Poly(aryl piperidinium) membranes and ionomers for hydroxide exchange membrane fuel cells
Abstract
One promising approach to reduce the cost of fuel cell systems is to develop hydroxide exchange membrane fuel cells (HEMFCs), which open up the possibility of platinum-group-metal-free catalysts and low-cost bipolar plates. However, scalable alkaline polyelectrolytes (hydroxide exchange membranes and hydroxide exchange ionomers), a key component of HEMFCs, with desired properties are currently unavailable, which presents a major barrier to the development of HEMFCs. Here we show hydroxide exchange membranes and hydroxide exchange ionomers based on poly(aryl piperidinium) (PAP) that simultaneously possess adequate ionic conductivity, chemical stability, mechanical robustness, gas separation and selective solubility. Here, these properties originate from the combination of the piperidinium cation and the rigid ether-bond-free aryl backbone. A low-Pt membrane electrode assembly with a Ag-based cathode using PAP materials showed an excellent peak power density of 920 mW cm-2 and operated stably at a constant current density of 500 mA cm-2 for 300 h with H2/CO2-free air at 95 °C.
- Authors:
-
- Univ. of Delaware, Newark, DE (United States)
- Elbit Systems Ltd, Caesarea (Israel)
- Publication Date:
- Research Org.:
- Univ. of Delaware, Newark, DE (United States)
- Sponsoring Org.:
- USDOE Advanced Research Projects Agency - Energy (ARPA-E)
- OSTI Identifier:
- 1545542
- Grant/Contract Number:
- AR0000771
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Energy
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 5; Journal ID: ISSN 2058-7546
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE
Citation Formats
Wang, Junhua, Zhao, Yun, Setzler, Brian P., Rojas-Carbonell, Santiago, Ben Yehuda, Chaya, Amel, Alina, Page, Miles, Wang, Lan, Hu, Keda, Shi, Lin, Gottesfeld, Shimshon, Xu, Bingjun, and Yan, Yushan. Poly(aryl piperidinium) membranes and ionomers for hydroxide exchange membrane fuel cells. United States: N. p., 2019.
Web. doi:10.1038/s41560-019-0372-8.
Wang, Junhua, Zhao, Yun, Setzler, Brian P., Rojas-Carbonell, Santiago, Ben Yehuda, Chaya, Amel, Alina, Page, Miles, Wang, Lan, Hu, Keda, Shi, Lin, Gottesfeld, Shimshon, Xu, Bingjun, & Yan, Yushan. Poly(aryl piperidinium) membranes and ionomers for hydroxide exchange membrane fuel cells. United States. https://doi.org/10.1038/s41560-019-0372-8
Wang, Junhua, Zhao, Yun, Setzler, Brian P., Rojas-Carbonell, Santiago, Ben Yehuda, Chaya, Amel, Alina, Page, Miles, Wang, Lan, Hu, Keda, Shi, Lin, Gottesfeld, Shimshon, Xu, Bingjun, and Yan, Yushan. Mon .
"Poly(aryl piperidinium) membranes and ionomers for hydroxide exchange membrane fuel cells". United States. https://doi.org/10.1038/s41560-019-0372-8. https://www.osti.gov/servlets/purl/1545542.
