systems (IKTS)
Denys Makarov: Institute of Ion Beam Physics and Materials Research
Ehrenfried Zschech: Fraunhofer Institute for Ceramic Technologies and Systems (IKTS)
Eike Brunner: Technische Universität Dresden
Inez M. Weidinger: Technische Universität Dresden
Jian Zhang: Technische Universität Dresden
Arkady V. Krasheninnikov: Institute of Ion Beam Physics and Materials Research
Stefan Kaskel: Technische Universität Dresden
Renhao Dong: Technische Universität Dresden
Xinliang Feng: Technische Universität Dresden

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-15141-y

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