Physical Sciences and Engineering

Hydrogen and Fuel Cell Materials

Hydrogen is a versatile fuel and chemical feedstock for applications such as fuel for stationary and mobile power generation. It can fuel polymer electrolyte fuel cells (PEFC) systems, offering an alternative to conventional energy conversion devices.
Polymer electrolyte fuel cell assembly (H2 + ½ O2 = H2O)

Water electrolyzers are being deployed to store excess electricity in the chemical bonds of hydrogen. Hydrogen can then be used in a variety of applications, such as petroleum refining, ammonia production, and as a fuel for stationary and mobile power generation. Hydrogen is the fuel of choice for many power applications, particularly mobile applications, due to its high energy density per mass of fuel, high conversion efficiency, and ability to be coupled with polymer electrolyte fuel cells (PEFCs) which are high-efficiency energy conversion devices. The major issues impeding the widespread implementation of both water electrolyzers and hydrogen-fueled PEFC power systems are hydrogen fuel cost, hydrogen fueling infrastructure, and PEFC system cost and lifetime. The Hydrogen and Fuel Cell Materials group in CSE has active research projects to develop new materials and enable existing materials to overcome the major barriers to enable cost-competitive use of hydrogen and PEFCs in a variety of applications. 

Hydrogen can play a key role in increasing energy efficiency in many sectors beyond transportation, such as residential and commercial electricity and steel and ammonia production. Hydrogen can be utilized for storage of excess electricity from intermittent sources and from sources such as nuclear energy. To be widely adopted, however, hydrogen must be cost competitive with incumbent fuels.  The current projected cost of hydrogen by low-temperature water electrolysis using a proton-exchange membrane electrolyzers is between 3 and 5 times higher than the cost needed to be widely adopted due to the cost of electricity and the capital cost of the precious metal catalysts.  The Hydrogen and Fuel Cell Materials group has active research projects to develop new materials and enable existing materials to increase the efficiency of electrolyzers, thus reducing contribution of electricity cost to the overall cost of hydrogen and to reduce or completely eliminate the use of precious metals.

This work is primarily funded by the Hydrogen and Fuel Cell Technologies Office (HFTO) in the Department of Energy’s (DOE) Office of Energy Efficiency and Renewable Energy. The focus of HFTO has historically been on the automotive application, where cost competitiveness with the incumbent internal combustion engine requires PEFCs with low loadings of costly platinum-based electrocatalyst. Recently, HFTO’s R&D emphasis has shifted to PEFC systems for heavy duty vehicles, such as long-haul trucks.  In 2020 HFTO established a consortium of five core national laboratories to address PEFC performance and durability for heavy-duty applications called the Million Mile Fuel Cell Truck consortium (M2FCT). The emphasis here is on efficiency (i.e., current density at high voltages) and durability and less on cost.  In 2020, HFTO also established another national laboratory consortium to address the cost, efficiency, and lifetime issues with the production of hydrogen from low and high-temperature electrolysis:  Hydrogen from the Next Generation of Electrolyzers of Water (H2NEW).  This consortium aims to reduce the cost of hydrogen produced by these processes to $2/kg by 2026 and to $1/kg by 2030.

In support of efforts to enable a variety of sources of liquid fuels and chemical feedstocks to enhance energy resiliency, DOE is also exploring processes to convert carbon dioxide into liquid fuels or chemicals. One such process converts captured carbon dioxide to fuels/chemicals such as methanol,  ethanol, isopropanol, and acetone using direct electrochemical reduction. Along with water electrolysis to produce hydrogen, these electrochemical processes can serve as effective means to store and utilize the energy produced from intermittent sources such as solar and wind and from nuclear sources.

Our research addresses the main issues facing the widespread deployment of PEFC power systems and low-temperature water electrolyzers for numerous applications: performance, durability and cost. Additionally, the group is also developing materials and supporting the development of cells for the electrochemical conversion of carbon dioxide to fuels/chemicals. 

