Use of a segmented cell for the combinatorial development of platinum group metal-free electrodes for polymer electrolyte fuel cells

Osmieri, Luigi; Mauger, Scott A.; Ulsh, Michael J.; Neyerlin, Kenneth C.; Bender, Guido

doi:10.1016/j.jpowsour.2020.227829

Title: Use of a segmented cell for the combinatorial development of platinum group metal-free electrodes for polymer electrolyte fuel cells

Journal Article · Fri Feb 07 00:00:00 UTC 2020 · Journal of Power Sources

DOI: https://doi.org/10.1016/j.jpowsour.2020.227829 · OSTI ID:1602179

Osmieri, Luigi ^[1];

^[1];

^[1]; Neyerlin, Kenneth C. ^[1]; Bender, Guido ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)

The development of novel platinum group metal (PGM)-free catalysts is a difficult task, particularly when coupled with the integration into a cathode catalyst layer (CCL). The optimization of such PGM-free electrode structures is often non-linear and iterative, making it a demanding task due to the high number of parameters that affect performance. To accelerate both materials discovery and electrode development, this work demonstrates the application of a high-resolution segmented cell (SC) with 121 segments of 0.413 cm² size for combinatorial high-throughput PGM-free catalyst screening and CCL optimization. The approach utilizes three flow-field strips with active areas of 4.45 cm² each, distributed over 11 segments. Electrodes with identical catalyst material and fabrication method result in reproducible data with typically less than 10% variation between each segment and match in performance with differential single cell data. High throughput testing of combinatorial sample sets, with varied PGM-free electrocatalyst materials or electrode composition, demonstrated the ability to rapidly discern high performing outliers, and establish or confirm trends in electrode optimization. The results indicated significant performance benefits of electrodes with ionomer content of 45 wt% over lower values, and of water rich inks with 82% water content over those with 50%.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Program (EE-3F)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1602179

Report Number(s):: NREL/JA--5900-76033

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Journal Issue: C Vol. 452; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (55)

