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One-Step Electrochemical Ethylene-to-Ethylene Glycol Conversion over a Multitasking Molecular Catalyst

  • An Zhen Li
  • , Bo Jun Yuan
  • , Ming Xu
  • , Ye Wang
  • , Chunyu Zhang
  • , Xiongbo Wang
  • , Xi Wang
  • , Jing Li
  • , Lirong Zheng
  • , Bi Jie Li*
  • , Haohong Duan*
  • *此作品的通讯作者
  • Tsinghua University
  • Beijing University of Chemical Technology
  • CAS - Institute of High Energy Physics
  • Haihe Laboratory of Sustainable Chemical Transformations

科研成果: 期刊稿件文章同行评审

摘要

Ethylene glycol is an essential commodity chemical with high demand, which is conventionally produced via thermocatalytic oxidation of ethylene with huge fossil fuel consumption and CO2 emission. The one-step electrochemical approach offers a sustainable route but suffers from reliance on noble metal catalysts, low activity, and mediocre selectivity. Herein, we report a one-step electrochemical oxidation of ethylene to ethylene glycol over an earth-abundant metal-based molecular catalyst, a cobalt phthalocyanine supported on a carbon nanotube (CoPc/CNT). The catalyst delivers ethylene glycol with 100% selectivity and 1.78 min-1 turnover frequency at room temperature and ambient pressure, more competitive than those obtained over palladium catalysts. Experimental data demonstrate that the catalyst orchestrates multiple tasks in sequence, involving electrochemical water activation to generate high-valence Co-oxo species, ethylene epoxidation to afford an ethylene oxide intermediate via oxygen transfer, and eventually ring-opening of ethylene oxide to ethylene glycol facilitated by in situ formed Lewis acid site. This work offers a great opportunity for commodity chemicals synthesis based on a one-step, earth-abundant metal-catalyzed, and renewable electricity-driven route.

源语言英语
页(从-至)5622-5633
页数12
期刊Journal of the American Chemical Society
146
8
DOI
出版状态已出版 - 28 2月 2024
已对外发布

联合国可持续发展目标

此成果有助于实现下列可持续发展目标:

  1. 可持续发展目标 7 - 经济适用的清洁能源
    可持续发展目标 7 经济适用的清洁能源

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