Journal of Energy Chemistry ›› 2023, Vol. 85 ›› Issue (10): 102-107.DOI: 10.1016/j.jechem.2023.06.013

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Boosting C-C coupling to multicarbon products via high-pressure CO electroreduction

Wenqiang Yanga,b,1, Huan Liua,1, Yutai Qia, Yifan Lic, Yi Cuic, Liang Yua,b,*, Xiaoju Cuia,b,*, Dehui Denga,b,*   

  1. aState Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
    bUniversity of Chinese Academy of Sciences, Beijing 100049, China;
    cVacuum Interconnected Nanotech Workstation, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, Jiangsu, China
  • Received:2023-05-04 Revised:2023-06-09 Accepted:2023-06-11 Online:2023-10-15 Published:2023-11-06
  • Contact: *E-mail addresses: lyu@dicp.ac.cn (L. Yu), cuixiaoju@dicp.ac.cn (X. Cui), dhdeng@-dicp.ac.cn (D. Deng).
  • About author:1These authors contributed equally to this work.

Abstract: Electrochemical CO reduction reaction (CORR) provides a promising approach for producing valuable multicarbon products (C2+), while the low solubility of CO in aqueous solution and high energy barrier of C-C coupling as well as the competing hydrogen evolution reaction (HER) largely limit the efficiency for C2+ production in CORR. Here we report an overturn on the Faradaic efficiency of CORR from being HER-dominant to C2+ formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like Cu catalyst via pressuring CO. With the CO pressure rising from 1 to 40 atm, the C2+ Faradaic efficiency and partial current density remarkably increase from 22.8% and 18.9 mA cm-2 to 89.7% and 116.7 mA cm-2, respectively. Experimental and theoretical investigations reveal that high pressure-induced high CO coverage on metallic Cu surface weakens the Cu-C bond via reducing electron transfer from Cu to adsorbed CO and restrains hydrogen adsorption, which significantly facilitates the C-C coupling while suppressing HER on the predominant Cu(111) surface, thereby boosting the CO electroreduction to C2+ activity.

Key words: CO electroreduction, High pressure electrochemistry, Cu catalyst, C-C coupling, Multicarbon products