Electrocatalytic Acetylene Semi-Hydrogenation to Ethylene with High Energy Efficiency

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-02-15 DOI:10.1002/anie.202423381
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(ash)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,与传统电催化剂相比,高过电位和强析氢竞争反应的挑战导致了大量的能量消耗,限制了ash技术的实际应用。本文设计并制备了锌掺杂铜催化剂,采用易浸渍和电还原接力法。制备的Cu‐2.7Zn催化剂的乙烯分电流密度为−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相结合的结果表明,锌掺杂显著增强了乙炔吸附,加速了反应动力学,导致过电位显著降低。此外,增加的*H - *H结合能垒和改善的Cu‐2.7Zn上的乙烯解吸有效地抑制了析氢和乙炔的过加氢,有助于提高乙烯的法拉第效率。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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