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
{"title":"用柠檬酸盐辅助浸渍法制备均匀的支撑钯镍催化剂","authors":"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","doi":"10.1016/j.jcat.2024.115624","DOIUrl":null,"url":null,"abstract":"<div><p>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)<sub>2</sub> or Pd(NH<sub>3</sub>)<sub>4</sub>(NO<sub>3</sub>)<sub>2</sub> 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. CO<sub>2</sub> 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.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0021951724003373/pdfft?md5=dfd2af5b2b8d5c60d606e25629936f9f&pid=1-s2.0-S0021951724003373-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Preparing uniform supported Pd-Ni catalysts with citrate-assisted impregnation\",\"authors\":\"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\",\"doi\":\"10.1016/j.jcat.2024.115624\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>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)<sub>2</sub> or Pd(NH<sub>3</sub>)<sub>4</sub>(NO<sub>3</sub>)<sub>2</sub> 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. CO<sub>2</sub> 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.</p></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-06-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0021951724003373/pdfft?md5=dfd2af5b2b8d5c60d606e25629936f9f&pid=1-s2.0-S0021951724003373-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951724003373\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951724003373","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Preparing uniform supported Pd-Ni catalysts with citrate-assisted impregnation
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.
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.