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

Author

Listed:
  • 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
    Northwestern Polytechnical University)

  • Arkady V. Krasheninnikov

    (Institute of Ion Beam Physics and Materials Research
    Aalto University)

  • Stefan Kaskel

    (Technische Universität Dresden)

  • Renhao Dong

    (Technische Universität Dresden)

  • Xinliang Feng

    (Technische Universität Dresden)

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.

Suggested Citation

  • 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, 2020. "Synergistic electroreduction of carbon dioxide to carbon monoxide on bimetallic layered conjugated metal-organic frameworks," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-15141-y
    DOI: 10.1038/s41467-020-15141-y
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    Cited by:

    1. Chuanhui Huang & Xinglong Shang & Xinyuan Zhou & Zhe Zhang & Xing Huang & Yang Lu & Mingchao Wang & Markus Löffler & Zhongquan Liao & Haoyuan Qi & Ute Kaiser & Dana Schwarz & Andreas Fery & Tie Wang &, 2023. "Hierarchical conductive metal-organic framework films enabling efficient interfacial mass transfer," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Nannan Meng & Zhitan Wu & Yanmei Huang & Jie Zhang & Maoxin Chen & Haibin Ma & Hongjiao Li & Shibo Xi & Ming Lin & Wenya Wu & Shuhe Han & Yifu Yu & Quan-Hong Yang & Bin Zhang & Kian Ping Loh, 2024. "High yield electrosynthesis of oxygenates from CO using a relay Cu-Ag co-catalyst system," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Yu Zhang & Long-Zhang Dong & Shan Li & Xin Huang & Jia-Nan Chang & Jian-Hui Wang & Jie Zhou & Shun-Li Li & Ya-Qian Lan, 2021. "Coordination environment dependent selectivity of single-site-Cu enriched crystalline porous catalysts in CO2 reduction to CH4," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    4. Chen, Zhangsen & Zhang, Gaixia & Chen, Hangrong & Prakash, Jai & Zheng, Yi & Sun, Shuhui, 2022. "Multi-metallic catalysts for the electroreduction of carbon dioxide: Recent advances and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 155(C).
    5. Jiexin Zhu & Jiantao Li & Ruihu Lu & Ruohan Yu & Shiyong Zhao & Chengbo Li & Lei Lv & Lixue Xia & Xingbao Chen & Wenwei Cai & Jiashen Meng & Wei Zhang & Xuelei Pan & Xufeng Hong & Yuhang Dai & Yu Mao , 2023. "Surface passivation for highly active, selective, stable, and scalable CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    6. Yang Lu & Yingying Zhang & Chi-Yuan Yang & Sergio Revuelta & Haoyuan Qi & Chuanhui Huang & Wenlong Jin & Zichao Li & Victor Vega-Mayoral & Yannan Liu & Xing Huang & Darius Pohl & Miroslav Položij & Sh, 2022. "Precise tuning of interlayer electronic coupling in layered conductive metal-organic frameworks," Nature Communications, Nature, vol. 13(1), pages 1-7, December.

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