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

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 PtCl 4 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).
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [5] ; ORCiD logo [3] ;  [2] ;  [1]
  1. Univ. of Texas, Austin, TX (United States). Texas Materials Inst., and Dept. of Chemistry
  2. Univ. of Texas, Austin, TX (United States). Inst. for Computational and Engineering Sciences, and Dept. of Chemistry
  3. Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering
  4. Univ. of Texas, Austin, TX (United States). Texas Materials Inst., and Dept. of Chemistry; Wayne State Univ., Detroit, MI (United States). Dept. of Chemistry
  5. Thermo Fisher Scientific, Hillsboro, OR (United States)
Publication Date:
Report Number(s):
BNL-203640-2018-JAAM
Journal ID: ISSN 0002-7863
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Name: Journal of the American Chemical Society; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1436448

Lapp, Aliya S., Duan, Zhiyao, Marcella, Nicholas, Luo, Long, Genc, Arda, Ringnalda, Jan, Frenkel, Anatoly I., Henkelman, Graeme, and Crooks, Richard M.. Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method. United States: N. p., Web. doi:10.1021/jacs.7b12306.
Lapp, Aliya S., Duan, Zhiyao, Marcella, Nicholas, Luo, Long, Genc, Arda, Ringnalda, Jan, Frenkel, Anatoly I., Henkelman, Graeme, & Crooks, Richard M.. Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method. United States. doi:10.1021/jacs.7b12306.
Lapp, Aliya S., Duan, Zhiyao, Marcella, Nicholas, Luo, Long, Genc, Arda, Ringnalda, Jan, Frenkel, Anatoly I., Henkelman, Graeme, and Crooks, Richard M.. 2018. "Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method". United States. doi:10.1021/jacs.7b12306.
@article{osti_1436448,
title = {Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method},
author = {Lapp, Aliya S. and Duan, Zhiyao and Marcella, Nicholas and Luo, Long and Genc, Arda and Ringnalda, Jan and Frenkel, Anatoly I. and Henkelman, Graeme and Crooks, Richard M.},
abstractNote = {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 PtCl42-, 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).},
doi = {10.1021/jacs.7b12306},
journal = {Journal of the American Chemical Society},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {6}
}