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 |
| 卷 | 146 |
| 期 | 8 |
| DOI | |
| 出版状态 | 已出版 - 28 2月 2024 |
| 已对外发布 | 是 |
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:
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可持续发展目标 7 经济适用的清洁能源
学术指纹
探究 'One-Step Electrochemical Ethylene-to-Ethylene Glycol Conversion over a Multitasking Molecular Catalyst' 的科研主题。它们共同构成独一无二的学术指纹。引用此
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