Properties of PdAg/Al2O3 Egg–Shell Single-Atom Catalysts in Front-End Hydrogenation of Acetylene

IF 16.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Accounts of Chemical Research Pub Date : 2024-09-17 DOI:10.1134/s0965544124050165

I. S. Mashkovsky, P. V. Markov, G. N. Baeva, N. S. Smirnova, A. E. Vaulina, D. P. Mel’nikov, A. Yu. Stakheev

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Abstract

Two samples of PdAg/Al₂O₃ egg–shell single-atom catalysts, with Ag/Pd ratios of 1 : 1 and 3 : 1, were synthesized and characterized by TEM, XPS, and DRIFTS-CO methods. The formation of bimetallic PdAg alloy nanoparticles with single-atom Pd₁ active sites was demonstrated. Furthermore, a physicochemical characterization showed a egg–shell distribution of the active component. The catalytic performance of the samples was tested in front-end selective hydrogenation of acetylene. The H₂/C₂H₂ ratio in the model mixture was varied from 20 to 60. Under front-end acetylene hydrogenation conditions, the highest ethylene selectivity (about 87 at 90% acetylene conversion) was achieved in the presence of the Pd₁Ag₃/Al₂O₃ catalyst at H₂/C₂H₂ = 20. Finally, it was shown that, unlike the monometallic Pd catalyst, the Ag-promoted catalysts were completely free of any local thermal runaway effect.

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PdAg/Al2O3 蛋壳单原子催化剂在乙炔前端加氢反应中的特性

摘要采用 TEM、XPS 和 DRIFTS-CO 方法合成并表征了 Ag/Pd 比为 1 : 1 和 3 : 1 的两种 PdAg/Al2O3 蛋壳单原子催化剂样品。结果表明形成了具有单原子 Pd1 活性位点的双金属 PdAg 合金纳米颗粒。此外，理化表征显示活性成分呈蛋壳状分布。在乙炔的前端选择性氢化中测试了样品的催化性能。模型混合物中的 H2/C2H2 比率从 20 到 60 不等。在前端乙炔加氢条件下，当 H2/C2H2 = 20 时，Pd1Ag3/Al2O3 催化剂具有最高的乙烯选择性（乙炔转化率为 90% 时约为 87）。最后，研究表明，与单金属钯催化剂不同，Ag 促进催化剂完全不存在任何局部热失控效应。

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来源期刊

Accounts of Chemical Research 化学-化学综合

CiteScore

31.40

自引率

1.10%

发文量

312

审稿时长

2 months

期刊介绍： Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.