@article{osti_1545542,
title = {Poly(aryl piperidinium) membranes and ionomers for hydroxide exchange membrane fuel cells},
author = {Wang, Junhua and Zhao, Yun and Setzler, Brian P. and Rojas-Carbonell, Santiago and Ben Yehuda, Chaya and Amel, Alina and Page, Miles and Wang, Lan and Hu, Keda and Shi, Lin and Gottesfeld, Shimshon and Xu, Bingjun and Yan, Yushan},
abstractNote = {One promising approach to reduce the cost of fuel cell systems is to develop hydroxide exchange membrane fuel cells (HEMFCs), which open up the possibility of platinum-group-metal-free catalysts and low-cost bipolar plates. However, scalable alkaline polyelectrolytes (hydroxide exchange membranes and hydroxide exchange ionomers), a key component of HEMFCs, with desired properties are currently unavailable, which presents a major barrier to the development of HEMFCs. Here we show hydroxide exchange membranes and hydroxide exchange ionomers based on poly(aryl piperidinium) (PAP) that simultaneously possess adequate ionic conductivity, chemical stability, mechanical robustness, gas separation and selective solubility. Here, these properties originate from the combination of the piperidinium cation and the rigid ether-bond-free aryl backbone. A low-Pt membrane electrode assembly with a Ag-based cathode using PAP materials showed an excellent peak power density of 920 mW cm-2 and operated stably at a constant current density of 500 mA cm-2 for 300 h with H2/CO2-free air at 95 °C.},
doi = {10.1038/s41560-019-0372-8},
journal = {Nature Energy},
number = 5,
volume = 4,
place = {United States},
year = {2019},
month = {4}
}
Web of Science
Works referenced in this record:
Poly( N , N -diallylazacycloalkane)s for Anion-Exchange Membranes Functionalized with N -Spirocyclic Quaternary Ammonium Cations
journal, March 2017
- Olsson, Joel S.; Pham, Thanh Huong; Jannasch, Patric
- Macromolecules, Vol. 50, Issue 7
Prospects for Alkaline Anion-Exchange Membranes in Low Temperature Fuel Cells
journal, October 2004
- Varcoe, J.; Slade, R.
- Fuel Cells, Vol. 5, Issue 2, p. 187-200
Aromatic Polymers Incorporating Bis- N -spirocyclic Quaternary Ammonium Moieties for Anion-Exchange Membranes
journal, November 2015
- Pham, Thanh Huong; Jannasch, Patric
- ACS Macro Letters, Vol. 4, Issue 12
Toyota MIRAI Fuel Cell Vehicle and Progress Toward a Future Hydrogen Society
journal, January 2015
- Yoshida, T.; Kojima, K.
- Interface magazine, Vol. 24, Issue 2
Review of cell performance in anion exchange membrane fuel cells
journal, January 2018
- Dekel, Dario R.
- Journal of Power Sources, Vol. 375
Robust Hydroxide Ion Conducting Poly(biphenyl alkylene)s for Alkaline Fuel Cell Membranes
journal, July 2015
- Lee, Woo-Hyung; Kim, Yu Seung; Bae, Chulsung
- ACS Macro Letters, Vol. 4, Issue 8
Alkaline polymer electrolyte fuel cells stably working at 80 °C
journal, June 2018
- Peng, Hanqing; Li, Qihao; Hu, Meixue
- Journal of Power Sources, Vol. 390
Highly Stable, Anion Conductive, Comb-Shaped Copolymers for Alkaline Fuel Cells
journal, June 2013
- Li, Nanwen; Leng, Yongjun; Hickner, Michael A.
- Journal of the American Chemical Society, Vol. 135, Issue 27
Synthesis and Characterization of Poly(phenylene)-Based Anion Exchange Membranes for Alkaline Fuel Cells
journal, November 2009
- Hibbs, Michael R.; Fujimoto, Cy H.; Cornelius, Christopher J.
- Macromolecules, Vol. 42, Issue 21, p. 8316-8321
Alkaline Stability of Quaternary Ammonium Cations for Alkaline Fuel Cell Membranes and Ionic Liquids
journal, November 2014
- Marino, M. G.; Kreuer, K. D.
- ChemSusChem, Vol. 8, Issue 3
Two-dimensional NMR spectroscopy reveals cation-triggered backbone degradation in polysulfone-based anion exchange membranes
journal, January 2013
- Arges, C. G.; Ramani, V.
- Proceedings of the National Academy of Sciences, Vol. 110, Issue 7
Imidazolium Cations with Exceptional Alkaline Stability: A Systematic Study of Structure–Stability Relationships
journal, July 2015
- Hugar, Kristina M.; Kostalik, Henry A.; Coates, Geoffrey W.
