Effect of Organic Cations on Hydrogen Oxidation Reaction of Carbon Supported Platinum
Abstract
Effect of organic cations on hydrogen oxidation reaction (HOR) of carbon supported platinum (Pt/C) is investigated using three 0.1 M alkaline electrolytes, tetramethylammonium hydroxide (TMAOH), tetrabutylammonium hydroxide (TBAOH) and tetrabutylphosphonium hydroxide (TBPOH). Rotating disk electrode experiments indicate that the HOR of Pt/C is adversely impacted by time-dependent and potential-driven chemisorption of organic cations. In-situ infrared reflection adsorption spectroscopy experiments indicated that the specific chemisorption of organic cations drives the hydroxide co-adsorption on Pt surface. The co-adsorption of TMA+ and hydroxide at 0.1 V vs. reversible hydrogen electrode is the strongest; consequently, complete removal of the co-adsorbed layer from Pt surface is difficult even after exposure the Pt surface to 1.2 V. Conversely, the chemisorption of TBP+ is the weakest, yet notable decrease of HOR current density is still observed. The adsorption energies, ΔE, for TMA+, TBA+, and TBP+ on Pt (111) surface from density functional theory are computed to be -2.79, -2.42 and -2.00 eV, respectively. The relatively low adsorption energy of TBP+ is explained by the steric hindrance and electronic effect. This study emphasizes the importance of cationic group on HOR activity of alkaline anion exchange membrane fuel cells.
- Authors:
-
[1];
[1];
[1];
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
- Rensselaer Polytechnic Inst., Troy, NY (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1345940
- Report Number(s):
- LA-UR-16-26356
Journal ID: ISSN 0013-4651
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Volume: 163; Journal Issue: 14; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Energy Sciences
Citation Formats
Chung, Hoon Taek, Choe, Yong-Kee, Martinez, Ulises, Dumont, Joseph Henry, Monahty, Angela, Bae, Chulsung, Matanovic, Ivana, and Kim, Yu Seung. Effect of Organic Cations on Hydrogen Oxidation Reaction of Carbon Supported Platinum. United States: N. p., 2016.
Web. doi:10.1149/2.0511614jes.
Chung, Hoon Taek, Choe, Yong-Kee, Martinez, Ulises, Dumont, Joseph Henry, Monahty, Angela, Bae, Chulsung, Matanovic, Ivana, & Kim, Yu Seung. Effect of Organic Cations on Hydrogen Oxidation Reaction of Carbon Supported Platinum. United States. https://doi.org/10.1149/2.0511614jes
Chung, Hoon Taek, Choe, Yong-Kee, Martinez, Ulises, Dumont, Joseph Henry, Monahty, Angela, Bae, Chulsung, Matanovic, Ivana, and Kim, Yu Seung. Wed .
"Effect of Organic Cations on Hydrogen Oxidation Reaction of Carbon Supported Platinum". United States. https://doi.org/10.1149/2.0511614jes. https://www.osti.gov/servlets/purl/1345940.
@article{osti_1345940,
title = {Effect of Organic Cations on Hydrogen Oxidation Reaction of Carbon Supported Platinum},
author = {Chung, Hoon Taek and Choe, Yong-Kee and Martinez, Ulises and Dumont, Joseph Henry and Monahty, Angela and Bae, Chulsung and Matanovic, Ivana and Kim, Yu Seung},
abstractNote = {Effect of organic cations on hydrogen oxidation reaction (HOR) of carbon supported platinum (Pt/C) is investigated using three 0.1 M alkaline electrolytes, tetramethylammonium hydroxide (TMAOH), tetrabutylammonium hydroxide (TBAOH) and tetrabutylphosphonium hydroxide (TBPOH). Rotating disk electrode experiments indicate that the HOR of Pt/C is adversely impacted by time-dependent and potential-driven chemisorption of organic cations. In-situ infrared reflection adsorption spectroscopy experiments indicated that the specific chemisorption of organic cations drives the hydroxide co-adsorption on Pt surface. The co-adsorption of TMA+ and hydroxide at 0.1 V vs. reversible hydrogen electrode is the strongest; consequently, complete removal of the co-adsorbed layer from Pt surface is difficult even after exposure the Pt surface to 1.2 V. Conversely, the chemisorption of TBP+ is the weakest, yet notable decrease of HOR current density is still observed. The adsorption energies, ΔE, for TMA+, TBA+, and TBP+ on Pt (111) surface from density functional theory are computed to be -2.79, -2.42 and -2.00 eV, respectively. The relatively low adsorption energy of TBP+ is explained by the steric hindrance and electronic effect. This study emphasizes the importance of cationic group on HOR activity of alkaline anion exchange membrane fuel cells.},
doi = {10.1149/2.0511614jes},
journal = {Journal of the Electrochemical Society},
number = 14,
volume = 163,
place = {United States},
year = {Wed Nov 02 00:00:00 EDT 2016},
month = {Wed Nov 02 00:00:00 EDT 2016}
}
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Works referenced in this record:
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Natural population analysis
journal, July 1985
- Reed, Alan E.; Weinstock, Robert B.; Weinhold, Frank
- The Journal of Chemical Physics, Vol. 83, Issue 2
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Decomposition pathways of an alkaline fuel cell membrane material component via evolved gas analysis
journal, July 2008
- Macomber, C. S.; Boncella, J. M.; Pivovar, B. S.
