Bond Selective Photochemistry at Metal Nanoparticle Surfaces: CO Desorption from Pt and Pd

Barraza Alvarez, Isabel; Le, Tien; Hosseini, Hajar; Samira, Samji; Beck, Arik; Marlowe, Justin; Montemore, Matthew M.; Wang, Bin; Christopher, Phillip

doi:10.1021/jacs.3c13874

Title: Bond Selective Photochemistry at Metal Nanoparticle Surfaces: CO Desorption from Pt and Pd

Journal Article · 25 April 2024 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.3c13874 · OSTI ID:2350681

Barraza Alvarez, Isabel ^[1];

^[2]; Hosseini, Hajar ^[3];

^[4];

^[4]; Marlowe, Justin ^[4];

^[3];

^[2];

^[4]

Univ. of California, Santa Barbara, CA (United States); University of California Santa Barbara
Univ. of Oklahoma, Norman, OK (United States)
Tulane Univ., New Orleans, LA (United States)
Univ. of California, Santa Barbara, CA (United States)

The use of visible photon fluxes to influence catalytic reactions on metal nanoparticle surfaces has attracted attention based on observations of reaction mechanisms and selectivity not observed under equilibrium heating. These observations suggest that photon fluxes can selectively impact the rates of certain elementary steps, creating non-equilibrium energy distributions among various reaction pathways. However, quantitative studies validating these hypotheses on metal nanoparticle surfaces are lacking. Here we examine the influence of continuous wave visible photon fluxes on CO desorption rates from 1-2 nm diameter Pt and Pd nanoparticle surfaces supported on γ-Al₂O₃. Temperature programmed desorption (TPD) measurements quantified via diffuse reflectance infrared Fourier transform spectroscopy demonstrate that visible photon fluxes significantly enhanced the CO desorption rate from Pt nanoparticles in a wavelength dependent manner. 440 nm photons most efficiently promoted CO desorption from Pt nanoparticle surfaces, aligning with the excitation energy for the interfacial electronic transition within the Pt-CO bond. Conversely, visible photon fluxes had no measurable influence on CO desorption rates from Pd nanoparticle surfaces after accounting for photon induced heating. Density Functional Theory calculations demonstrate that the Pt-CO bond exhibits a narrower LUMO resonance, stronger coupling between the photoexcitation and forces induced on the metal-C bond, and vibrational energy dissipation that more effectively couples to desorption as compared to Pd-CO. These results demonstrate the specificity photons provide in facilitating chemical processes on metal nanoparticle surfaces and substantiate the idea that photon fluxes can be used to steer processes and outcomes of catalytic reactions in ways not achievable by equilibrium heating.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Programmable Energy Catalysis (CPEC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); US Army Research Office (ARO)

Grant/Contract Number:: SC0023464; SC0020300

OSTI ID:: 2350681

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 18 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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