PGM Free Catalysts

A major cost contributor to PEFC power systems and low-temperature water electrolysis hydrogen production systems and one of the major sources of efficiency loss for both technologies are the platinum group metal oxygen reduction reaction and oxygen evolution reaction catalysts. To address this issue, the Hydrogen and Fuel Cell Materials group is developing platinum group metal-free (PGM-free) catalysts with the aim of maximizing the active site density, accessibility of the active sites, and the activity and durability of those sites. Among other tools, to achieve these goals, the group is utilizing high-throughput materials synthesis coupled with machine learning,1 characterization2 and equipment and methodologies development for performance evaluation.3 This research takes advantage of the capabilities within CSE’s Accelerated Discovery Laboratory. This activity is a cornerstone of the DOE’s ElectroCat consortium, which is co-led by Argonne and Los Alamos National Laboratory. 

Platinum Alloy Electrocatalysts 

The group also seeks to determine the performance and durability-limiting properties of platinum and platinum alloy catalysts, electrode layer precursor solutions, and electrodes utilizing a combination of in-cell diagnostics and structural analyses, ex situ time-resolved detection of catalyst degradation products, and X-ray scattering, spectroscopy, and tomography techniques at Argonne’s Advanced Photon Source.4-6 The information from these characterizations and the impact of electrode layer composition and precursor solution solvent on the performance and structure is used to inform the design of electrodes with technology-enabling performance and durability for the heavy duty vehicle application.  This work is part of the DOE Hydrogen and Fuel Cell Technologies Office’s Million Mile Fuel Cell Truck Consortium (M2FCT).

Our group is also addressing the limited durability of PEFCs by identifying the mechanisms of catalyst degradation and determining the catalyst, catalyst support properties and operating conditions that limit catalyst lifetime. This research utilizes ex situ, in situ, and operando X-ray absorption and scattering techniques at Argonne’s Advanced Photon Source, aqueous dissolution studies, modeling of platinum dissolution and de-alloying, and modeling of the effect of catalyst degradation on cell performance, in collaboration with Argonne’s Transportation Power Systems.7,8  This work is also part of M2FCT.

Hydrogen Production 

Water electrolysis represents one of the critical technologies for distributed hydrogen production. Barriers to widespread implementation of this hydrogen production technology are cost and lifetime/durability. Due to the sluggish kinetics of the oxygen evolution reaction (OER), high loadings of costly iridium are needed to achieve reasonable electrolyzer efficiency and durability. The group has developed PGM-free OER catalysts to address the cost and durability issues of iridium OER catalysts. These materials are based on porous, stable transition metal composites derived from, for example, cobalt metal organic frameworks incorporated into a 3-D nano-network architecture.9 

The group is also part of the DOE-HFTO ​“Hydrogen from the Next Generation of Electrolyzers of Water” consortium (H2NEW), which aims to lower the cost of hydrogen by improving existing designs and materials of proton exchange membrane, liquid alkaline, and solid oxide water electrolyzers.  The group’s roles in the consortium are to define catalyst, electrode design, and operating conditions to improve the performance and extend the lifetime of the electrolyzers.  We are utilizing a combination of in situ and operando X-ray absorption spectroscopy and scattering coupled with on-line inductively-coupled plasma mass spectrometry techniques to determine the mechanisms of catalyst degradation, to link catalyst atomic structure with performance, and to define the interactions in the catalyst-ionomer ink determining electrode structure and performance.10,11

Carbon Dioxide to Fuel

Our group has developed highly effective and selective transition metal-based catalysts and is studying the fundamental science of the electrochemical conversion of carbon dioxide to chemicals, particularly for those widely used in the chemical industry such as ethanol, ethylene, and formate.12-15 In collaboration with the National Renewable Energy Laboratory, the group is also providing critical information for the development of selective, high efficiency, high current density cells for the conversion of carbon dioxide to fuels, such as formic acid.16 

