Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method

Lapp, Aliya S.; Duan, Zhiyao; Marcella, Nicholas; Luo, Long; Genc, Arda; Ringnalda, Jan; Frenkel, Anatoly I.; Henkelman, Graeme; Crooks, Richard M.

doi:10.1021/jacs.7b12306

Title: Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method

Journal Article · Fri May 11 00:00:00 EDT 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b12306· OSTI ID:1436448

Lapp, Aliya S. ^[1]; Duan, Zhiyao ^[2];

^[3];

^[4]; Genc, Arda ^[5]; Ringnalda, Jan ^[5];

^[3];

^[2];

^[1]

Univ. of Texas, Austin, TX (United States). Texas Materials Inst., and Dept. of Chemistry
Univ. of Texas, Austin, TX (United States). Inst. for Computational and Engineering Sciences, and Dept. of Chemistry
Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
Univ. of Texas, Austin, TX (United States). Texas Materials Inst., and Dept. of Chemistry; Wayne State Univ., Detroit, MI (United States). Dept. of Chemistry
Thermo Fisher Scientific, Hillsboro, OR (United States)

In this report we examine the structure of bimetallic nanomaterials prepared by an electrochemical approach known as hydride-terminated (HT) electrodeposition. It has been shown previously that this method can lead to deposition of a single Pt monolayer on bulk-phase Au surfaces. Specifically, under appropriate electrochemical conditions and using a solution containing PtCl₄^2-, a monolayer of Pt atoms electrodeposits onto bulk-phase Au immediately followed by a monolayer of H atoms. The H-atom capping layer prevents deposition of Pt multilayers. We applied this method to ~1.6 nm Au nanoparticles (AuNPs) immobilized on an inert electrode surface. In contrast to the well-defined, segregated Au/Pt structure of the bulk-phase surface, we observe that HT electrodeposition leads to the formation of AuPt quasi-random alloy NPs rather than the core@shell structure anticipated from earlier reports relating to deposition onto bulk phases. The results provide a good example of how the phase behavior of macro materials does not always translate to the nano world. A key component of this study was the structure determination of the AuPt NPs, which required a combination of electrochemical methods, electron microscopy, X-ray absorption spectroscopy, and theory (DFT and MD).

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Univ. of Texas, Austin, TX (United States)

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

Grant/Contract Number:: SC0012704; SC0010576

OSTI ID:: 1436448

Alternate ID(s):: OSTI ID: 1617139

Report Number(s):: BNL-203640-2018-JAAM

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 20; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 28 works

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