Building Random Alloy Surfaces from Intermetallic Seeds: A General Route to Strain-Engineered Electrocatalysts with High Durability

Gamler, Jocelyn T.  L.; Ashberry, Hannah M.; Sang, Xiahan; Unocic, Raymond R.; Skrabalak, Sara E.

doi:10.1021/acsanm.9b00901

Title: Building Random Alloy Surfaces from Intermetallic Seeds: A General Route to Strain-Engineered Electrocatalysts with High Durability

Journal Article · 27 June 2019 · ACS Applied Nano Materials

DOI: https://doi.org/10.1021/acsanm.9b00901 · OSTI ID:1564157

Gamler, Jocelyn T. L. ^[1]; Ashberry, Hannah M. ^[1];

^[2];

^[1]

Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences

Pt-based catalysts are common in fuel cells but suffer from high cost and poor durability. To overcome these limitations, earth-abundant metals are often incorporated with Pt in core@shell architectures or through alloy formation. In this work, the concepts of a core@shell architecture, alloyed surfaces, and high-durability intermetallics are integrated into one nanostructure platform using seed-mediated co-reduction (SMCR). Specifically, random alloy PtM (where M = Ni, Co, Cu, or Fe) shells are deposited on intermetallic PdCu B2 seeds. Control of shell thickness and Pt:M ratios is also demonstrated, providing a general route to strain-engineered alloyed surfaces. The performance of these nanocatalysts was evaluated for the oxygen reduction reaction (ORR) as a function of shell thickness and shell composition, where PtCu and PtNi shells showed a 230% and 270% activity increase, respectively, compared to the Pt reference. This evaluation is coupled with Tafel plot analysis which shows significant changes in the Tafel slopes, which indicate a shift in the rate-limiting step when a core@shell architecture is incorporated. Significantly, this work demonstrates the versatility of SMCR as a facile way to integrate a core@shell architecture, alloyed surfaces, and high-durability intermetallics within one platform.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Indiana Univ., Bloomington, IN (United States)

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

Grant/Contract Number:: AC05-00OR22725; SC0018961

OSTI ID:: 1564157

Alternate ID(s):: OSTI ID: 1659487

Journal Information:: ACS Applied Nano Materials, Vol. 2, Issue 7; ISSN 2574-0970

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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