DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Inhibitive effect of Pt on Pd-hydride formation of Pd@Pt core-shell electrocatalysts: An in situ EXAFS and XRD study

Abstract

In situ EXAFS and XRD have been used to study the electrochemical formation of hydride phases, Habs, in 0.5 M H2SO4 for a Pd/C catalyst and a series of Pd@Pt core-shell catalysts with varying Pt shell thickness, from 0.5 to 4 monolayers. Based on the XRD data a 3% lattice expansion is observed for the Pd/C core catalyst upon hydride formation at 0.0 V. In contrast, the expansion was ≤0.6% for all of the core-shell catalysts. The limited extent of the lattice expansion observed suggests that hydride formation, which may occur during periodic active surface area measurements conducting during accelerated aging tests or driven by H2 crossover in PEM fuel cells, is unlikely to contribute significantly to the degradation of Pd@Pt core-shell electrocatalysts in contrast to the effects of oxide formation.

Authors:
 [1];  [2];  [3];  [2];  [2];  [4];  [5];  [2]
  1. Univ. of Southampton (United Kingdom). Dept. of Chemistry; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  2. Univ. of Southampton (United Kingdom). Dept. of Chemistry
  3. Univ. of Southampton (United Kingdom). Dept. of Chemistry; Science and Technology Facilities Council (STFC), Harwell Campus, Oxford (United Kingdom). Diamond Light Source, Ltd.
  4. Univ. of Southampton (United Kingdom). Dept. of Chemistry; Ventacon UK, Gable Cottage, Crawley, Hampshire (United Kingdom)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1425664
Alternate Identifier(s):
OSTI ID: 1548870
Grant/Contract Number:  
AC02-76SF00515; AC02-98CH10886
Resource Type:
Accepted Manuscript
Journal Name:
Electrochimica Acta
Additional Journal Information:
Journal Volume: 262; Journal Issue: C; Journal ID: ISSN 0013-4686
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 25 ENERGY STORAGE; Electrocatalyst; EXAFS; XRD; Core-shell

Citation Formats

Wise, Anna M., Richardson, Peter W., Price, Stephen W. T., Chouchelamane, Gaël, Calvillo, Laura, Hendra, Patrick J., Toney, Michael F., and Russell, Andrea E. Inhibitive effect of Pt on Pd-hydride formation of Pd@Pt core-shell electrocatalysts: An in situ EXAFS and XRD study. United States: N. p., 2017. Web. doi:10.1016/j.electacta.2017.12.161.
Wise, Anna M., Richardson, Peter W., Price, Stephen W. T., Chouchelamane, Gaël, Calvillo, Laura, Hendra, Patrick J., Toney, Michael F., & Russell, Andrea E. Inhibitive effect of Pt on Pd-hydride formation of Pd@Pt core-shell electrocatalysts: An in situ EXAFS and XRD study. United States. https://doi.org/10.1016/j.electacta.2017.12.161
Wise, Anna M., Richardson, Peter W., Price, Stephen W. T., Chouchelamane, Gaël, Calvillo, Laura, Hendra, Patrick J., Toney, Michael F., and Russell, Andrea E. Wed . "Inhibitive effect of Pt on Pd-hydride formation of Pd@Pt core-shell electrocatalysts: An in situ EXAFS and XRD study". United States. https://doi.org/10.1016/j.electacta.2017.12.161. https://www.osti.gov/servlets/purl/1425664.
@article{osti_1425664,
title = {Inhibitive effect of Pt on Pd-hydride formation of Pd@Pt core-shell electrocatalysts: An in situ EXAFS and XRD study},
author = {Wise, Anna M. and Richardson, Peter W. and Price, Stephen W. T. and Chouchelamane, Gaël and Calvillo, Laura and Hendra, Patrick J. and Toney, Michael F. and Russell, Andrea E.},
abstractNote = {In situ EXAFS and XRD have been used to study the electrochemical formation of hydride phases, Habs, in 0.5 M H2SO4 for a Pd/C catalyst and a series of Pd@Pt core-shell catalysts with varying Pt shell thickness, from 0.5 to 4 monolayers. Based on the XRD data a 3% lattice expansion is observed for the Pd/C core catalyst upon hydride formation at 0.0 V. In contrast, the expansion was ≤0.6% for all of the core-shell catalysts. The limited extent of the lattice expansion observed suggests that hydride formation, which may occur during periodic active surface area measurements conducting during accelerated aging tests or driven by H2 crossover in PEM fuel cells, is unlikely to contribute significantly to the degradation of Pd@Pt core-shell electrocatalysts in contrast to the effects of oxide formation.},
doi = {10.1016/j.electacta.2017.12.161},
journal = {Electrochimica Acta},
number = C,
volume = 262,
place = {United States},
year = {Wed Dec 27 00:00:00 EST 2017},
month = {Wed Dec 27 00:00:00 EST 2017}
}

Journal Article:

Citation Metrics:
Cited by: 15 works
Citation information provided by
Web of Science

Figures / Tables:

Table 1 Table 1: Composition and particle size of the catalysts.

