skip to main content

DOE PAGESDOE PAGES

This content will become publicly available on September 1, 2019

Title: Application of differential resonant high-energy X-ray diffraction to three-dimensional structure studies of nanosized materials: A case study of Pt–Pd nanoalloy catalysts

Atoms in many of the increasingly complex nanosized materials of interest to science and technology do not necessarily occupy the vertices of Bravais lattices. The atomic scale structure of such materials is difficult to determine by traditional X-ray diffraction and so their functional properties remain difficult to optimize by rational design. Here, the three-dimensional structure of Pt xPd 100–x nanoalloy particles is determined, where x = 0, 14, 36, 47, 64 and 100, by a non-traditional technique involving differential resonant high-energy X-ray diffraction experiments conducted at the K edge of Pt and Pd. The technique is coupled with three-dimensional modeling guided by the experimental total and element-specific atomic pair distribution functions. Furthermore, using DFT (density functional theory) calculation based on the positions of atoms in the obtained three-dimensional structure models, the catalytic performance of Pt–Pd particles is explained. Furthermore, differential resonant high-energy X-ray diffraction is shown to be an excellent tool for three-dimensional structure studies of nanosized materials. The experimental and modeling procedures are described in good detail, to facilitate their wider usage.
Authors:
ORCiD logo [1] ;  [2] ;  [2] ;  [3] ; ORCiD logo [3] ;  [3] ;  [3]
  1. Central Michigan Univ., Mt. Pleasant, MI (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. State Univ. of New York, Binghamton, NY (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Acta Crystallographica. Section A, Foundations and Advances (Online)
Additional Journal Information:
Journal Name: Acta Crystallographica. Section A, Foundations and Advances (Online); Journal Volume: 74; Journal Issue: 5; Journal ID: ISSN 2053-2733
Publisher:
International Union of Crystallography
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; element-specific pair distribution functions; nanosized materials; resonant high-energy X-ray diffraction; structural coherence; structure-function relationships
OSTI Identifier:
1475064

Petkov, Valeri, Shastri, Sarvjit, Kim, Jong -Woo, Shan, Shiyao, Luo, Jin, Wu, Jinfang, and Zhong, Chuan -Jian. Application of differential resonant high-energy X-ray diffraction to three-dimensional structure studies of nanosized materials: A case study of Pt–Pd nanoalloy catalysts. United States: N. p., Web. doi:10.1107/S2053273318009282.
Petkov, Valeri, Shastri, Sarvjit, Kim, Jong -Woo, Shan, Shiyao, Luo, Jin, Wu, Jinfang, & Zhong, Chuan -Jian. Application of differential resonant high-energy X-ray diffraction to three-dimensional structure studies of nanosized materials: A case study of Pt–Pd nanoalloy catalysts. United States. doi:10.1107/S2053273318009282.
Petkov, Valeri, Shastri, Sarvjit, Kim, Jong -Woo, Shan, Shiyao, Luo, Jin, Wu, Jinfang, and Zhong, Chuan -Jian. 2018. "Application of differential resonant high-energy X-ray diffraction to three-dimensional structure studies of nanosized materials: A case study of Pt–Pd nanoalloy catalysts". United States. doi:10.1107/S2053273318009282.
@article{osti_1475064,
title = {Application of differential resonant high-energy X-ray diffraction to three-dimensional structure studies of nanosized materials: A case study of Pt–Pd nanoalloy catalysts},
author = {Petkov, Valeri and Shastri, Sarvjit and Kim, Jong -Woo and Shan, Shiyao and Luo, Jin and Wu, Jinfang and Zhong, Chuan -Jian},
abstractNote = {Atoms in many of the increasingly complex nanosized materials of interest to science and technology do not necessarily occupy the vertices of Bravais lattices. The atomic scale structure of such materials is difficult to determine by traditional X-ray diffraction and so their functional properties remain difficult to optimize by rational design. Here, the three-dimensional structure of PtxPd100–x nanoalloy particles is determined, where x = 0, 14, 36, 47, 64 and 100, by a non-traditional technique involving differential resonant high-energy X-ray diffraction experiments conducted at the K edge of Pt and Pd. The technique is coupled with three-dimensional modeling guided by the experimental total and element-specific atomic pair distribution functions. Furthermore, using DFT (density functional theory) calculation based on the positions of atoms in the obtained three-dimensional structure models, the catalytic performance of Pt–Pd particles is explained. Furthermore, differential resonant high-energy X-ray diffraction is shown to be an excellent tool for three-dimensional structure studies of nanosized materials. The experimental and modeling procedures are described in good detail, to facilitate their wider usage.},
doi = {10.1107/S2053273318009282},
journal = {Acta Crystallographica. Section A, Foundations and Advances (Online)},
number = 5,
volume = 74,
place = {United States},
year = {2018},
month = {9}
}

Works referenced in this record:

Platinum Metal Catalysts of High-Index Surfaces: From Single-Crystal Planes to Electrochemically Shape-Controlled Nanoparticles
journal, November 2008
  • Tian, Na; Zhou, Zhi-You; Sun, Shi-Gang
  • The Journal of Physical Chemistry C, Vol. 112, Issue 50, p. 19801-19817
  • DOI: 10.1021/jp804051e

Finite size effects of nanoparticles on the atomic pair distribution functions
journal, October 2006
  • Kodama, Katsuaki; Iikubo, Satoshi; Taguchi, Tomitsugu
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 62, Issue 6, p. 444-453
  • DOI: 10.1107/S0108767306034635