Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO2 : Stable Au-Based Oxidation Catalysts

Luneau, Mathilde; Shirman, Tanya; Filie, Amanda; Timoshenko, Janis; Chen, Wei; Trimpalis, Antonios; Flytzani-Stephanopoulos, Maria; Kaxiras, Efthimios; Frenkel, Anatoly I.; Aizenberg, Joanna; Friend, Cynthia M.; Madix, Robert J.

doi:10.1021/acs.chemmater.9b01779

Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO₂ : Stable Au-Based Oxidation Catalysts

Journal Article · Wed Jul 10 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b01779· OSTI ID:1560004

Luneau, Mathilde ^[1]; Shirman, Tanya ^[1]; Filie, Amanda ^[1]; Timoshenko, Janis ^[2]; ^[1]; Trimpalis, Antonios ^[3]; Flytzani-Stephanopoulos, Maria ^[3]; Kaxiras, Efthimios ^[1]; ^[4]; Aizenberg, Joanna ^[1]; ;

Harvard Univ., Cambridge, MA (United States)
Stony Brook Univ., NY (United States)
Tufts Univ., Medford, MA (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Dilute alloy materials hold great promise for enhancing selectivity in catalytic reactions. A major challenge with such catalytic materials is developing supported alloy nanoparticles (NPs) with a catalytically optimal composition that are stable with respect to sintering. Here, we demonstrate that NP Pd/Au catalysts with minor concentrations of Pd prepared by a colloid-templating approach are active for oxygen dissociation and catalytic oxidation, as exemplified by CO oxidation. Using electron microscopic imaging, infrared spectroscopy, and X-ray photoelectron spectroscopy, we demonstrate that Pd is stabilized within the Au nanoparticle in its metallic state with minor amounts of Pd at the surface. The Pd–Au nanoparticles are embedded in the colloidally templated silica and form a thermally stable catalyst at high temperature. Surface analysis by diffuse reflectance infrared spectroscopy indicates that the Pd atomic distribution at the surface varies with the bulk concentration, forming isolated Pd atoms at 2% Pd and a mixture of Pd monomers and small Pd clusters at 9% Pd. X-ray absorption fine structure analysis indicates that Pd is well distributed in the bulk of the nanoparticle. In conclusion, in-depth understanding of this new class of catalytic materials opens the way to a wide array of possibilities for crucial enhancement of activity and selectivity in catalysis.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1560004

Report Number(s):: BNL--212061-2019-JAAM

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 15 Vol. 31; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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