Enhancing CO Oxidation Activity via Tuning a Charge Transfer Between Gold Nanoparticles and Supports

Yang, Haotian; Cen, Jiajie; Wu, Qiyuan; Ridge, Claron J.; Tong, Xiao; Zhou, Chenyu; Veerasamy, Vijayen; Su, Dong; Lindsay, C. Michael; Liu, Mingzhao; Orlov, Alexander

doi:10.1021/acs.jpcc.1c10072

Title: Enhancing CO Oxidation Activity via Tuning a Charge Transfer Between Gold Nanoparticles and Supports

Journal Article · Tue Mar 08 00:00:00 EST 2022 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c10072· OSTI ID:1870396

^[1]; Cen, Jiajie ^[1];

^[2]; Ridge, Claron J. ^[3]; Tong, Xiao ^[4];

^[5]; Veerasamy, Vijayen ^[1];

^[6]; Lindsay, C. Michael ^[3];

^[4]; Orlov, Alexander ^[1]

Stony Brook Univ., NY (United States)
Stony Brook Univ., NY (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Air Force Research Lab. (AFRL), Eglin Air Force Base, FL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Chinese Academy of Sciences (CAS), Beijing (China)

Charge transfer from the supports to nanoparticles at the interface is one of the key factors to determine the catalytic performances of supported nanoparticles. In this work, we revealed that the charge transfer from semiconductor support to Au nanoparticle catalysts enhanced their activity toward CO oxidation. In this work, a novel Au/SiO₂/Si composite system with precisely controllable SiO₂ layer thickness was fabricated to tune the magnitude of interfacial charge transfer. With the support of X-ray photoelectron spectroscopy and numerical simulations, it was demonstrated that the Schottoky barrier formed across the Au/SiO₂/Si heterojunction led to negative charge accumulation at the surface of Au nanoparticles, which may be transferred to the antibonding orbitral of adsorbed O₂ molecules to the O-O bonds. This discovery highlights a new perspective in explaining the role of strong metal-support interactions for catalytic reactions and provides a fresh path for designing the next generation of nanocatalysts.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; 2015275

OSTI ID:: 1870396

Report Number(s):: BNL-223029-2022-JAAM

Journal Information:: Journal of Physical Chemistry. C, Vol. 126, Issue 10; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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