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Title: Self-terminating electrodeposition of Pt on WC electrocatalysts

Abstract

Self-terminated electrochemical deposition is used to grow Pt nanoparticles on tungsten monocarbide (WC) from a pH 4 electrolyte of 3 mmol/L K2PtCl4-0.5 mol/L NaCl. An unconventional potentiodynamic deposition program is used where nucleation is promoted at large over potentials followed by growth termination at still larger over potentials to yield a high coverage of Pt nanoparticles. Following three deposition cycles between –0.8 VSCE and –0.45 VSCE, the surface is covered by a monolayer equivalent charge of Pt in the form of ≈3×1011 particles/cm2 that are ≈6.7 ± 1.1 nm in diameter. The number and size of nanoparticles increase monotonically for five deposition cycles. Area-normalized kinetics for hydrogen evolution (HER) and oxidation (HOR) on Pt-WC were determined in 0.5 mol/L H2SO4. For the lowest surface coverage of Pt nanoparticles on WC, ≈ 0.01, an exchange current density of ≈ 100 mA/cm2 is achieved, comparable to the highest reported values for Pt nanoparticles and ultra microelectrodes. The area normalized apparent exchange current density decreases with increasing Pt coverage as the relative contribution of point versus planar diffusion decreases. Self-terminated electrodeposition of Pt provides an attractive approach to achieving ultra-low loadings of well-dispersed Pt nanoparticles on a non-precious metal support like WC.

Authors:
 [1];  [2];  [3];  [3];  [3];  [4]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Lam Research, Tualatin, OR (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Columbia Univ., New York, NY (United States)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Columbia University; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; University of Delaware; National Institute of Standards and Technology (NIST)
OSTI Identifier:
1579193
Alternate Identifier(s):
OSTI ID: 1776966
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Applied Surface Science
Additional Journal Information:
Journal Volume: 504; Journal Issue: C; Journal ID: ISSN 0169-4332
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; XPS; electrocatalysis; electrodeposition; self-terminated growth

Citation Formats

Liu, Yihua, You, Hoydoo, Kimmel, Yannick C., Esposito, Daniel V., Chen, Jingguang G., and Moffat, Thomas P. Self-terminating electrodeposition of Pt on WC electrocatalysts. United States: N. p., 2019. Web. doi:10.1016/j.apsusc.2019.144472.
Liu, Yihua, You, Hoydoo, Kimmel, Yannick C., Esposito, Daniel V., Chen, Jingguang G., & Moffat, Thomas P. Self-terminating electrodeposition of Pt on WC electrocatalysts. United States. https://doi.org/10.1016/j.apsusc.2019.144472
Liu, Yihua, You, Hoydoo, Kimmel, Yannick C., Esposito, Daniel V., Chen, Jingguang G., and Moffat, Thomas P. Mon . "Self-terminating electrodeposition of Pt on WC electrocatalysts". United States. https://doi.org/10.1016/j.apsusc.2019.144472. https://www.osti.gov/servlets/purl/1579193.
@article{osti_1579193,
title = {Self-terminating electrodeposition of Pt on WC electrocatalysts},
author = {Liu, Yihua and You, Hoydoo and Kimmel, Yannick C. and Esposito, Daniel V. and Chen, Jingguang G. and Moffat, Thomas P.},
abstractNote = {Self-terminated electrochemical deposition is used to grow Pt nanoparticles on tungsten monocarbide (WC) from a pH 4 electrolyte of 3 mmol/L K2PtCl4-0.5 mol/L NaCl. An unconventional potentiodynamic deposition program is used where nucleation is promoted at large over potentials followed by growth termination at still larger over potentials to yield a high coverage of Pt nanoparticles. Following three deposition cycles between –0.8 VSCE and –0.45 VSCE, the surface is covered by a monolayer equivalent charge of Pt in the form of ≈3×1011 particles/cm2 that are ≈6.7 ± 1.1 nm in diameter. The number and size of nanoparticles increase monotonically for five deposition cycles. Area-normalized kinetics for hydrogen evolution (HER) and oxidation (HOR) on Pt-WC were determined in 0.5 mol/L H2SO4. For the lowest surface coverage of Pt nanoparticles on WC, ≈ 0.01, an exchange current density of ≈ 100 mA/cm2 is achieved, comparable to the highest reported values for Pt nanoparticles and ultra microelectrodes. The area normalized apparent exchange current density decreases with increasing Pt coverage as the relative contribution of point versus planar diffusion decreases. Self-terminated electrodeposition of Pt provides an attractive approach to achieving ultra-low loadings of well-dispersed Pt nanoparticles on a non-precious metal support like WC.},
doi = {10.1016/j.apsusc.2019.144472},
journal = {Applied Surface Science},
number = C,
volume = 504,
place = {United States},
year = {2019},
month = {10}
}

Journal Article:

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Cited by: 4 works
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Figures / Tables:

Fig. 1 Fig. 1: (a) Linear scan voltammetry from −0.8 VSCE probing the oxidation of W (black solid line) and WC (red solid line) in pH 4 0.5mol/L NaCl. Inset shows multicycle voltammetry for W. (b) Potentiodynamic Pt deposition in pH 4, 0.5mol/L NaCl+ 3mmol/L K2PtCl4 initiated at −0.8 VSCE on Au,more » W and WC electrodes. All voltammograms were collected at 2mV/s with the RDE rotating at 400 rpm. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)« less

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