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, Xinliang Feng*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

59 Citations (Scopus)
184 Downloads (Pure)

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.

Original languageEnglish
Article number1409
Number of pages10
JournalNature Communications
Volume11
Issue number1
DOIs
Publication statusPublished - 16 Mar 2020
MoE publication typeA1 Journal article-refereed

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