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Title: Adsorption of Polyaromatic Backbone Impacts the Performance of Anion Exchange Membrane Fuel Cells

Abstract

The performance of anion exchange membrane fuel cells (AEMFCs) employing Pt or PtRu electrocatalyst and ionomers with different polyaromatic backbones is correlated with the density functional theory (DFT)-calculated adsorption energies of the ionomer fragments on the metal surfaces. The performance of the AEMFCs tested in this work significantly changes depending on the backbone structure of polyaromatic ionomer or the type of the catalyst used at the anode. For the same anode catalyst, the performance decreases in the order poly(fluorene) > poly(p-biphenyl alkylene) > poly(terphenyl alkylene)s, which is in excellent agreement with the decrease in the DFT-calculated interaction energies between the catalyst surface and the corresponding ionomer fragment. Namely, DFT-calculated adsorption energies decrease in the order: p-terphenyl ≥ m-terphenyl > biphenyl > diphenyl ether > benzene ≥ o-terphenyl > 9,9-dimethyl fluorene. The trend in the adsorption energies is explained on the basis of the structural and conformational features of the ionomer fragments. Namely, strong adsorption of the polyaromatic ionomer fragments correlates with the number of benzene rings with a low rotational barrier that can bind parallel to the metal surfaces, leading to strong interaction and hybridization of the aromatic π-orbitals with metal electronic states. Furthermore, the results of this work suggest,more » therefore, that the interaction between the ionomer and electrocatalyst should be taken into account when designing high-performing ionomers even before considering other factors such as hydroxide conductivity, gas permeability, and water uptake of the ionomeric binder.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2];  [3]; ORCiD logo [3]; ORCiD logo [2]
+ Show Author Affiliations
  1. Univ. of New Mexico, Albuquerque, NM (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Rensselaer Polytechnic Institute, Troy, NY (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Oakland, CA (United States); Rensselaer Polytechnic Inst., Troy, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office
OSTI Identifier:
1577485
Grant/Contract Number:  
89233218CNA000001; AC02-05CH11231; AR0000769
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 11; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; chemistry; materials science; hydrocarbons; aromatic compounds; adsorption; phenyls; ionomers

Citation Formats

Matanovic, Ivana, Maurya, Sandip, Park, Eun Joo, Jeon, Jong Yeob, Bae, Chulsung, and Kim, Yu Seung. Adsorption of Polyaromatic Backbone Impacts the Performance of Anion Exchange Membrane Fuel Cells. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b01092.
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Matanovic, Ivana, Maurya, Sandip, Park, Eun Joo, Jeon, Jong Yeob, Bae, Chulsung, & Kim, Yu Seung. Adsorption of Polyaromatic Backbone Impacts the Performance of Anion Exchange Membrane Fuel Cells. United States. https://doi.org/10.1021/acs.chemmater.9b01092
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Matanovic, Ivana, Maurya, Sandip, Park, Eun Joo, Jeon, Jong Yeob, Bae, Chulsung, and Kim, Yu Seung. Wed . "Adsorption of Polyaromatic Backbone Impacts the Performance of Anion Exchange Membrane Fuel Cells". United States. https://doi.org/10.1021/acs.chemmater.9b01092. https://www.osti.gov/servlets/purl/1577485.
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@article{osti_1577485,
title = {Adsorption of Polyaromatic Backbone Impacts the Performance of Anion Exchange Membrane Fuel Cells},
author = {Matanovic, Ivana and Maurya, Sandip and Park, Eun Joo and Jeon, Jong Yeob and Bae, Chulsung and Kim, Yu Seung},
abstractNote = {The performance of anion exchange membrane fuel cells (AEMFCs) employing Pt or PtRu electrocatalyst and ionomers with different polyaromatic backbones is correlated with the density functional theory (DFT)-calculated adsorption energies of the ionomer fragments on the metal surfaces. The performance of the AEMFCs tested in this work significantly changes depending on the backbone structure of polyaromatic ionomer or the type of the catalyst used at the anode. For the same anode catalyst, the performance decreases in the order poly(fluorene) > poly(p-biphenyl alkylene) > poly(terphenyl alkylene)s, which is in excellent agreement with the decrease in the DFT-calculated interaction energies between the catalyst surface and the corresponding ionomer fragment. Namely, DFT-calculated adsorption energies decrease in the order: p-terphenyl ≥ m-terphenyl > biphenyl > diphenyl ether > benzene ≥ o-terphenyl > 9,9-dimethyl fluorene. The trend in the adsorption energies is explained on the basis of the structural and conformational features of the ionomer fragments. Namely, strong adsorption of the polyaromatic ionomer fragments correlates with the number of benzene rings with a low rotational barrier that can bind parallel to the metal surfaces, leading to strong interaction and hybridization of the aromatic π-orbitals with metal electronic states. Furthermore, the results of this work suggest, therefore, that the interaction between the ionomer and electrocatalyst should be taken into account when designing high-performing ionomers even before considering other factors such as hydroxide conductivity, gas permeability, and water uptake of the ionomeric binder.},
doi = {10.1021/acs.chemmater.9b01092},
journal = {Chemistry of Materials},
number = 11,
volume = 31,
place = {United States},
year = {Wed May 22 00:00:00 EDT 2019},
month = {Wed May 22 00:00:00 EDT 2019}
}
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https://doi.org/10.1021/acs.chemmater.9b01092
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    How does a small structural change of anode ionomer make a big difference in alkaline membrane fuel cell performance?
    journal, January 2019

    • Park, Eun Joo; Maurya, Sandip; Lee, Albert S.
    • Journal of Materials Chemistry A, Vol. 7, Issue 43
    • DOI: 10.1039/c9ta10157h

    Ultrafine Pt cluster and RuO 2 heterojunction anode catalysts designed for ultra-low Pt-loading anion exchange membrane fuel cells
    journal, January 2020

    • Wang, Rongyue; Li, Dongguo; Maurya, Sandip
    • Nanoscale Horizons, Vol. 5, Issue 2
    • DOI: 10.1039/c9nh00533a
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