Save / Share:

Works referenced in this record:

Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs
journal, March 2005

  • Gasteiger, Hubert A.; Kocha, Shyam S.; Sompalli, Bhaskar
  • Applied Catalysis B: Environmental, Vol. 56, Issue 1-2, p. 9-35
  • DOI: 10.1016/j.apcatb.2004.06.021

Platinum-Based Oxygen Reduction Electrocatalysts
journal, April 2013

  • Wu, Jianbo; Yang, Hong
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar300359w

Overview of recent developments in oxygen reduction electrocatalysis
journal, December 2012


Tuning Nanoparticle Catalysis for the Oxygen Reduction Reaction
journal, June 2013

  • Guo, Shaojun; Zhang, Sen; Sun, Shouheng
  • Angewandte Chemie International Edition, Vol. 52, Issue 33
  • DOI: 10.1002/anie.201207186

Controlling the Catalytic Activity of Platinum-Monolayer Electrocatalysts for Oxygen Reduction with Different Substrates
journal, March 2005

  • Zhang, Junliang; Vukmirovic, Miomir B.; Xu, Ye
  • Angewandte Chemie International Edition, Vol. 44, Issue 14, p. 2132-2135
  • DOI: 10.1002/anie.200462335

Platinum monolayer electrocatalysts for oxygen reduction: Effect of substrates, and long-term stability
journal, January 2005

  • Zhang, J.; Vukmirovic, M. B.; Sasaki, K.
  • Journal of the Serbian Chemical Society, Vol. 70, Issue 3
  • DOI: 10.2298/JSC0503513Z

Platinum Monolayer Electrocatalysts for O2 Reduction:  Pt Monolayer on Pd(111) and on Carbon-Supported Pd Nanoparticles
journal, July 2004

  • Zhang, J.; Mo, Y.; Vukmirovic, M. B.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 30, p. 10955-10964
  • DOI: 10.1021/jp0379953

Palladium Monolayer and Palladium Alloy Electrocatalysts for Oxygen Reduction
journal, December 2006


Bimetallic and Ternary Alloys for Improved Oxygen Reduction Catalysis
journal, November 2007


Platinum and Palladium Nano-Structured Catalysts for Polymer Electrolyte Fuel Cells and Direct Methanol Fuel Cells
journal, July 2013

  • Long, Nguyen Viet; Thi, Cao Minh; Yong, Yang
  • Journal of Nanoscience and Nanotechnology, Vol. 13, Issue 7
  • DOI: 10.1166/jnn.2013.7570

Enhancing the catalytic and electrocatalytic properties of Pt-based catalysts by forming bimetallic nanocrystals with Pd
journal, January 2012

  • Zhang, Hui; Jin, Mingshang; Xia, Younan
  • Chemical Society Reviews, Vol. 41, Issue 24
  • DOI: 10.1039/c2cs35173k

Hydrogen-Storage Properties of Solid-Solution Alloys of Immiscible Neighboring Elements with Pd
journal, November 2010

  • Kusada, Kohei; Yamauchi, Miho; Kobayashi, Hirokazu
  • Journal of the American Chemical Society, Vol. 132, Issue 45
  • DOI: 10.1021/ja107362z

Atomic-Level Pd−Pt Alloying and Largely Enhanced Hydrogen-Storage Capacity in Bimetallic Nanoparticles Reconstructed from Core/Shell Structure by a Process of Hydrogen Absorption/Desorption
journal, April 2010

  • Kobayashi, Hirokazu; Yamauchi, Miho; Kitagawa, Hiroshi
  • Journal of the American Chemical Society, Vol. 132, Issue 16
  • DOI: 10.1021/ja1013163

Hydrogen Absorption in the Core/Shell Interface of Pd/Pt Nanoparticles
journal, February 2008

  • Kobayashi, Hirokazu; Yamauchi, Miho; Kitagawa, Hiroshi
  • Journal of the American Chemical Society, Vol. 130, Issue 6
  • DOI: 10.1021/ja078126k

Spillover in Heterogeneous Catalysis
journal, May 1995

  • Conner, W. Curtis.; Falconer, John L.
  • Chemical Reviews, Vol. 95, Issue 3
  • DOI: 10.1021/cr00035a014

Hydrogen Storage Mediated by Pd and Pt Nanoparticles
journal, October 2009

  • Yamauchi, Miho; Kobayashi, Hirokazu; Kitagawa, Hiroshi
  • ChemPhysChem, Vol. 10, Issue 15
  • DOI: 10.1002/cphc.200900289

Accelerated stress test procedures for PEM fuel cells under actual load constraints: State-of-art and proposals
journal, September 2015


In Situ XAS Studies of Core-Shell PEM Fuel Cell Catalysts: The Opportunities and Challenges
journal, October 2011

  • Russell, Andrea E.; Tessier, Beatrice; Wise, Anna
  • ECS Transactions, Vol. 41, Issue 1
  • DOI: 10.1149/1.3635543

