Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnOx Supports

Ostojic, Nevena; Duan, Zhiyao; Galyamova, Aigerim; Henkelman, Graeme; Crooks, Richard M.

doi:10.1021/jacs.8b08036

Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnO_x Supports

Journal Article · Fri Oct 12 00:00:00 EDT 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b08036· OSTI ID:1496830

Ostojic, Nevena ^[1]; Duan, Zhiyao ^[2]; Galyamova, Aigerim ^[2]; ^[2]; ^[2]

The Univ. of Texas at Austin, Austin, TX (United States); The University of Texas
The Univ. of Texas at Austin, Austin, TX (United States)

Here we report that density functional theory (DFT) can be used to accurately predict how Au nanoparticle (NP) catalysts cooperate with SnO_x (x = 1.9 or 2.0) supports to carry out the oxygen reduction reaction (ORR). Specifically, dendrimers were used to encapsulate AuNPs and prevent their interactions with the underlying SnO_x supports. After removal of the dendrimers, however, the AuNPs are brought into direct contact with the support and hence feel its effect. The results show that both SnO_1.9 and SnO_2.0 supports strongly enhance the electrocatalytic properties of AuNPs for the ORR. In the case of AuNP interaction with a SnO_1.9 support, the number of electrons involved in the ORR (n_eff) increases from 2.1 ± 0.2 to 2.9 ± 0.1 following removal of the dendrimers, indicating an increased preference for the desired four-electron product (water), while the overpotential decreases by 0.32 V. Similarly, direct interactions between AuNPs and a SnO_2.0 support result in an increase in n_eff from 2.2 ± 0.1 to 3.1 ± 0.1 and a reduction of the overpotential by 0.28 V. These experimental results are in excellent agreement with the theoretically predicted onset potential shift of 0.30 V. According to the DFT calculations, the observed activity enhancements are attributed to the existence of anionic Au resulting from electron transfer from surface oxygen vacancies within the SnO_x supports to the AuNPs. This theoretical finding was confirmed experimentally using X-ray photoelectron spectroscopy. Importantly, the calculations reported here were performed prior to the experiments. Furthermore, this study represents an unusual case of theory accurately predicting the electrocatalytic manifestation of strong metal support interactions.

View Accepted Manuscript (DOE)

Research Organization:: The Univ. of Texas at Austin, Austin, TX (United States); Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: Robert A. Welch Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0010576

OSTI ID:: 1496830

Alternate ID(s):: OSTI ID: 1617148

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 42 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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