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

Research output: Contribution to journalArticleScientificpeer-review

Researchers

  • 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

Research units

  • Technische Universität Dresden
  • Helmholtz-Zentrum Dresden-Rossendorf
  • Fraunhofer Institute for Ceramic Technologies and Systems
  • Northwestern Polytechnical University Xian
  • CAS - Shanghai Advanced Research Institute

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.

Details

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

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