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Title: In-situ and ex-situ comparison of the electrochemical oxidation of SO2 on carbon supported Pt and Au catalysts

Abstract

Electrochemical characterizations are performed using thin films and commercial carbon supported platinum and gold catalysts for sulfur dioxide oxidation, the primary electrochemical oxidation reaction in the Hybrid-sulfur (HyS) thermochemical process. Electrochemical evaluation of metal thin films qualitatively confirms the higher activity of Au over Pt, AuPt, Pd, and Ir for the electrochemical oxidation of SO2. Ex-situ testing, using rotating disk electrode (RDE), shows an earlier onset potential for Au/C at low sulfuric acid concentrations (C ≤ 3.5 M) and a higher turnover frequency than Pt/C at sulfuric acid concentrations ranging from 3.5 M to 9 M. In-situ electrolysis experiments using low catalyst loadings (0.1 mgAu cm–2, a factor of ≥5 lower than typical loadings) confirm that Au nanoparticles exhibit higher current densities and greater stability than Pt nanoparticles. This is consistent with the thin film screening studies, which showed higher activity with increasing gold content in AuPt thin films. Here, this work reveals an alternative material to state-of-the-art Pt to lower the energy needs and aid the HyS cycle in reaching the target of $2/kg H2 set forth by the Department of Energy to achieve economic feasibility of large-scale hydrogen generation.

Authors:
 [1];  [2];  [1];  [3];  [4];  [4];  [5];  [5];  [5];  [5];  [1];  [1];  [2]
+ Show Author Affiliations
  1. Univ. of South Carolina, Columbia, SC (United States)
  2. Savannah River National Lab., Aiken, SC (United States)
  3. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  4. Savannah River Consulting, LLC, Aiken, SC (United States)
  5. PVD Products, Inc., Wilmington, MA (United States)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States); Savannah River National Laboratory (SRNL), Aiken, SC (United States)
Sponsoring Org.:
USDOE Office of Environmental Management (EM)
OSTI Identifier:
1591775
Alternate Identifier(s):
OSTI ID: 1580803
Report Number(s):
SRNL-STI-2019-00365
Journal ID: ISSN 0360-3199; TRN: US2102091
Grant/Contract Number:  
AC09-08SR22470
Resource Type:
Accepted Manuscript
Journal Name:
International Journal of Hydrogen Energy
Additional Journal Information:
Journal Volume: 45; Journal Issue: 3; Journal ID: ISSN 0360-3199
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; Hybrid sulfur; Gold catalyst; Platinum catalyst; Hydrogen production; Sulfur dioxide electrochemical oxidation

Citation Formats

Meekins, Benjamin H., Thompson, Anthony B., Gopal, Varsha, Mehrabadi, Bahareh A. Tavakoli, Elvington, Mark C., Ganesan, Prabhu, Newhouse-Illige, Ty A., Shepard, Adam W., Scipioni, Lawrence E., Greer, James A., Weiss, John C., Weidner, John W., and Colón-Mercado, Héctor R. In-situ and ex-situ comparison of the electrochemical oxidation of SO2 on carbon supported Pt and Au catalysts. United States: N. p., 2019. Web. doi:10.1016/j.ijhydene.2019.11.112.
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Meekins, Benjamin H., Thompson, Anthony B., Gopal, Varsha, Mehrabadi, Bahareh A. Tavakoli, Elvington, Mark C., Ganesan, Prabhu, Newhouse-Illige, Ty A., Shepard, Adam W., Scipioni, Lawrence E., Greer, James A., Weiss, John C., Weidner, John W., & Colón-Mercado, Héctor R. In-situ and ex-situ comparison of the electrochemical oxidation of SO2 on carbon supported Pt and Au catalysts. United States. https://doi.org/10.1016/j.ijhydene.2019.11.112
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Meekins, Benjamin H., Thompson, Anthony B., Gopal, Varsha, Mehrabadi, Bahareh A. Tavakoli, Elvington, Mark C., Ganesan, Prabhu, Newhouse-Illige, Ty A., Shepard, Adam W., Scipioni, Lawrence E., Greer, James A., Weiss, John C., Weidner, John W., and Colón-Mercado, Héctor R. Thu . "In-situ and ex-situ comparison of the electrochemical oxidation of SO2 on carbon supported Pt and Au catalysts". United States. https://doi.org/10.1016/j.ijhydene.2019.11.112. https://www.osti.gov/servlets/purl/1591775.
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@article{osti_1591775,
title = {In-situ and ex-situ comparison of the electrochemical oxidation of SO2 on carbon supported Pt and Au catalysts},
author = {Meekins, Benjamin H. and Thompson, Anthony B. and Gopal, Varsha and Mehrabadi, Bahareh A. Tavakoli and Elvington, Mark C. and Ganesan, Prabhu and Newhouse-Illige, Ty A. and Shepard, Adam W. and Scipioni, Lawrence E. and Greer, James A. and Weiss, John C. and Weidner, John W. and Colón-Mercado, Héctor R.},
abstractNote = {Electrochemical characterizations are performed using thin films and commercial carbon supported platinum and gold catalysts for sulfur dioxide oxidation, the primary electrochemical oxidation reaction in the Hybrid-sulfur (HyS) thermochemical process. Electrochemical evaluation of metal thin films qualitatively confirms the higher activity of Au over Pt, AuPt, Pd, and Ir for the electrochemical oxidation of SO2. Ex-situ testing, using rotating disk electrode (RDE), shows an earlier onset potential for Au/C at low sulfuric acid concentrations (C ≤ 3.5 M) and a higher turnover frequency than Pt/C at sulfuric acid concentrations ranging from 3.5 M to 9 M. In-situ electrolysis experiments using low catalyst loadings (0.1 mgAu cm–2, a factor of ≥5 lower than typical loadings) confirm that Au nanoparticles exhibit higher current densities and greater stability than Pt nanoparticles. This is consistent with the thin film screening studies, which showed higher activity with increasing gold content in AuPt thin films. Here, this work reveals an alternative material to state-of-the-art Pt to lower the energy needs and aid the HyS cycle in reaching the target of $2/kg H2 set forth by the Department of Energy to achieve economic feasibility of large-scale hydrogen generation.},
doi = {10.1016/j.ijhydene.2019.11.112},
journal = {International Journal of Hydrogen Energy},
number = 3,
volume = 45,
place = {United States},
year = {Thu Dec 12 00:00:00 EST 2019},
month = {Thu Dec 12 00:00:00 EST 2019}
}
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https://doi.org/10.1016/j.ijhydene.2019.11.112
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