Hydrogen migration at restructuring palladium–silver oxide boundaries dramatically enhances reduction rate of silver oxide

O’Connor, Christopher R.; van Spronsen, Matthijs A.; Egle, Tobias; Xu, Fang; Kersell, Heath R.; Oliver-Meseguer, Judit; Karatok, Mustafa; Salmeron, Miquel; Madix, Robert J.; Friend, Cynthia M.

doi:10.1038/s41467-020-15536-x

Title: Hydrogen migration at restructuring palladium–silver oxide boundaries dramatically enhances reduction rate of silver oxide

Journal Article · Wed Apr 15 00:00:00 EDT 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-15536-x· OSTI ID:1695723

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^[1]; Kersell, Heath R. ^[3]; Oliver-Meseguer, Judit ^[3];

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^[4]; Madix, Robert J. ^[1];

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Harvard Univ., Cambridge, MA (United States)
Harvard Univ., Cambridge, MA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Heterogeneous catalysts are complex materials with multiple interfaces. A critical proposition in exploiting bifunctionality in alloy catalysts is to achieve surface migration across interfaces separating functionally dissimilar regions. Herein, we demonstrate the enhancement of more than 10⁴ in the rate of molecular hydrogen reduction of a silver surface oxide in the presence of palladium oxide compared to pure silver oxide resulting from the transfer of atomic hydrogen from palladium oxide islands onto the surrounding surface formed from oxidation of a palladium-silver alloy. The palladium-silver interface also dynamically restructures during reduction, resulting in silver-palladium intermixing. This study clearly demonstrates the migration of reaction intermediates and catalyst material across surface interfacial boundaries in alloys with a significant effect on surface reactivity, having broad implications for the catalytic function of bimetallic materials.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Harvard Univ., Cambridge, MA (United States)

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

Grant/Contract Number:: AC02-05CH11231; SC0012573

OSTI ID:: 1695723

Alternate ID(s):: OSTI ID: 1843584

Journal Information:: Nature Communications, Vol. 11, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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