Revealing How Acid Sites Enhance the Electrocatalytic Glycerol Oxidation Performance on Pt Loaded Zeolite‐Carbon Composite Materials

IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Ju Ye Kim, Sunjae No, Jinwoo Hwang, Mi Yoo, Hakju Lee, Youngbi Kim, Youngmin Kim, Yong Tae Kim, Jeong‐Chul Kim, Jeong Woo Han, Kyoungsoo Kim, Hyung Ju Kim
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引用次数: 0

Abstract

The catalytic role and function of acid sites in solid acid catalysts, such as zeolites, are well understood in the context of heterogeneous catalytic reactions. But although many studies have highlighted the importance of acid sites, their catalytic effects in electrocatalytic reactions have rarely been investigated. In this work, a novel catalyst synthesis strategy is developed, integrating metal sites with acid sites for application in the electrocatalytic glycerol oxidation reaction (EGOR). Specifically, an ordered microporous carbon support containing acidic aluminum sites (AlYTC) is prepared through a nanocasting approach using a sacrificial zeolite template. Platinum (Pt) nanoclusters are then deposited onto the AlYTC support, forming a structure that exposes both acid sites and Pt nanoclusters on a zeolite‐templated 3D carbon framework (PtAlYTC). The prepared PtAlYTC catalyst demonstrates a turnover frequency (TOF, s−1) 30 times higher and a reaction rate () 17 times greater than those of a Pt catalyst lacking acid sites (PtYTC) in the EGOR. First‐principles density functional theory (DFT) calculations indicate that the combination of Pt sites and acidic Al sites lowers the Gibbs free energy of key reaction steps, improves charge transfer, and strengthens hydrogen adsorption, thereby significantly enhancing the catalytic performance in EGOR.
揭示酸位如何增强Pt负载沸石-碳复合材料电催化甘油氧化性能
固体酸催化剂(如沸石)中酸位的催化作用和功能在非均相催化反应中得到了很好的理解。但是,尽管许多研究都强调了酸位点的重要性,但它们在电催化反应中的催化作用却很少被研究。在这项工作中,开发了一种新的催化剂合成策略,将金属位点与酸位点相结合,用于电催化甘油氧化反应(EGOR)。具体而言,采用牺牲沸石模板,通过纳米铸造方法制备了含有酸性铝位的有序微孔碳载体(AlYTC)。然后将铂(Pt)纳米团簇沉积在AlYTC载体上,形成一种结构,将酸位和铂纳米团簇暴露在沸石模板3D碳框架(PtAlYTC)上。制备的PtAlYTC催化剂的转换频率(TOF, s−1)比EGOR中缺乏酸位的Pt催化剂(PtYTC)高30倍,反应速率()高17倍。第一性原理密度泛函数理论(DFT)计算表明,Pt位和酸性Al位的结合降低了关键反应步骤的吉布斯自由能,改善了电荷转移,加强了氢的吸附,从而显著提高了EGOR的催化性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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