Dynamic Behavior of Platinum Atoms and Clusters in the Native Oxide Layer of Aluminum Nanocrystals

Robatjazi, Hossein; Battsengel, Tsatsral; Finzel, Jordan; Tieu, Peter; Xu, Mingjie; Hoffman, Adam S.; Qi, Ji; Bare, Simon R.; Pan, Xiaoqing; Chmelka, Bradley F.; Halas, Naomi J.; Christopher, Phillip

doi:10.1021/acsnano.3c12869

Dynamic Behavior of Platinum Atoms and Clusters in the Native Oxide Layer of Aluminum Nanocrystals

Journal Article · Tue Feb 13 00:00:00 EST 2024 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.3c12869· OSTI ID:2323394

^[1]; Battsengel, Tsatsral ^[2]; ^[2]; ^[3]; Xu, Mingjie ^[3]; ^[4]; Qi, Ji ^[2]; ^[4]; Pan, Xiaoqing ^[3]; Chmelka, Bradley F. ^[2]; ^[5]; ^[2]

University of California, Santa Barbara, CA (United States); Rice University, Houston, TX (United States); SLAC
University of California, Santa Barbara, CA (United States)
University of California, Irvine, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Rice University, Houston, TX (United States)

Strong metal–support interactions (SMSIs) are well-known in the field of heterogeneous catalysis to induce the encapsulation of platinum (Pt) group metals by oxide supports through high temperature H₂ reduction. However, demonstrations of SMSI overlayers have largely been limited to reducible oxides, such as TiO₂ and Nb₂O₅. In this report we show that the amorphous native surface oxide of plasmonic aluminum nanocrystals (AlNCs) exhibits SMSI-induced encapsulation of Pt following reduction in H₂ in a Pt structure dependent manner. Reductive treatment in H₂ at 300 °C induces the formation of an AlO_x SMSI overlayer on Pt clusters, leaving Pt single-atom sites (Ptiso) exposed available for catalysis. The remaining exposed Pt_iso species possess a more uniform local coordination environment than has been observed on other forms of Al₂O₃, suggesting that the AlO_x native oxide of AlNCs presents well-defined anchoring sites for individual Pt atoms. This observation extends our understanding of SMSIs by providing evidence that H₂-induced encapsulation can occur for a wider variety of materials and should stimulate expanded studies of this effect to include nonreducible oxides with oxygen defects and the presence of disorder. It also suggests that the single-atom sites created in this manner, when combined with the plasmonic properties of the Al nanocrystal core, may allow for site-specific single-atom plasmonic photocatalysis, providing dynamic control over the light-driven reactivity in these systems.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: Air Force Office of Scientific Research (AFOSR); Arnold O. and Mabel Beckman Foundation; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2323394

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 8 Vol. 18; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
aluminum nanocrystals
aluminum oxide
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Dynamic Behavior of Platinum Atoms and Clusters in the Native Oxide Layer of Aluminum Nanocrystals

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