- Journal of Thermal Analysis and Calorimetry, Vol. 93, Issue 1
Differential Capacitance of the Electrical Double Layer in Imidazolium-Based Ionic Liquids: Influence of Potential, Cation Size, and Temperature
journal, April 2008
- Lockett, Vera; Sedev, Rossen; Ralston, John
- The Journal of Physical Chemistry C, Vol. 112, Issue 19
Analysis of Double Layer and Adsorption Effects at the Alkaline Polymer Electrolyte-Electrode Interface
journal, January 2011
- Ünlü, Murat; Abbott, Daniel; Ramaswamy, Nagappan
- Journal of The Electrochemical Society, Vol. 158, Issue 11
Correlating hydrogen oxidation and evolution activity on platinum at different pH with measured hydrogen binding energy
journal, January 2015
- Sheng, Wenchao; Zhuang, Zhongbin; Gao, Minrui
- Nature Communications, Vol. 6, Issue 1
Design and Performance of a New Infrared Reflection Accessory for Spectroelectrochemical Studies
journal, March 1996
- Faguy, Peter W.; Marinković, Nebojša S.
- Applied Spectroscopy, Vol. 50, Issue 3
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Active and stable carbon nanotube/nanoparticle composite electrocatalyst for oxygen reduction
journal, May 2013
- Chung, Hoon T.; Won, Jong H.; Zelenay, Piotr
- Nature Communications, Vol. 4, Issue 1
pH and Alkali Cation Effects on the Pt Cyclic Voltammogram Explained Using Density Functional Theory
journal, December 2015
- McCrum, Ian T.; Janik, Michael J.
- The Journal of Physical Chemistry C, Vol. 120, Issue 1
Improving the hydrogen oxidation reaction rate by promotion of hydroxyl adsorption
journal, February 2013
- Strmcnik, Dusan; Uchimura, Masanobu; Wang, Chao
- Nature Chemistry, Vol. 5, Issue 4
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Theoretical study of CH4 photodissociation on the Pt(111) surface
journal, July 1997
- Akinaga, Yoshinobu; Taketsugu, Tetsuya; Hirao, Kimihiko
- The Journal of Chemical Physics, Vol. 107, Issue 2
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation
journal, September 1992
- Perdew, John P.; Chevary, J. A.; Vosko, S. H.
- Physical Review B, Vol. 46, Issue 11
Cation–Hydroxide–Water Coadsorption Inhibits the Alkaline Hydrogen Oxidation Reaction
journal, October 2016
- Chung, Hoon Taek; Martinez, Ulises; Matanovic, Ivana
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 22
Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992
- Perdew, John P.; Wang, Yue
- Physical Review B, Vol. 45, Issue 23, p. 13244-13249
Density functional theory study of the electrochemical interface between a Pt electrode and an aqueous electrolyte using an implicit solvent method
journal, June 2015
- Sakong, Sung; Naderian, Maryam; Mathew, Kiran
- The Journal of Chemical Physics, Vol. 142, Issue 23
Aerosol-derived Ni1−xZnx electrocatalysts for direct hydrazine fuel cells
journal, January 2012
- Martinez, Ulises; Asazawa, Koichiro; Halevi, Barr
- Physical Chemistry Chemical Physics, Vol. 14, Issue 16
Bamboo-like Carbon Nanotube/Fe 3 C Nanoparticle Hybrids and Their Highly Efficient Catalysis for Oxygen Reduction
journal, January 2015
- Yang, Wenxiu; Liu, Xiangjian; Yue, Xiaoyu
- Journal of the American Chemical Society, Vol. 137, Issue 4
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Solvation Effects on OH Adsorbates on Stepped Pt Surfaces
journal, July 2015
- Jinnouchi, Ryosuke; Nagoya, Akihiro; Kodama, Kensaku
- The Journal of Physical Chemistry C, Vol. 119, Issue 29
Hydrogen Oxidation and Evolution Reaction Kinetics on Platinum: Acid vs Alkaline Electrolytes
journal, January 2010
- Sheng, Wenchao; Gasteiger, Hubert A.; Shao-Horn, Yang
- Journal of The Electrochemical Society, Vol. 157, Issue 11
Density Functional Theory Study of the Alkali Metal Cation Adsorption on Pt(111), Pt(100), and Pt(110) Surfaces
journal, September 2014
- Matanovic, I.; Atanassov, P.; Garzon, F.
- ECS Transactions, Vol. 61, Issue 13
A Microelectrode Study of Interfacial Reactions at the Platinum-Alkaline Polymer Interface
journal, January 2015
- Yim, Sung-Dae; Chung, Hoon T.; Chlistunoff, Jerzy
- Journal of The Electrochemical Society, Vol. 162, Issue 6
Alkaline polymer electrolyte fuel cells completely free from noble metal catalysts
journal, December 2008
- Lu, S.; Pan, J.; Huang, A.
- Proceedings of the National Academy of Sciences, Vol. 105, Issue 52, p. 20611-20614
Platinum Supported on NbRu y O z as Electrocatalyst for Ethanol Oxidation in Acid and Alkaline Fuel Cells
journal, February 2011
- Konopka, Daniel A.; Li, Meng; Artyushkova, Kateryna
- The Journal of Physical Chemistry C, Vol. 115, Issue 7
Works referencing / citing this record:
Quaternary Ammonium Cation Specific Adsorption on Platinum Electrodes: A Combined Experimental and Density Functional Theory Study
journal, January 2018
- McCrum, I. T.; Hickner, M. A.; Janik, M. J.
- Journal of The Electrochemical Society, Vol. 165, Issue 2