Unusual roles of ceria as the support of a single-atom catalyst in hydroisomerization of n-heptane: Phase boundary acts as transport channels between different active centers

IF 5.2 1区 化学 Q1 CHEMISTRY, APPLIED Journal of Rare Earths Pub Date : 2024-03-01 DOI:10.1016/j.jre.2024.02.020
Hao Qin, Hui Wan, Guofeng Guan
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Abstract

Hydroisomerization of n-alkanes plays an important role in fuel and lubricants processing. Bifunctional catalysts with ultralow platinum loading have recently been reported successively for hydroisomerisation. Herein, the catalysts were prepared successfully with different methods to improve the catalytic performance. The conversion of 0.01%Pt1@CeOx/SAPO-11 prepared by co-calcination method (0.01%Pt1@CS-c) is 71.4%, 25% higher than the other prepared by precipitation method. The turnover frequency per active surface platinum site (TOFPt) of 0.01%Pt1@CS-c is as high as 13115 h–1. Revealed by the X-ray photoelectron spectroscopy (XPS) results, the quality of phase boundary/intersurface between ceria and zeolite is found significantly different. The conjunction quality of phase boundary directly affects the spillover rate of intermediate species, which further leads to an apparent activity difference. In addition, the possible role of ceria in the reaction is discussed, rather than just as a carrier for the active metal atoms.
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铈在正庚烷加氢异构化过程中作为单原子催化剂载体的不寻常作用:相界充当不同活性中心之间的传输通道
正构烷烃的加氢异构化在燃料和润滑油加工中发挥着重要作用。近来,用于加氢异构化的超低铂载量双功能催化剂已被相继报道。本文采用不同的方法成功制备了催化剂,以提高催化性能。共煅烧法制备的 0.01%Pt1@CeOx/SAPO-11 的转化率为 71.4%,比沉淀法制备的转化率高 25%。0.01%Pt1@CS-c 每个活性表面铂位点的周转频率(TOFPt)高达 13115 h-1。X 射线光电子能谱(XPS)结果表明,铈与沸石之间的相界/内表面质量存在显著差异。相界的结合质量会直接影响中间物种的溢出率,从而进一步导致明显的活性差异。此外,还讨论了铈在反应中可能扮演的角色,而不仅仅是活性金属原子的载体。
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来源期刊
Journal of Rare Earths
Journal of Rare Earths 化学-应用化学
CiteScore
8.70
自引率
14.30%
发文量
374
审稿时长
1.7 months
期刊介绍: The Journal of Rare Earths reports studies on the 17 rare earth elements. It is a unique English-language learned journal that publishes works on various aspects of basic theory and applied science in the field of rare earths (RE). The journal accepts original high-quality original research papers and review articles with inventive content, and complete experimental data. It represents high academic standards and new progress in the RE field. Due to the advantage of abundant RE resources of China, the research on RE develops very actively, and papers on the latest progress in this field emerge every year. It is not only an important resource in which technicians publish and obtain their latest research results on RE, but also an important way of reflecting the updated progress in RE research field. The Journal of Rare Earths covers all research and application of RE rare earths including spectroscopy, luminescence and phosphors, rare earth catalysis, magnetism and magnetic materials, advanced rare earth materials, RE chemistry & hydrometallurgy, RE metallography & pyrometallurgy, RE new materials, RE solid state physics & solid state chemistry, rare earth applications, RE analysis & test, RE geology & ore dressing, etc.
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