Quantitative Analysis of the Reduction Kinetics Responsible for the One-Pot Synthesis of Pd–Pt Bimetallic Nanocrystals with Different Structures

Zhou, Ming; Wang, Helan; Vara, Madeline; Hood, Zachary D.; Luo, Ming; Yang, Tung-Han; Bao, Shixiong; Chi, Miaofang; Xiao, Peng; Zhang, Yunhuai; Xia, Younan

doi:10.1021/jacs.6b07213

Title: Quantitative Analysis of the Reduction Kinetics Responsible for the One-Pot Synthesis of Pd–Pt Bimetallic Nanocrystals with Different Structures

Journal Article · Mon Sep 12 00:00:00 EDT 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.6b07213· OSTI ID:1760157

Zhou, Ming ^[1]; Wang, Helan ^[2]; Vara, Madeline ^[3]; Hood, Zachary D. ^[4]; Luo, Ming ^[2]; Yang, Tung-Han ^[2]; Bao, Shixiong ^[2];

^[5]; Xiao, Peng ^[6]; Zhang, Yunhuai ^[6]; Xia, Younan ^[2]

Chongqing Univ. (China); Emory Univ., Atlanta, GA (United States); Georgia Institute of Technology, Atlanta, GA (United States)
Emory Univ., Atlanta, GA (United States); Georgia Institute of Technology, Atlanta, GA (United States)
Georgia Institute of Technology, Atlanta, GA (United States)
Emory Univ., Atlanta, GA (United States); Georgia Institute of Technology, Atlanta, GA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Chongqing Univ. (China)

We report a quantitative understanding of the reduction kinetics responsible for the formation of Pd–Pt bimetallic nanocrystals with two distinctive structures. The syntheses involve the use of KBr to manipulate the reaction kinetics by influencing the redox potentials of metal precursor ions via ligand exchange. In the absence of KBr, the ratio between the initial reduction rates of PdCl₄^2– and PtCl₄^2– was about 10.0, leading to the formation of Pd@Pt octahedra with a core–shell structure. In the presence of 63 mM KBr, the products became Pd–Pt alloy nanocrystals. In this case, the ratio between the initial reduction rates of the two precursors dropped to 2.4 because of ligand exchange and, thus, the formation of PdBr₄^2– and PtBr₄^2–. The alloy nanocrystals took a cubic shape owing to the selective capping effect of Br^– ions toward the {100} facets. Relative to the alloy nanocubes, the Pd@Pt core–shell octahedra showed substantial enhancement in both catalytic activity and durability toward the oxygen reduction reaction (ORR). Specifically, the specific (1.51 mA cm^–2) and mass (1.05 A mg^–1Pt) activities of the core–shell octahedra were enhanced by about four- and three-fold relative to the alloy nanocubes (0.39 mA cm^–2 and 0.34 A mg^–1Pt, respectively). Even after 20000 cycles of accelerated durability test, the core–shell octahedra still exhibited a mass activity of 0.68 A mg^–1Pt, twice that of a pristine commercial Pt/C catalyst.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1760157

Journal Information:: Journal of the American Chemical Society, Vol. 138, Issue 37; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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