Catalytic activity of gold-perovskite catalysts in the oxidation of carbon monoxide

IF 2.2 4区 工程技术 Q2 Chemistry Gold Bulletin Pub Date : 2016-07-06 DOI:10.1007/s13404-016-0180-x
Leboheng Mokoena, Gary Pattrick, Mike S Scurrell
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引用次数: 7

Abstract

Perovskites (ABO3 structures), which can be manipulated by partial substitution, are reported to be active supports for CO oxidation, but only at high temperatures, with no activity being shown for temperatures below 200?°C. In this study, these perovskites were investigated at low temperatures (below 100?°C) with improved activity found upon gold deposition. The presence of gold nanoparticles therefore significantly enhanced the catalytic activity, while the support itself was suspected to be involved in the reaction mechanism. A series of perovskites of the type ABO3 (LaMnO3, LaFeO3, LaCoO3, and LaCuO3) were prepared using the citrate method, while the gold was deposited on them using the deposition-precipitation method. The supports were calcined at different temperatures for optimization. With the support calcined at 800?°C, the best catalyst was 1?wt% Au supported on LaFeO3. Calcium-doping of this system showed decreased surface area, poorer crystallinity, and a drop in catalytic activity relative to the Au-LaFeO3. In addition, Au-LaFeO3 showed online stability over 21?h. Calcining the support improved the incorporation of gold nanoparticles into the perovskite lattice, resulting in superior catalytic activity. Nevertheless, at higher calcination temperatures, the catalytic activity of Au-CaTiO3 was depressed while that of Au-LaFeO3 was enhanced. XPS revealed that in the active catalysts, both cationic and metallic gold coexisted, while in the inactive catalysts, the gold existed predominantly either as cationic or metallic gold.

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金-钙钛矿催化剂在一氧化碳氧化中的催化活性
据报道,钙钛矿(ABO3结构)可以通过部分取代来控制,是CO氧化的活性载体,但仅在高温下,在低于200°C的温度下没有活性。在这项研究中,这些钙钛矿在低温(低于100°C)下进行了研究,发现金沉积后活性有所提高。因此,金纳米颗粒的存在显著增强了催化活性,而载体本身也被怀疑参与了反应机理。采用柠檬酸盐法制备了一系列ABO3型钙钛矿(LaMnO3、LaFeO3、LaCoO3和LaCuO3),并采用沉积-沉淀法在其上沉积金。在不同的温度下对支架进行了煅烧,以进行优化。在800度的高温下?℃时,最佳催化剂为1?LaFeO3支持wt% Au。与Au-LaFeO3相比,钙掺杂的体系表面积减小,结晶度差,催化活性下降。此外,Au-LaFeO3在21 h内表现出在线稳定性。煅烧载体改善了金纳米颗粒在钙钛矿晶格中的掺入,从而产生了优异的催化活性。然而,在较高的煅烧温度下,Au-CaTiO3的催化活性降低,而Au-LaFeO3的催化活性增强。XPS结果表明,在活性催化剂中,阳离子金和金属金同时存在,而在非活性催化剂中,金主要以阳离子金和金属金的形式存在。
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来源期刊
Gold Bulletin
Gold Bulletin 工程技术-材料科学:综合
CiteScore
3.30
自引率
4.50%
发文量
0
审稿时长
3 months
期刊介绍: Gold Bulletin is the premier international peer reviewed journal on the latest science, technology and applications of gold. It includes papers on the latest research advances, state-of-the-art reviews, conference reports, book reviews and highlights of patents and scientific literature. Gold Bulletin does not publish manuscripts covering the snthesis of Gold nanoparticles in the presence of plant extracts or other nature-derived extracts. Gold Bulletin has been published over 40 years as a multidisciplinary journal read by chemists, physicists, engineers, metallurgists, materials scientists, biotechnologists, surface scientists, and nanotechnologists amongst others, both within industry and academia. Gold Bulletin is published in Association with the World Gold Council.
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