In Situ Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy of Nickel-Catalyzed Hydrogenation Reactions.

Chemphyschem

Inorganic Chemistry and Catalysis Group Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.

Published: April 2020

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@SiO 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@SiO 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@SiO SHINs deposited on a Si wafer. These Ni/Au@SiO 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.

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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7187311PMC
http://dx.doi.org/10.1002/cphc.201901162DOI Listing

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