- Journal of the American Chemical Society, Vol. 137, Issue 27
Fluorene-Based Hydroxide Ion Conducting Polymers for Chemically Stable Anion Exchange Membrane Fuel Cells
journal, April 2015
- Lee, Woo-Hyung; Mohanty, Angela D.; Bae, Chulsung
- ACS Macro Letters, Vol. 4, Issue 4
Anion Conductive Block Poly(arylene ether)s: Synthesis, Properties, and Application in Alkaline Fuel Cells
journal, July 2011
- Tanaka, Manabu; Fukasawa, Keita; Nishino, Eriko
- Journal of the American Chemical Society, Vol. 133, Issue 27, p. 10646-10654
A Novel, One-Pot Synthesis of Novel 3F, 5F, and 8F Aromatic Polymers
journal, January 2007
- Diaz, Adan M.; Zolotukhin, Mikhail G.; Fomine, Serguei
- Macromolecular Rapid Communications, Vol. 28, Issue 2
A high conductivity ultrathin anion-exchange membrane with 500+ h alkali stability for use in alkaline membrane fuel cells that can achieve 2 W cm −2 at 80 °C
journal, January 2018
- Wang, Lianqin; Bellini, Marco; Miller, Hamish A.
- Journal of Materials Chemistry A, Vol. 6, Issue 31
Co3O4 nanocrystals on graphene as a synergistic catalyst for oxygen reduction reaction
journal, August 2011
- Liang, Yongye; Li, Yanguang; Wang, Hailiang
- Nature Materials, Vol. 10, Issue 10, p. 780-786
Stabilizing the Imidazolium Cation in Hydroxide-Exchange Membranes for Fuel Cells
journal, August 2013
- Wang, Junhua; Gu, Shuang; Kaspar, Robert B.
- ChemSusChem, Vol. 6, Issue 11
Phosphonium-Functionalized Polyethylene: A New Class of Base-Stable Alkaline Anion Exchange Membranes
journal, October 2012
- Noonan, Kevin J. T.; Hugar, Kristina M.; Kostalik, Henry A.
- Journal of the American Chemical Society, Vol. 134, Issue 44
High performance aliphatic-heterocyclic benzyl-quaternary ammonium radiation-grafted anion-exchange membranes
journal, January 2016
- Ponce-González, Julia; Whelligan, Daniel K.; Wang, Lianqin
- Energy & Environmental Science, Vol. 9, Issue 12
High-Performance Alkaline Polymer Electrolyte for Fuel Cell Applications
journal, January 2010
- Pan, Jing; Lu, Shanfu; Li, Yan
- Advanced Functional Materials, Vol. 20, Issue 2
Alkali-stable and highly anion conducting poly(phenylene oxide)s carrying quaternary piperidinium cations
journal, January 2016
- Dang, Hai-Son; Jannasch, Patric
- Journal of Materials Chemistry A, Vol. 4, Issue 30
Systematic Alkaline Stability Study of Polymer Backbones for Anion Exchange Membrane Applications
journal, April 2016
- Mohanty, Angela D.; Tignor, Steven E.; Krause, Jessica A.
- Macromolecules, Vol. 49, Issue 9
Ionomeric Poly(phenylene) Prepared by Diels−Alder Polymerization: Synthesis and Physical Properties of a Novel Polyelectrolyte
journal, June 2005
- Fujimoto, Cy H.; Hickner, Michael A.; Cornelius, Christopher J.
- Macromolecules, Vol. 38, Issue 12, p. 5010-5016
Precision Synthesis of Narrow Polydispersity, Ultrahigh Molecular Weight Linear Aromatic Polymers by A 2 + B 2 Nonstoichiometric Step-Selective Polymerization
journal, August 2012
- Cruz, Alfredo R.; Hernandez, M. Carmen G.; Guzmán-Gutiérrez, Maria T.
- Macromolecules, Vol. 45, Issue 17
A class of non-precious metal composite catalysts for fuel cells
journal, September 2006
- Bashyam, Rajesh; Zelenay, Piotr
- Nature, Vol. 443, Issue 7107
Metal-Cation-Based Anion Exchange Membranes
journal, March 2012
- Zha, Yongping; Disabb-Miller, Melanie L.; Johnson, Zachary D.
- Journal of the American Chemical Society, Vol. 134, Issue 10
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
journal, April 2011
- Wu, G.; More, K. L.; Johnston, C. M.
