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CO2-mediated organocatalytic chlorine evolution under industrial conditions

Author

Listed:
  • Jiarui Yang

    (Tsinghua University)

  • Wen-Hao Li

    (Tsinghua University)

  • Hai-Tao Tang

    (School of Chemistry and Pharmaceutical Sciences, Guangxi Normal University)

  • Ying-Ming Pan

    (School of Chemistry and Pharmaceutical Sciences, Guangxi Normal University)

  • Dingsheng Wang

    (Tsinghua University)

  • Yadong Li

    (Tsinghua University)

Abstract

During the chlor-alkali process, in operation since the nineteenth century, electrolysis of sodium chloride solutions generates chlorine and sodium hydroxide that are both important for chemical manufacturing1–4. As the process is very energy intensive, with 4% of globally produced electricity (about 150 TWh) going to the chlor-alkali industry5–8, even modest efficiency improvements can deliver substantial cost and energy savings. A particular focus in this regard is the demanding chlorine evolution reaction, for which the state-of-the-art electrocatalyst is still the dimensionally stable anode developed decades ago9–11. New catalysts for the chlorine evolution reaction have been reported12,13, but they still mainly consist of noble metal14–18. Here we show that an organocatalyst with an amide functional group enables the chlorine evolution reaction; and that in the presence of CO2, it achieves a current density of 10 kA m−2 and a selectivity of 99.6% at an overpotential of only 89 mV and thus rivals the dimensionally stable anode. We find that reversible binding of CO2 to the amide nitrogen facilitates formation of a radical species that plays a critical role in Cl2 generation, and that might also prove useful in the context of Cl− batteries and organic synthesis19–21. Although organocatalysts are typically not considered promising for demanding electrochemical applications, this work demonstrates their broader potential and the opportunities they offer for developing industrially relevant new processes and exploring new electrochemical mechanisms.

Suggested Citation

  • Jiarui Yang & Wen-Hao Li & Hai-Tao Tang & Ying-Ming Pan & Dingsheng Wang & Yadong Li, 2023. "CO2-mediated organocatalytic chlorine evolution under industrial conditions," Nature, Nature, vol. 617(7961), pages 519-523, May.
  • Handle: RePEc:nat:nature:v:617:y:2023:i:7961:d:10.1038_s41586-023-05886-z
    DOI: 10.1038/s41586-023-05886-z
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    Cited by:

    1. Wenting Feng & Xinru Wei & Jianhang Yang & Chenyu Ma & Yiming Sun & Junwei Han & Debin Kong & Linjie Zhi, 2024. "Iodine-induced self-depassivation strategy to improve reversible kinetics in Na-Cl2 battery," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Wenpeng Ni & Houjun Chen & Naizhuo Tang & Ting Hu & Wei Zhang & Yan Zhang & Shiguo Zhang, 2024. "High-purity ethylene production via indirect carbon dioxide electrochemical reduction," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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