PtML/Pd/C Core-Shell Electrocatalysts for the ORR in PEMFCs
journal, August 2009

  • Tessier, Béatrice C.; Russell, Andrea E.; Theobald, Brian R.
  • ECS Transactions, Vol. 16, Issue 37
  • DOI: 10.1149/1.3106718

Synthesis and characterisation of carbon-supported PtGe electrocatalysts for CO oxidation
journal, January 2001


Controlled Modification of Carbon Supported Platinum Electrocatalysts by Mo
journal, January 2002

  • Crabb, E. M.; Ravikumar, M. K.; Qian, Y.
  • Electrochemical and Solid-State Letters, Vol. 5, Issue 1
  • DOI: 10.1149/1.1419703

Preparation, structure, and stability of Pt and Pd monolayer modified Pd and Pt electrocatalysts
journal, January 2009

  • Wells, P. P.; Crabb, E. M.; King, C. R.
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 27
  • DOI: 10.1039/b823504j

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

  • Hammersley, A. P.; Svensson, S. O.; Hanfland, M.
  • High Pressure Research, Vol. 14, Issue 4-6, p. 235-248
  • DOI: 10.1080/08957959608201408

CO monolayer oxidation on Pt nanoparticles: Further insights into the particle size effects
journal, January 2007

  • Maillard, Frédéric; Savinova, Elena R.; Stimming, Ulrich
  • Journal of Electroanalytical Chemistry, Vol. 599, Issue 2
  • DOI: 10.1016/j.jelechem.2006.02.024

Pd/CO Average Chemisorption Stoichiometry in Highly Dispersed Supported Pd/γ-Al 2 O 3 Catalysts
journal, August 2002

  • Canton, Patrizia; Fagherazzi, Giuliano; Battagliarin, Marino
  • Langmuir, Vol. 18, Issue 17
  • DOI: 10.1021/la015650a

X-ray Absorption Spectroscopy of Low Temperature Fuel Cell Catalysts
journal, October 2004

  • Russell, Andrea E.; Rose, Abigail
  • Chemical Reviews, Vol. 104, Issue 10
  • DOI: 10.1021/cr020708r

X-ray-absorption study of the interaction of hydrogen with clusters of supported palladium
journal, May 1989


In-situ x-ray absorption spectroscopy studies of hydride and carbide formation in supported palladium catalysts
journal, October 1993

  • McCaulley, James A.
  • The Journal of Physical Chemistry, Vol. 97, Issue 40
  • DOI: 10.1021/j100142a018

Hydride phase formation in carbon supported palladium nanoparticle electrodes investigated using in situ EXAFS and XRD
journal, January 2003

  • Rose, Abigail; Maniguet, Stephanie; Mathew, Rebecca J.
  • Physical Chemistry Chemical Physics, Vol. 5, Issue 15
  • DOI: 10.1039/b302956e

Palladium nanoparticles “breathe” hydrogen; a surgical view with X-ray diffraction
journal, August 2010


Enhanced Oxygen Reduction Reaction Activity and Characterization of Pt–Pd/C Bimetallic Fuel Cell Catalysts with Pt-Enriched Surfaces in Acid Media
journal, October 2012

  • Liu, Licheng; Samjeske, Gabor; Nagamatsu, Shin-ichi
  • The Journal of Physical Chemistry C, Vol. 116, Issue 44
  • DOI: 10.1021/jp308021a

Hydrogen sorption ATIN electrodes
journal, February 1998


Thermodynamic and electrode kinetic factors in cathodic hydrogen sorption into metals and its relationship to hydrogen adsorption and poisoning
journal, October 1993


Factors in the Electrolytic Sorption of H into Metals and Its Relation to Cathodic Hydrogen Evolution Kinetics*
journal, January 1994


Hydrogen on and in Selected Overlayer Near-Surface Alloys and the Effect of Subsurface Hydrogen on the Reactivity of Alloy Surfaces
journal, February 2010


The effect of surface species on the rate of H sorption into nanostructured Pd
journal, January 2004

  • Bartlett, P. N.; Marwan, J.
  • Physical Chemistry Chemical Physics, Vol. 6, Issue 11
  • DOI: 10.1039/b404028g

Work function, electronegativity, and electrochemical behaviour of metals
journal, September 1972


Trends in the Exchange Current for Hydrogen Evolution
journal, January 2005

  • Nørskov, J. K.; Bligaard, T.; Logadottir, A.
  • Journal of The Electrochemical Society, Vol. 152, Issue 3
  • DOI: 10.1149/1.1856988

Simultaneous Operando Time-Resolved XAFS–XRD Measurements of a Pt/C Cathode Catalyst in Polymer Electrolyte Fuel Cell under Transient Potential Operations
journal, March 2017


Works referencing / citing this record:

Activity and stability improvement of platinum loaded on reduced graphene oxide and carbon nanotube composites for methanol oxidation
journal, December 2019

  • Pongpichayakul, Natthapong; Waenkeaw, Paralee; Jakmunee, Jaroon
  • Journal of Applied Electrochemistry, Vol. 50, Issue 1
  • DOI: 10.1007/s10800-019-01368-1

Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
journal, August 2019