- Science, Vol. 332, Issue 6028, p. 443-447
Backbone stability of quaternized polyaromatics for alkaline membrane fuel cells
journal, December 2012
- Fujimoto, Cy; Kim, Dae-Sik; Hibbs, Michael
- Journal of Membrane Science, Vol. 423-424, p. 438-449
Structure-Property Relationships in Hydroxide-Exchange Membranes with Cation Strings and High Ion-Exchange Capacity
journal, December 2015
- Wang, Junhua; Gu, Shuang; Xiong, Ruichang
- ChemSusChem, Vol. 8, Issue 24
Just a Dream—or Future Reality?
journal, April 2009
- Gasteiger, Hubert A.; Marković, Nenad M
- Science, Vol. 324, Issue 5923, p. 48-49
Anion-exchange membranes in electrochemical energy systems
journal, January 2014
- Varcoe, John R.; Atanassov, Plamen; Dekel, Dario R.
- Energy & Environmental Science, Vol. 7, Issue 10, p. 3135-3191
Base stable poly(diallylpiperidinium hydroxide) multiblock copolymers for anion exchange membranes
journal, January 2017
- Strasser, Derek J.; Graziano, Brendan J.; Knauss, Daniel M.
- Journal of Materials Chemistry A, Vol. 5, Issue 20
Effect of Water on the Stability of Quaternary Ammonium Groups for Anion Exchange Membrane Fuel Cell Applications
journal, May 2017
- Dekel, Dario R.; Amar, Michal; Willdorf, Sapir
- Chemistry of Materials, Vol. 29, Issue 10
A Soluble and Highly Conductive Ionomer for High-Performance Hydroxide Exchange Membrane Fuel Cells
journal, August 2009
- Gu, Shuang; Cai, Rui; Luo, Ting
- Angewandte Chemie International Edition, Vol. 48, Issue 35, p. 6499-6502
Novel Hydroxide-Conducting Polyelectrolyte Composed of an Poly(arylene ether sulfone) Containing Pendant Quaternary Guanidinium Groups for Alkaline Fuel Cell Applications
journal, April 2010
- Wang, Junhua; Li, Shenghai; Zhang, Suobo
- Macromolecules, Vol. 43, Issue 8, p. 3890-3896
Manipulating Water in High-Performance Hydroxide Exchange Membrane Fuel Cells through Asymmetric Humidification and Wetproofing
journal, January 2015
- Kaspar, Robert B.; Letterio, Michael P.; Wittkopf, Jarrid A.
- Journal of The Electrochemical Society, Vol. 162, Issue 6
Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells
journal, April 2009
- Lefèvre, Michel; Proietti, Eric; Jaouen, Frédéric
- Science, Vol. 324, Issue 5923, p. 71-74
Factors Enhancing the Reactivity of Carbonyl Compounds for Polycondensations with Aromatic Hydrocarbons. A Computational Study
journal, August 2004
- Peña, Estrella Ramos; Zolotukhin, Mikhail; Fomine, Serguei
- Macromolecules, Vol. 37, Issue 16
Polyethylene-Based Block Copolymers for Anion Exchange Membranes
journal, September 2015
- Li, Yifan; Liu, Ye; Savage, Alice M.
- Macromolecules, Vol. 48, Issue 18
Constructing ionic highway in alkaline polymer electrolytes
journal, January 2014
- Pan, Jing; Chen, Chen; Li, Yao
- Energy Environ. Sci., Vol. 7, Issue 1
Synthesis of Soluble Poly(arylene ether sulfone) Ionomers with Pendant Quaternary Ammonium Groups for Anion Exchange Membranes
journal, November 2009
- Wang, Junhua; Zhao, Zhuo; Gong, Feixiang
- Macromolecules, Vol. 42, Issue 22, p. 8711-8717
Alkaline polymer electrolyte membranes for fuel cell applications
journal, January 2013
- Wang, Yan-Jie; Qiao, Jinli; Baker, Ryan
- Chemical Society Reviews, Vol. 42, Issue 13
N -Spirocyclic Quaternary Ammonium Ionenes for Anion-Exchange Membranes
journal, February 2017
- Pham, Thanh Huong; Olsson, Joel S.; Jannasch, Patric
- Journal of the American Chemical Society, Vol. 139, Issue 8
Comb-shaped polymers to enhance hydroxide transport in anion exchange membranes
journal, January 2012
- Li, Nanwen; Yan, Tingzi; Li, Zheng
- Energy & Environmental Science, Vol. 5, Issue 7
Activity targets for nanostructured platinum-group-metal-free catalysts in hydroxide exchange membrane fuel cells
journal, December 2016
- Setzler, Brian P.; Zhuang, Zhongbin; Wittkopf, Jarrid A.
