Preparing uniform supported Pd-Ni catalysts with citrate-assisted impregnation

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-06-26 DOI:10.1016/j.jcat.2024.115624
Kristiaan H. Helfferich , Charles A. Fabrie , Johannes D. Meeldijk , George F. Tierney , Jessi E.S. van der Hoeven , Peter J. van den Brink , Krijn P. de Jong , Petra E. de Jongh
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Abstract

Bimetallic supported catalysts can show synergistic effects compared to their monometallic constituents. However, it is challenging to produce bimetallic catalysts with a uniform nanoparticle distribution over the support, while ensuring each nanoparticle contains both metals. A promising strategy is to use impregnation precursors that facilitate uniform distribution of both metals over a support. In this work, citrate-based precursors were studied to prepare bimetallic Pd-Ni nanoparticles supported on SBA-15 mesoporous silica. Amongst others, cryo-electron microscopy demonstrated the excellent distribution of Ni citrate precursor after drying. Co-impregnation with Ni citrate precursor and Pd(OAc)2 or Pd(NH3)4(NO3)2 produced well-distributed Pd-Ni nanoparticles with a narrow particle size distribution. Extensive characterization with STEM-EDX, EXAFS and TPR showed that the type of Pd precursor controlled the Pd to Ni nanoscale intimacy. CO2 hydrogenation experiments demonstrated that increasing Pd-Ni intimacy decreased the activity. Our strategy to produce uniform Pd-Ni nanoparticles using citric acid is relevant also for other bimetallic systems.

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用柠檬酸盐辅助浸渍法制备均匀的支撑钯镍催化剂
与单金属催化剂相比,双金属载体催化剂可以产生协同效应。然而,要生产出纳米颗粒在载体上均匀分布的双金属催化剂,同时确保每个纳米颗粒都含有两种金属,是一项挑战。一种可行的策略是使用浸渍前驱体,以促进两种金属在载体上的均匀分布。在这项工作中,研究人员使用柠檬酸盐类前驱体制备了支撑在 SBA-15 介孔二氧化硅上的双金属钯镍纳米粒子。其中,冷冻电镜显示柠檬酸镍前驱体在干燥后分布良好。柠檬酸镍前驱体与 Pd(OAc)2 或 Pd(NH3)4(NO3)2 共同浸渍后,生成的钯镍纳米粒子分布均匀,粒径分布较窄。利用 STEM-EDX、EXAFS 和 TPR 进行的广泛表征表明,钯前驱体的类型控制着钯与镍纳米尺度的亲密程度。二氧化碳氢化实验表明,Pd-Ni 亲密程度的增加会降低活性。我们利用柠檬酸生产均匀的钯镍纳米粒子的策略也适用于其他双金属系统。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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