Electrocatalytic Acetylene Semi-Hydrogenation to Ethylene with High Energy Efficiency

Cong Dou, Yanmei Huang, Bohang Zhao, Weiwei Lei, Prof. Bin Zhang, Prof. Yifu Yu
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Abstract

Electrocatalytic acetylene semi-hydrogenation (EASH) provides a petroleum-independent strategy for ethylene production. However, the challenges of high overpotentials and strong hydrogen evolution competition reaction over conventional electrocatalysts at industrial current densities result in substantial energy consumption, limiting the practical application of EASH technology. Herein, zinc-doped copper catalysts are designed and prepared via a facile impregnation and electroreduction relay method. The as-prepared Cu-2.7Zn catalyst exhibits an ethylene partial current density of −0.29 A cm−2 with a Faradaic efficiency of 96 % and a reaction potential of −0.62 V versus reversible hydrogen electrode (RHE), surpassing the previously reported electrocatalysts. The combined results of experimental tests and theoretical calculations demonstrate zinc doping significantly enhances acetylene adsorption and accelerates reaction kinetics, leading to a notable decrease in overpotential. Furthermore, the increased *H-*H binding energy barrier and the improved ethylene desorption on Cu-2.7Zn effectively suppress hydrogen evolution and acetylene over-hydrogenation, contributing to the enhancement of ethylene Faradaic efficiency.

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高效电催化乙炔半加氢制乙烯
电催化乙炔半加氢(EASH)为乙烯生产提供了一种不依赖石油的策略。然而,在工业电流密度下,传统电催化剂面临高过电位和强氢进化竞争反应的挑战,导致大量能源消耗,限制了 EASH 技术的实际应用。本文设计并通过简便的浸渍和电还原接力法制备了掺锌铜催化剂。制备的 Cu-2.7Zn 催化剂的乙烯部分电流密度为 -0.29 A cm-2,法拉第效率为 96%,与可逆氢电极(RHE)的反应电位为 -0.62 V,超过了之前报道的电催化剂。实验测试和理论计算的综合结果表明,锌掺杂能显著增强对乙炔的吸附并加速反应动力学,从而显著降低过电位。此外,Cu-2.7Zn 上 *H-*H 结合能势垒的增加和乙烯解吸的改善有效地抑制了氢的演化和乙炔的过氢化,从而提高了乙烯的法拉第效率。
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来源期刊
Angewandte Chemie
Angewandte Chemie 化学科学, 有机化学, 有机合成
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