In Situ Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy of Nickel-Catalyzed Hydrogenation Reactions
| Autor: | Wondergem, Caterina S., Kromwijk, Josepha J.G., Slagter, Mark, Vrijburg, Wilbert L., Hensen, Emiel J.M., Monai, Matteo, Vogt, Charlotte, Weckhuysen, Bert M., Sub Inorganic Chemistry and Catalysis, Inorganic Chemistry and Catalysis |
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| Přispěvatelé: | Sub Inorganic Chemistry and Catalysis, Inorganic Chemistry and Catalysis, Inorganic Materials & Catalysis, EIRES Chem. for Sustainable Energy Systems |
| Jazyk: | angličtina |
| Rok vydání: | 2020 |
| Předmět: |
Materials science
chemistry.chemical_element Nanoparticle 02 engineering and technology 010402 general chemistry Heterogeneous catalysis 01 natural sciences in situ spectroscopy Article Catalysis Metal symbols.namesake chemistry.chemical_compound nickel Transition metal Atomic and Molecular Physics Physical and Theoretical Chemistry SHINERS Articles 021001 nanoscience & nanotechnology Atomic and Molecular Physics and Optics 0104 chemical sciences Nickel heterogeneous catalysis chemistry Chemical engineering Acetylene visual_art Raman spectroscopy visual_art.visual_art_medium symbols and Optics 0210 nano-technology |
| Zdroj: | Chemphyschem ChemPhysChem, 21(7), 625. Wiley-VCH Verlag ChemPhysChem, 21(7), 625-632. Wiley-VCH Verlag |
| ISSN: | 1439-4235 |
| Popis: | Synthesis methods to prepare lower transition metal catalysts and specifically Ni for Shell‐Isolated Nanoparticle‐Enhanced Raman Spectroscopy (SHINERS) are explored. Impregnation, colloidal deposition, and spark ablation have been investigated as suitable synthesis routes to prepare SHINERS‐active Ni/Au@SiO2 catalyst/Shell‐Isolated Nanoparticles (SHINs). Ni precursors are confirmed to be notoriously difficult to reduce and the temperatures required are generally harsh enough to destroy SHINs, rendering SHINERS experiments on Ni infeasible using this approach. For colloidally synthesized Ni nanoparticles deposited on Au@SiO2 SHINs, stabilizing ligands first need to be removed before application is possible in catalysis. The required procedure results in transformation of the metallic Ni core to a fully oxidized metal nanoparticle, again too challenging to reduce at temperatures still compatible with SHINs. Finally, by use of spark ablation we were able to prepare metallic Ni catalysts directly on Au@SiO2 SHINs deposited on a Si wafer. These Ni/Au@SiO2 catalyst/SHINs were subsequently successfully probed with several molecules (i. e. CO and acetylene) of interest for heterogeneous catalysis, and we show that they could be used to study the in situ hydrogenation of acetylene. We observe the interaction of acetylene with the Ni surface. This study further illustrates the true potential of SHINERS by opening the door to studying industrially relevant reactions under in situ or operando reaction conditions. Sparking the reaction: Spark ablation is presented as a new method for the preparation of working lower transition metal catalysts supported on Shell‐Isolated Nanoparticle‐Enhanced Raman Spectroscopy (SHINERS)‐active Au@SiO2 nanoparticles. The gas phase hydrogenation of acetylene is studied with in situ SHINERS over the prepared Ni catalysts, reporting the first non‐noble metal catalysis study with SHINERS. |
| Databáze: | OpenAIRE |
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