Hydrogen Sorption Kinetics on Bare and Platinum-Modified Palladium Nanofilms, Grown by Electrochemical Atomic Layer Deposition (E-ALD)

Jagannathan, Kaushik; Benson, David M.; Robinson, David B.; Stickney, John L.

doi:10.1149/2.0051612jes

Title: Hydrogen Sorption Kinetics on Bare and Platinum-Modified Palladium Nanofilms, Grown by Electrochemical Atomic Layer Deposition (E-ALD)

Abstract

Nanofilms of Pd were grown using an electrochemical form of atomic layer deposition (E-ALD) on 100 nm evaporated Au films on glass. Multiple cycles of surface-limited redox replacement (SLRR) were used to grow deposits. Each SLRR involved the underpotential deposition (UPD) of a Cu atomic layer, followed by open circuit replacement via redox exchange with tetrachloropalladate, forming a Pd atomic layer: one E-ALD deposition cycle. That cycle was repeated in order to grow deposits of a desired thickness. 5 cycles of Pd deposition were performed on the Au on glass substrates, resulting in the formation of 2.5 monolayers of Pd. Those Pd films were then modified with varying coverages of Pt, also formed using SLRR. The amount of Pt was controlled by changing the potential for Cu UPD, and by increasing the number of Pt deposition cycles. Hydrogen absorption was studied using coulometry and cyclic voltammetry in 0.1 M H₂SO₄ as a function of Pt coverage. The presence of even a small fraction of a Pt monolayer dramatically increased the rate of hydrogen desorption. However, this did not reduce the films’ hydrogen storage capacity. The increase in desorption rate in the presence of Pt was over an order of magnitude.

Authors:

Jagannathan, Kaushik ^[1]; Benson, David M. ^[1]; Robinson, David B. ^[2]; Stickney, John L. ^[1]

Univ. of Georgia, Athens, GA (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Publication Date:: Fri Jan 01 00:00:00 EST 2016

Research Org.:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1338320

Report Number(s):: SAND-2016-7191J
Journal ID: ISSN 0013-4651; 646103

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the Electrochemical Society

Additional Journal Information:: Journal Volume: 163; Journal Issue: 12; Journal ID: ISSN 0013-4651

Publisher:: The Electrochemical Society

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Jagannathan, Kaushik, Benson, David M., Robinson, David B., and Stickney, John L. Hydrogen Sorption Kinetics on Bare and Platinum-Modified Palladium Nanofilms, Grown by Electrochemical Atomic Layer Deposition (E-ALD).  United States: N. p., 2016. 
Web.  doi:10.1149/2.0051612jes.

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                    Jagannathan, Kaushik, Benson, David M., Robinson, David B., & Stickney, John L. Hydrogen Sorption Kinetics on Bare and Platinum-Modified Palladium Nanofilms, Grown by Electrochemical Atomic Layer Deposition (E-ALD).  United States.  https://doi.org/10.1149/2.0051612jes

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                    Jagannathan, Kaushik, Benson, David M., Robinson, David B., and Stickney, John L. Fri .  
"Hydrogen Sorption Kinetics on Bare and Platinum-Modified Palladium Nanofilms, Grown by Electrochemical Atomic Layer Deposition (E-ALD)".  United States.  https://doi.org/10.1149/2.0051612jes.  https://www.osti.gov/servlets/purl/1338320.

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@article{osti_1338320,

  title        = {Hydrogen Sorption Kinetics on Bare and Platinum-Modified Palladium Nanofilms, Grown by Electrochemical Atomic Layer Deposition (E-ALD)},

  author       = {Jagannathan, Kaushik and Benson, David M. and Robinson, David B. and Stickney, John L.},

  abstractNote = {Nanofilms of Pd were grown using an electrochemical form of atomic layer deposition (E-ALD) on 100 nm evaporated Au films on glass. Multiple cycles of surface-limited redox replacement (SLRR) were used to grow deposits. Each SLRR involved the underpotential deposition (UPD) of a Cu atomic layer, followed by open circuit replacement via redox exchange with tetrachloropalladate, forming a Pd atomic layer: one E-ALD deposition cycle. That cycle was repeated in order to grow deposits of a desired thickness. 5 cycles of Pd deposition were performed on the Au on glass substrates, resulting in the formation of 2.5 monolayers of Pd. Those Pd films were then modified with varying coverages of Pt, also formed using SLRR. The amount of Pt was controlled by changing the potential for Cu UPD, and by increasing the number of Pt deposition cycles. Hydrogen absorption was studied using coulometry and cyclic voltammetry in 0.1 M H2SO4 as a function of Pt coverage. The presence of even a small fraction of a Pt monolayer dramatically increased the rate of hydrogen desorption. However, this did not reduce the films’ hydrogen storage capacity. The increase in desorption rate in the presence of Pt was over an order of magnitude.},

  doi          = {10.1149/2.0051612jes},

  journal      = {Journal of the Electrochemical Society},

  number       = 12,

  volume       = 163,

  place        = {United States},

  year         = {Fri Jan 01 00:00:00 EST 2016},

  month        = {Fri Jan 01 00:00:00 EST 2016}

}

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Title: Hydrogen Sorption Kinetics on Bare and Platinum-Modified Palladium Nanofilms, Grown by Electrochemical Atomic Layer Deposition (E-ALD)

Abstract

Citation Formats

Pd–Pt alloys: correlation between electronic structure and hydrogenation properties journal, June 2001

Investigation of Hydrogen Adsorption and Absorption in Palladium Thin Films journal, January 2004

Comparison of Hydrogen Electroadsorption from the Electrolyte with Hydrogen Adsorption from the Gas Phase journal, January 1996

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Pd deposition onto Au(111) electrodes from sulphuric acid solution
journal, October 2005

Surface-Enhanced Raman Scattering on Uniform Platinum-Group Overlayers: Preparation by Redox Replacement of Underpotential-Deposited Metals on Gold
journal, December 2001

Electrochemical absorption and oxidation of hydrogen on palladium alloys with platinum, gold and rhodium
journal, January 2010

The influence of carbon monoxide on hydrogen absorption by thin films of palladium
journal, April 1991

The Hydrogen Economy
journal, December 2004

The Palladium-Hydrogen System
journal, August 1991

Electrochemical atomic layer epitaxy (ECALE)
journal, February 1991

Metal monolayer deposition by replacement of metal adlayers on electrode surfaces
journal, March 2001

A hydrogen adsorption and absorption study with ultrathin Pd overlayers on Au(111) and Au(100)
journal, October 1993

Investigation of Hydrogen Adsorption and Absorption in Palladium Thin Films
journal, January 2004

The hydrogen economy
journal, January 2006