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Electrokinetic and in situ spectroscopic investigations of CO electrochemical reduction on copper

Author

Listed:
  • Jing Li

    (Tsinghua University)

  • Xiaoxia Chang

    (University of Delaware)

  • Haochen Zhang

    (Tsinghua University)

  • Arnav S. Malkani

    (University of Delaware)

  • Mu-jeng Cheng

    (National Cheng Kung University)

  • Bingjun Xu

    (University of Delaware
    Peking University)

  • Qi Lu

    (Tsinghua University)

Abstract

Rigorous electrokinetic results are key to understanding the reaction mechanisms in the electrochemical CO reduction reaction (CORR), however, most reported results are compromised by the CO mass transport limitation. In this work, we determined mass transport-free CORR kinetics by employing a gas-diffusion type electrode and identified dependence of catalyst surface speciation on the electrolyte pH using in-situ surface enhanced vibrational spectroscopies. Based on the measured Tafel slopes and reaction orders, we demonstrate that the formation rates of C2+ products are most likely limited by the dimerization of CO adsorbate. CH4 production is limited by the CO hydrogenation step via a proton coupled electron transfer and a chemical hydrogenation step of CO by adsorbed hydrogen atom in weakly (7 11) alkaline electrolytes, respectively. Further, CH4 and C2+ products are likely formed on distinct types of active sites.

Suggested Citation

  • Jing Li & Xiaoxia Chang & Haochen Zhang & Arnav S. Malkani & Mu-jeng Cheng & Bingjun Xu & Qi Lu, 2021. "Electrokinetic and in situ spectroscopic investigations of CO electrochemical reduction on copper," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-23582-2
    DOI: 10.1038/s41467-021-23582-2
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    Cited by:

    1. Antonia Herzog & Mauricio Lopez Luna & Hyo Sang Jeon & Clara Rettenmaier & Philipp Grosse & Arno Bergmann & Beatriz Roldan Cuenya, 2024. "Operando Raman spectroscopy uncovers hydroxide and CO species enhance ethanol selectivity during pulsed CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Yan Lin & Tuo Wang & Lili Zhang & Gong Zhang & Lulu Li & Qingfeng Chang & Zifan Pang & Hui Gao & Kai Huang & Peng Zhang & Zhi-Jian Zhao & Chunlei Pei & Jinlong Gong, 2023. "Tunable CO2 electroreduction to ethanol and ethylene with controllable interfacial wettability," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Erfan Shirzadi & Qiu Jin & Ali Shayesteh Zeraati & Roham Dorakhan & Tiago J. Goncalves & Jehad Abed & Byoung-Hoon Lee & Armin Sedighian Rasouli & Joshua Wicks & Jinqiang Zhang & Pengfei Ou & Victor Bo, 2024. "Ligand-modified nanoparticle surfaces influence CO electroreduction selectivity," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. Jing Li & Haocheng Xiong & Xiaozhi Liu & Donghuan Wu & Dong Su & Bingjun Xu & Qi Lu, 2023. "Weak CO binding sites induced by Cu–Ag interfaces promote CO electroreduction to multi-carbon liquid products," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Siqi Zhao & Oliver Christensen & Zhaozong Sun & Hongqing Liang & Alexander Bagger & Kristian Torbensen & Pegah Nazari & Jeppe Vang Lauritsen & Steen Uttrup Pedersen & Jan Rossmeisl & Kim Daasbjerg, 2023. "Steering carbon dioxide reduction toward C–C coupling using copper electrodes modified with porous molecular films," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    6. Seung-Jae Shin & Hansol Choi & Stefan Ringe & Da Hye Won & Hyung-Suk Oh & Dong Hyun Kim & Taemin Lee & Dae-Hyun Nam & Hyungjun Kim & Chang Hyuck Choi, 2022. "A unifying mechanism for cation effect modulating C1 and C2 productions from CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    7. Wanyu Deng & Peng Zhang & Yu Qiao & Georg Kastlunger & Nitish Govindarajan & Aoni Xu & Ib Chorkendorff & Brian Seger & Jinlong Gong, 2024. "Unraveling the rate-determining step of C2+ products during electrochemical CO reduction," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    8. Jiajie Hou & Bingjun Xu & Qi Lu, 2024. "Influence of electric double layer rigidity on CO adsorption and electroreduction rate," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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