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Site-Independent Hydrogenation Reactions on Oxide-Supported Au Nanoparticles Facilitated by Intraparticle Hydrogen Atom Diffusion.
| Content Provider | Europe PMC |
|---|---|
| Author | Dery, Shahar Mehlman, Hillel Hale, Lillian Carmiel-Kostan, Mazal Yemini, Reut Ben-Tzvi, Tzipora Noked, Malachi Toste, F. Dean Gross, Elad |
| Copyright Year | 2021 |
| Abstract | Metal–supportinteractions have been widely utilized foroptimizing the catalytic reactivity of oxide-supported Au nanoparticles.Optimized reactivity was mainly detected with small (1–5 nm)oxide-supported Au nanoparticles and correlated to highly reactivesites at the oxide–metal interface. However, catalyticallyactive sites are not necessarily restricted to the interface but resideas well on the Au surface. Uncovering the interconnection betweenreactive sites located at the interface and those situated at themetal surface is of crucial importance for understanding the reactionmechanism on Au nanoparticles. Herein, high-spatial-resolution IRnanospectroscopy measurements were conducted to map the localizedreactivity in hydrogenation reactions on oxide-supported Au particleswhile using nitro-functionalized ligands as probes molecules. Comparativeanalysis of the reactivity pattern on single particles supported onvarious oxides revealed that oxide-dependent reactivity enhancementwas not limited to the oxide–metal interface but was detectedthroughout the Au particle, leading to site-independent reactivity.These results indicate that reactive Au sites on both the oxide–metalinterface and metal surface can activate the nitro groups toward hydrogenationreactions. The observed influence of oxide support (TiO2 > SiO2 > Al2O3) on the overallreactivity pattern specified that hydrogen dissociation occurred atthe oxide–metal interface, followed by highly efficient intraparticlehydrogen atom diffusion to the interior parts of the Au particle.In contrast to Au particles, the oxide–metal interface hadonly a minor impact on the reactivity of supported Pt particles inwhich hydrogen dissociation and nitro group reduction were effectivelyactivated on Pt sites. Single-particle measurements provided insightsinto the relative reactivity pattern of oxide-supported Au particles,revealing that the less-reactive Au metal sites can activate hydrogenationreactions in the presence of hydrogen atoms that diffuse from theAu/oxide boundary. |
| Related Links | https://europepmc.org/backend/ptpmcrender.fcgi?accid=PMC9223368&blobtype=pdf |
| Journal | ACS Catalysis [ACS Catal] |
| Volume Number | 11 |
| DOI | 10.1021/acscatal.1c01987 |
| PubMed Central reference number | PMC9223368 |
| Issue Number | 15 |
| PubMed reference number | 35756326 |
| e-ISSN | 21555435 |
| Language | English |
| Publisher | AmericanChemical Society |
| Publisher Date | 2021-07-21 |
| Access Restriction | Open |
| Rights License | Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). © 2021 American ChemicalSociety |
| Subject Keyword | metal−support interactions IR nanospectroscopy Au nanoparticles metaloxide hydrogenation single-particle measurements |
| Content Type | Text |
| Resource Type | Article |
| Subject | Chemistry Catalysis |
