Citation: Lei Zhang, Chenyang Kou, Kun Ni, Yiwen Chen, Tongchuan Zhang, Baoliang Zhang. Microenvironment regulation of copper sites by chelating hydrophobic polymer for electrosynthesis of ethylene[J]. Chinese Chemical Letters, ;2025, 36(6): 110836. doi: 10.1016/j.cclet.2025.110836 shu

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

Lei Zhang ^{a, b, *,} ,
Chenyang Kou ^a ,
Kun Ni ^a ,
Yiwen Chen ^c ,
Tongchuan Zhang ^a ,
Baoliang Zhang ^{a, *,}

a.
School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi'an 710129, China
b.
Research & Development Institute of Northwestern Polytechnical University in Shenzhen, Shenzhen 518063, China
c.
Queen Mary University of London Engineering School, Northwestern Polytechnical University, Xi'an 710129, China

leizhang@nwpu.edu.cn

blzhang@nwpu.edu.cn

Received Date: 24 November 2024
Revised Date: 8 January 2025
Accepted Date: 8 January 2025
Available Online: 9 January 2025

Figures(4)

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.
- Molecular catalyst,
- Microenvironment regulation,
- Electrocatalytic acetylene semihydrogenation,
- Faradaic efficiency
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