Integrating PGM‐Free Catalysts into Catalyst Layers and Proton Exchange Membrane Fuel Cell Devices Banham, Dustin; Choi, Ja‐Yeon; Kishimoto, Takeaki Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201804846	journal	December 2018
Progress in the Development of Fe‐Based PGM‐Free Electrocatalysts for the Oxygen Reduction Reaction Martinez, Ulises; Komini Babu, Siddharth; Holby, Edward F. Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201806545	journal	December 2018
Doped Interlayers for Improved Selectivity in Bulk Heterojunction Organic Photovoltaic Devices Mauger, Scott A.; Glasser, Melodie P.; Tremolet de Villers, Bertrand J. Advanced Materials Interfaces, Vol. 3, Issue 2 https://doi.org/10.1002/admi.201500346	journal	November 2015
Analysis of the Microstructure Formation Process and Its Influence on the Performance of Polymer Electrolyte Fuel-Cell Catalyst Layers Takahashi, Shinichi; Mashio, Tetsuya; Horibe, Norifumi ChemElectroChem, Vol. 2, Issue 10 https://doi.org/10.1002/celc.201500131	journal	July 2015
Electrospun Fiber Mat Cathode with Platinum‐Group‐Metal‐Free Catalyst Powder and Nafion/PVDF Binder Slack, John; Halevi, Barr; McCool, Geoff ChemElectroChem, Vol. 5, Issue 12 https://doi.org/10.1002/celc.201800283	journal	April 2018
Utilizing a Segmented Fuel Cell to Study the Effects of Electrode Coating Irregularities on PEM Fuel Cell Initial Performance Phillips, A.; Ulsh, M.; Porter, J. Fuel Cells, Vol. 17, Issue 3 https://doi.org/10.1002/fuce.201600214	journal	April 2017
Nafion content in the catalyst layer of polymer electrolyte fuel cells: effects on structure and performance Passalacqua, E.; Lufrano, F.; Squadrito, G. Electrochimica Acta, Vol. 46, Issue 6 https://doi.org/10.1016/S0013-4686(00)00679-4	journal	January 2001
Evaluation of current distribution in a proton exchange membrane fuel cell by segmented cell approach Rajalakshmi, N. Journal of Power Sources, Vol. 112, Issue 1 https://doi.org/10.1016/S0378-7753(02)00352-X	journal	October 2002
Low Pt loading high performance cathodes for PEM fuel cells Qi, Zhigang; Kaufman, Arthur Journal of Power Sources, Vol. 113, Issue 1, p. 37-43 https://doi.org/10.1016/S0378-7753(02)00477-9	journal	January 2003
Further refinements in the segmented cell approach to diagnosing performance in polymer electrolyte fuel cells Bender, Guido; Wilson, Mahlon S.; Zawodzinski, Thomas A. Journal of Power Sources, Vol. 123, Issue 2 https://doi.org/10.1016/S0378-7753(03)00533-0	journal	September 2003
Performance of catalyst layers of polymer electrolyte fuel cells: exact solutions Kulikovsky, A. Electrochemistry Communications, Vol. 4, Issue 4 https://doi.org/10.1016/S1388-2481(02)00275-8	journal	April 2002
Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs Gasteiger, Hubert A.; Kocha, Shyam S.; Sompalli, Bhaskar Applied Catalysis B: Environmental, Vol. 56, Issue 1-2, p. 9-35 https://doi.org/10.1016/j.apcatb.2004.06.021	journal	March 2005
Performance of a Fe-N-C catalyst for the oxygen reduction reaction in direct methanol fuel cell: Cathode formulation optimization and short-term durability Osmieri, Luigi; Escudero-Cid, Ricardo; Monteverde Videla, Alessandro H. A. Applied Catalysis B: Environmental, Vol. 201 https://doi.org/10.1016/j.apcatb.2016.08.043	journal	February 2017
Elucidation of Fe-N-C electrocatalyst active site functionality via in-situ X-ray absorption and operando determination of oxygen reduction reaction kinetics in a PEFC Osmieri, Luigi; Ahluwalia, Rajesh K.; Wang, Xiaohua Applied Catalysis B: Environmental, Vol. 257 https://doi.org/10.1016/j.apcatb.2019.117929	journal	November 2019
Durability challenges and perspective in the development of PGM-free electrocatalysts for the oxygen reduction reaction Martinez, Ulises; Komini Babu, Siddharth; Holby, Edward F. Current Opinion in Electrochemistry, Vol. 9 https://doi.org/10.1016/j.coelec.2018.04.010	journal	June 2018
Application of a segmented cell setup to detect pinhole and catalyst loading defects in proton exchange membrane fuel cells Reshetenko, Tatyana V.; Bender, Guido; Bethune, Keith Electrochimica Acta, Vol. 76 https://doi.org/10.1016/j.electacta.2012.04.138	journal	August 2012
Experimental investigation of PEM fuel cell aging under current cycling using segmented fuel cell Weng, Fang-Bor; Hsu, Chun-Ying; Li, Chun-Wei International Journal of Hydrogen Energy, Vol. 35, Issue 8 https://doi.org/10.1016/j.ijhydene.2010.01.065	journal	April 2010
