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Title: Enhanced Kinetics of Electrochemical Hydrogen Uptake and Release by Palladium Powders Modified by Electrochemical Atomic Layer Deposition

Abstract

One method for the formation of nanofilms of materials, is Electrochemical atomic layer deposition (E-ALD), one atomic layer at a time. It uses the galvanic exchange of a less noble metal, deposited using underpotential deposition (UPD), to produce an atomic layer of a more noble element by reduction of its ions. This process is referred to as surface limited redox replacement and can be repeated in a cycle to grow thicker deposits. Previously, we performed it on nanoparticles and planar substrates. In the present report, E-ALD is applied for coating a submicron-sized powder substrate, making use of a new flow cell design. E-ALD is used to coat a Pd powder substrate with different thicknesses of Rh by exchanging it for Cu UPD. Furthermore, cyclic voltammetry and X-ray photoelectron spectroscopy indicate an increasing Rh coverage with increasing numbers of deposition cycles performed, in a manner consistent with the atomic layer deposition (ALD) mechanism. Cyclic voltammetry also indicated increased kinetics of H sorption and desorption in and out of the Pd powder with Rh present, relative to unmodified Pd.

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [2];  [2];  [3];  [1]
  1. Univ. of Georgia, Athens, GA (United States). Dept. of Chemistry
  2. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  3. Sandia National Lab. (SNL-CA), Livermore, CA (United States); Univ. of Massachusetts, North Dartmouth, MA (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1360933
Report Number(s):
SAND-2017-5175J
Journal ID: ISSN 1944-8244; 653340; TRN: US1701980
Grant/Contract Number:  
AC04-94AL85000; NA0003525; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 21; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; E-ALD; electrodeposition; flow cell; palladium; powder; rhodium; SLRR; UPD

Citation Formats

Benson, David M., Tsang, Chu F., Sugar, Joshua Daniel, Jagannathan, Kaushik, Robinson, David B., El Gabaly, Farid, Cappillino, Patrick J., and Stickney, John L. Enhanced Kinetics of Electrochemical Hydrogen Uptake and Release by Palladium Powders Modified by Electrochemical Atomic Layer Deposition. United States: N. p., 2017. Web. https://doi.org/10.1021/acsami.7b03005.
Benson, David M., Tsang, Chu F., Sugar, Joshua Daniel, Jagannathan, Kaushik, Robinson, David B., El Gabaly, Farid, Cappillino, Patrick J., & Stickney, John L. Enhanced Kinetics of Electrochemical Hydrogen Uptake and Release by Palladium Powders Modified by Electrochemical Atomic Layer Deposition. United States. https://doi.org/10.1021/acsami.7b03005
Benson, David M., Tsang, Chu F., Sugar, Joshua Daniel, Jagannathan, Kaushik, Robinson, David B., El Gabaly, Farid, Cappillino, Patrick J., and Stickney, John L. Fri . "Enhanced Kinetics of Electrochemical Hydrogen Uptake and Release by Palladium Powders Modified by Electrochemical Atomic Layer Deposition". United States. https://doi.org/10.1021/acsami.7b03005. https://www.osti.gov/servlets/purl/1360933.
@article{osti_1360933,
title = {Enhanced Kinetics of Electrochemical Hydrogen Uptake and Release by Palladium Powders Modified by Electrochemical Atomic Layer Deposition},
author = {Benson, David M. and Tsang, Chu F. and Sugar, Joshua Daniel and Jagannathan, Kaushik and Robinson, David B. and El Gabaly, Farid and Cappillino, Patrick J. and Stickney, John L.},
abstractNote = {One method for the formation of nanofilms of materials, is Electrochemical atomic layer deposition (E-ALD), one atomic layer at a time. It uses the galvanic exchange of a less noble metal, deposited using underpotential deposition (UPD), to produce an atomic layer of a more noble element by reduction of its ions. This process is referred to as surface limited redox replacement and can be repeated in a cycle to grow thicker deposits. Previously, we performed it on nanoparticles and planar substrates. In the present report, E-ALD is applied for coating a submicron-sized powder substrate, making use of a new flow cell design. E-ALD is used to coat a Pd powder substrate with different thicknesses of Rh by exchanging it for Cu UPD. Furthermore, cyclic voltammetry and X-ray photoelectron spectroscopy indicate an increasing Rh coverage with increasing numbers of deposition cycles performed, in a manner consistent with the atomic layer deposition (ALD) mechanism. Cyclic voltammetry also indicated increased kinetics of H sorption and desorption in and out of the Pd powder with Rh present, relative to unmodified Pd.},
doi = {10.1021/acsami.7b03005},
journal = {ACS Applied Materials and Interfaces},
number = 21,
volume = 9,
place = {United States},
year = {2017},
month = {4}
}

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