- Nature Nanotechnology, Vol. 11, Issue 12
A Soluble and Highly Conductive Ionomer for High-Performance Hydroxide Exchange Membrane Fuel Cells
journal, August 2009
- Gu, Shuang; Cai, Rui; Luo, Ting
- Angewandte Chemie, Vol. 121, Issue 35
Works referencing / citing this record:
Molecular Design of Single‐Atom Catalysts for Oxygen Reduction Reaction
journal, February 2020
- Wan, Chengzhang; Duan, Xiangfeng; Huang, Yu
- Advanced Energy Materials, Vol. 10, Issue 14
Enhanced Electrocatalytic Hydrogen Oxidation on Ni/NiO/C Derived from a Nickel‐Based Metal–Organic Framework
journal, June 2019
- Yang, Yang; Sun, Xiaodong; Han, Guanqun
- Angewandte Chemie, Vol. 131, Issue 31
Understanding the pH Dependence of Underpotential Deposited Hydrogen on Platinum
journal, October 2019
- Yang, Xuan; Nash, Jared; Oliveira, Nicholas
- Angewandte Chemie, Vol. 131, Issue 49
Enhanced Electrocatalytic Hydrogen Oxidation on Ni/NiO/C Derived from a Nickel-Based Metal-Organic Framework
journal, June 2019
- Yang, Yang; Sun, Xiaodong; Han, Guanqun
- Angewandte Chemie International Edition, Vol. 58, Issue 31
Understanding the pH Dependence of Underpotential Deposited Hydrogen on Platinum
journal, December 2019
- Yang, Xuan; Nash, Jared; Oliveira, Nicholas
- Angewandte Chemie International Edition, Vol. 58, Issue 49
Radiation-grafted anion-exchange membranes: the switch from low- to high-density polyethylene leads to remarkably enhanced fuel cell performance
journal, January 2019
- Wang, Lianqin; Peng, Xiong; Mustain, William E.
- Energy & Environmental Science, Vol. 12, Issue 5
Quantifying and elucidating the effect of CO 2 on the thermodynamics, kinetics and charge transport of AEMFCs
journal, January 2019
- Zheng, Yiwei; Omasta, Travis J.; Peng, Xiong
- Energy & Environmental Science, Vol. 12, Issue 9
Partially fluorinated copolymers containing pendant piperidinium head groups as anion exchange membranes for alkaline fuel cells
journal, January 2019
- Koronka, Daniel; Matsumoto, Akinobu; Otsuji, Kanji
- RSC Advances, Vol. 9, Issue 64
Effects of the N -alicyclic cation and backbone structures on the performance of poly(terphenyl)-based hydroxide exchange membranes
journal, January 2019
- Pham, Thanh Huong; Olsson, Joel S.; Jannasch, Patric
- Journal of Materials Chemistry A, Vol. 7, Issue 26
Ether-free polyfluorenes tethered with quinuclidinium cations as hydroxide exchange membranes
journal, January 2019
- Allushi, Andrit; Pham, Thanh Huong; Olsson, Joel S.
- Journal of Materials Chemistry A, Vol. 7, Issue 47
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
High-Performance Hydroxide Exchange Membrane Fuel Cells through Optimization of Relative Humidity, Backpressure and Catalyst Selection
journal, January 2019
- Wang, Teng; Shi, Lin; Wang, Junhua
- Journal of The Electrochemical Society, Vol. 166, Issue 7