Citations

  1. Wilton J.M. Kort-Kamp, Magali Ferrandon, Xiaoping Wang, Jae Hyung Park, Rajesh K. Malla, Towfiq Ahmed, Edward F. Holby, Deborah J. Myers, Piotr Zelenay, Journal of Power Sources, 559 (2023) 232583. 
  2. Magali S. Ferrandon, Jae Hyung Park, Xiaoping Wang, Eric Coleman, A. Jeremy Kropf, Deborah J. Myers, Electrochimica Acta, 441 (2023) 141850.
  3. Jae Hyung Park and Deborah J. Myers, Journal of Power Sources, 480 (2020) 228801-228810.
  4. Nagappan Ramaswamy, Swami Kumaraguru, Roland Koestner, Timothy Fuller, Wenbin Gu, Nancy Kariuki, Deborah Myers, Peter J. Dudenas, and Ahmet Kusoglu, Journal of The Electrochemical Society, 168 (2021) 024518.
  5. Deborah J. Myers, A. Jeremy Kropf, Evan C. Wegener, Hemma Mistry, Nancy Kariuki, and Jae Hyung Park, Journal of The Electrochemical Society, 168 (2021) 044510.
  6. Leiming Hu, Tim Van Cleve, Haoran Yu, Jae Hyung Park, Nancy Kariuki, A. Jeremy Kropf, Rangachary Mukundan, David A. Cullen, Deborah J. Myers, and Kenneth C. Neyerlin, Journal of Power Sources, 556 (2023) 232490.
  7. Nancy N. Kariuki and Deborah J. Myers*, Journal of The Electrochemical Society, 168 (2021) 064505.
  8. Firat C. Cetinbas, Rajesh K. Ahluwalia, Nancy N. Kariuki, Vincent De Andrade, and Deborah J. Myers, Journal of the Electrochemical Society, 167 (2020) 013508-013516.
  9. Lina Chong, Guoping Gao, Jianguo Wen, Haixia Li, Haiping Xu, Zach Greem, Joshua D. Sugar, A. Jeremy Kropf, Wenqian Xu, Xiao-Min Lin, Hui Xu, Lin-Wang Wang, and Di-Jia Liu, Science, 380 (2023) 609-616.
  10. Sunil Khandavalli, Jae Hyung Park, Robin Rice, Diana Y. Zhang, Sarah A. Berlinger, Guido Bender, Deborah J. Myers, Michael Ulsh, Scott A. Mauger, Soft Matter, 20(45) (2024) 9028-9049.
  11. Shaun M. Alia, Kimberly S. Reeves, David A. Cullen, Haoran Yu, A. Jeremy Kropf, Nancy N. Kariuki, Jae Hyung Park, Journal of The Electrochemical Society, 171(4) (2024) 044503.
  12. Haiping Xu, Dominic Rebollar, Haiying He, Lina Chong, Yuzi Liu, Cong Liu, Cheng-Jun Sun, Tao Li, John V. Muntean, Randall E. Winans, Di-Jia Liu, and Tao Xu, Nature Energy, 5 (2020) 623-632.
  13. Shichen Guo, Jianxin Wang, Haozhe Zhang, Chukwunwike O. Iloeje, Di-Jia Liu, ACS Energy Letter, 10 (2025) 600.
  14. Haiping Xu, Haiying He, Jianxin Wang, Inhui Hwang, Yuzi Liu, Chengjun Sun, Tao Li, John V. Muntean, Tao Xu, Di-Jia Liu,  J. Am. Chem. Soc., 146 (2024)10357−10366.
  15. Di-Jia Liu, Joule, 6 (2022) 1969–1980.
  16. Leiming Hu, Jacob A. Wrubel, Carlos M. Baez-Cotto, Fry Intia, Jae Hyung Park, A. Jeremy Kropf, Nancy N. Kariuki, , Zhe Huang, Ahmed Farghaly, Lynda Amichi, Prantik Saha, Ling Tao, David A. Cullen, Deborah J. Myers, Magali S. Ferrandon, and K.C. Neyerlin, Nature Communications, 14 (1) (2023) 7605.