Non precious metal catalysts for the PEM fuel cell cathode Othman, Rapidah; Dicks, Andrew L.; Zhu, Zhonghua International Journal of Hydrogen Energy, Vol. 37, Issue 1 https://doi.org/10.1016/j.ijhydene.2011.08.095	journal	January 2012
Effect of operating conditions on current density distribution and high frequency resistance in a segmented PEM fuel cell Gerteisen, Dietmar; Zamel, Nada; Sadeler, Christian International Journal of Hydrogen Energy, Vol. 37, Issue 9 https://doi.org/10.1016/j.ijhydene.2012.02.024	journal	May 2012
The effects of operating temperature on current density distribution and impedance spectroscopy by segmented fuel cell Tang, Wenchao; Lin, Rui; Weng, Yuanming International Journal of Hydrogen Energy, Vol. 38, Issue 25 https://doi.org/10.1016/j.ijhydene.2013.01.099	journal	August 2013
PEM fuel cell electrodes Litster, S.; McLean, G. Journal of Power Sources, Vol. 130, Issue 1-2 https://doi.org/10.1016/j.jpowsour.2003.12.055	journal	May 2004
Segmented cells as tool for development of fuel cells and error prevention/prediagnostic in fuel cell stacks Schulze, M.; Gülzow, E.; Schönbauer, St. Journal of Power Sources, Vol. 173, Issue 1 https://doi.org/10.1016/j.jpowsour.2007.03.055	journal	November 2007
Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells Nallathambi, Vijayadurga; Lee, Jong-Won; Kumaraguru, Swaminatha P. Journal of Power Sources, Vol. 183, Issue 1, p. 34-42 https://doi.org/10.1016/j.jpowsour.2008.05.020	journal	August 2008
Nitrogen-modified carbon-based catalysts for oxygen reduction reaction in polymer electrolyte membrane fuel cells Subramanian, Nalini P.; Li, Xuguang; Nallathambi, Vijayadurda Journal of Power Sources, Vol. 188, Issue 1, p. 38-44 https://doi.org/10.1016/j.jpowsour.2008.11.087	journal	March 2009
New insights into non-precious metal catalyst layer designs for proton exchange membrane fuel cells: Improving performance and stability Banham, Dustin; Kishimoto, Takeaki; Sato, Tetsutaro Journal of Power Sources, Vol. 344 https://doi.org/10.1016/j.jpowsour.2017.01.086	journal	March 2017
Enhanced Fe dispersion via “pinning” effect of thiocyanate ion on ferric ion in Fe-N-S-doped catalyst as an excellent oxygen reduction reaction electrode Shu, Chengyong; Chen, Yuanzhen; Yang, Xiao-Dong Journal of Power Sources, Vol. 376 https://doi.org/10.1016/j.jpowsour.2017.11.093	journal	February 2018
Directly converting Fe-doped metal–organic frameworks into highly active and stable Fe-N-C catalysts for oxygen reduction in acid Wang, Xiaojuan; Zhang, Hanguang; Lin, Honghong Nano Energy, Vol. 25 https://doi.org/10.1016/j.nanoen.2016.04.042	journal	July 2016
ElectroCat: DOE's approach to PGM-free catalyst and electrode R&D Thompson, Simon T.; Wilson, Adria R.; Zelenay, Piotr Solid State Ionics, Vol. 319 https://doi.org/10.1016/j.ssi.2018.01.030	journal	June 2018
Recent Advances in Electrocatalysts for Oxygen Reduction Reaction Shao, Minhua; Chang, Qiaowan; Dodelet, Jean-Pol Chemical Reviews, Vol. 116, Issue 6 https://doi.org/10.1021/acs.chemrev.5b00462	journal	February 2016
The Priority and Challenge of High-Power Performance of Low-Platinum Proton-Exchange Membrane Fuel Cells Kongkanand, Anusorn; Mathias, Mark F. The Journal of Physical Chemistry Letters, Vol. 7, Issue 7 https://doi.org/10.1021/acs.jpclett.6b00216	journal	March 2016
Resolving Electrode Morphology’s Impact on Platinum Group Metal-Free Cathode Performance Using Nano-CT of 3D Hierarchical Pore and Ionomer Distribution Komini Babu, Siddharth; Chung, Hoon T.; Zelenay, Piotr ACS Applied Materials & Interfaces, Vol. 8, Issue 48 https://doi.org/10.1021/acsami.6b08844	journal	November 2016
Elucidating the Dynamic Nature of Fuel Cell Electrodes as a Function of Conditioning: An ex Situ Material Characterization and in Situ Electrochemical Diagnostic Study Kabir, Sadia; Myers, Deborah J.; Kariuki, Nancy ACS Applied Materials & Interfaces, Vol. 11, Issue 48 https://doi.org/10.1021/acsami.9b11365	journal	November 2019
Dictating Pt-Based Electrocatalyst Performance in Polymer Electrolyte Fuel Cells, from Formulation to Application Van Cleve, Tim; Khandavalli, Sunilkumar; Chowdhury, Anamika ACS Applied Materials & Interfaces, Vol. 11, Issue 50 https://doi.org/10.1021/acsami.9b17614	journal	November 2019
Current Status and Future Development of Catalyst Materials and Catalyst Layers for Proton Exchange Membrane Fuel Cells: An Industrial Perspective Banham, Dustin; Ye, Siyu ACS Energy Letters, Vol. 2, Issue 3 https://doi.org/10.1021/acsenergylett.6b00644	journal	February 2017
Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation Zhang, Hanguang; