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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, H abs, in 0.5 M H 2SO 4 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 H 2 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) (SC-22)
OSTI Identifier:
1425664
Alternate Identifier(s):
OSTI ID: 1548870
Grant/Contract Number:  
AC02-76SF00515; AC02-98CH10886
Resource Type:
Journal Article: 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. 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., 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. doi: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},
issn = {0013-4686},
number = C,
volume = 262,
place = {United States},
year = {2017},
month = {12}
}

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Figures / Tables:

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

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