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

: Zhong, Haixia; Ghorbani-Asl, Mahdi; Ly, Khoa Hoang; Zhang, Jichao; Ge, Jin; Wang, Mingchao; Liao, Zhongquan; Makarov, Denys; Zschech, Ehrenfried; Brunner, Eike; Weidinger, Inez M.; Zhang, Jian; Krasheninnikov, Arkady V.; Kaskel, Stefan; Dong, Renhao; Feng, Xinliang

Fulltext ()

Nature Communications 11 (2020), Art. 1409, 10 pp.
ISSN: 2041-1723
European Commission EC
H2020; 785219; GrapheneCore2
Graphene Flagship Core Project 2
European Commission EC
H2020; 852909; FC2DMOF
Development of Functional Conjugated Two-Dimensional Metal-Organic Frameworks
Journal Article, Electronic Publication
Fraunhofer IKTS ()

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.