Ultrathin two-dimensional mesoporous holmium oxide nanosheet-stabilized copper nanoparticles for stable and efficient electrocatalytic semi-hydrogenation of acetylene†

IF 6.4 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Inorganic Chemistry Frontiers Pub Date : 2025-02-11 DOI:10.1039/D4QI03125C
Huawei Li, Miao He, Senyao Meng, Ping Wang, Cheng Yang, Jiasai Yao, Zikang Hu and Zhenxing Li
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Abstract

The removal of acetylene (C2H2) impurities from ethylene (C2H4) is a critical step in the production of high-purity C2H4. Due to its low reaction temperature, low energy consumption and high selectivity for C2H4, the electrocatalytic semi-hydrogenation of C2H2 is an ideal method for removing C2H2. Herein, ultrathin two-dimensional (2D) mesoporous holmium oxide nanosheet-stabilized copper nanoparticles (Cu/Ho2O3) for stable and efficient electrocatalytic semi-hydrogenation of C2H2 were prepared through a simple and one-step high-temperature calcination-reduction method. The ultra-thin two-dimensional mesoporous structure of holmium oxide creates abundant coordination defects, improving the faradaic efficiency and durability of copper nanoparticles for catalyzing the semi-hydrogenation of C2H2. The as-prepared Cu/Ho2O3 achieved a C2H4 selectivity of 99.6% and a faradaic efficiency of 98.1% because the presence of oxygen vacancies is conducive to forming electron-rich Cu nanoparticles, thereby promoting the adsorption of electrophilic C2H2 and the desorption of nucleophilic C2H4. Meanwhile, the holmium oxide nanosheet with unsaturated coordination sites can stabilize the Cu nanoparticles, and the faradaic efficiency and current density remain stable for more than 600 minutes. This work offers a promising design strategy for a stable and efficient electrocatalyst for the semi-hydrogenation of C2H2 to C2H4.

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超薄二维介孔氧化钬纳米片稳定铜纳米粒子用于稳定高效的乙炔电催化半加氢反应
从乙烯(C2H4)中脱除乙炔(C2H2)是生产高纯度C2H4的关键步骤。由于反应温度低、能耗低、选择性高,电催化半加氢是脱除C2H2的理想方法。本文通过简单的一步高温煅烧-还原法制备了用于稳定高效电催化C2H2半加氢的超薄二维介孔氧化钬纳米片稳定铜纳米颗粒(Cu/Ho2O3)。氧化钬的超薄二维介孔结构产生了丰富的配位缺陷,提高了铜纳米粒子催化C2H2半加氢的法拉第效率和耐久性。制备的Cu/Ho2O3对C2H4的选择性达到99.6%,法拉第效率达到98.1%,这是因为氧空位的存在有利于形成富电子的Cu纳米颗粒,从而促进亲电性C2H2的吸附和亲核性C2H4的解吸。同时,具有不饱和配位的氧化钬纳米片可以稳定Cu纳米粒子,且法拉第效率和电流密度在600分钟以上保持稳定。本研究为制备稳定高效的C2H2 - C2H4半加氢反应电催化剂提供了一种有前景的设计策略。
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Copper nitrate trihydrate
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Holmium nitrate pentahydrate
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Potassium hydroxide
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Deionized water
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Ethanol
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Nafion
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来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
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