Microenvironment regulation of copper sites by chelating hydrophobic polymer for electrosynthesis of ethylene

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters Pub Date : 2025-01-09 DOI:10.1016/j.cclet.2025.110836

Lei Zhang , Chenyang Kou , Kun Ni , Yiwen Chen , Tongchuan Zhang , Baoliang Zhang

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Abstract

Molecular catalysts can effectively steer the electrocatalytic acetylene semihydrogenation into ethylene, but realizing high Faradaic efficiency (FE) at industrial current densities remains a challenge. Herein, we report a ligand engineering strategy that utilizes polymeric N‑heterocyclic carbene (NHC) as a hydrophobic ligand to modulate the microenvironment of Cu sites. This polymeric NHC imparts appropriate hydrophobic properties for the chelated Cu sites, thereby moderating the H₂O transport and enabling easy access of acetylene. Consequently, the polymeric NHC chelated Cu exhibits an FE_ethylene of ∼97% at a current density of 500 mA/cm² in a flow cell. Particularly in a zero-gap reactor, the FE_ethylene consistently exceeds 86% across current densities from 100 mA/cm² to 400 mA/cm², reaching an optimal FE_ethylene of 98% at 200 mA/cm² and achieving durable operation for 155 h at 100 mA/cm². This work provides a promising paradigm to regulate the microenvironment of molecular catalysts for improving electrocatalytic performances under industrial current densities.

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通过螯合疏水聚合物调节用于乙烯电合成的铜位点微环境

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来源期刊

Chinese Chemical Letters 化学-化学综合

CiteScore

14.10

自引率

15.40%

发文量

8969

审稿时长

1.6 months

期刊介绍： Chinese Chemical Letters (CCL) (ISSN 1001-8417) was founded in July 1990. The journal publishes preliminary accounts in the whole field of chemistry, including inorganic chemistry, organic chemistry, analytical chemistry, physical chemistry, polymer chemistry, applied chemistry, etc.Chinese Chemical Letters does not accept articles previously published or scheduled to be published. To verify originality, your article may be checked by the originality detection service CrossCheck.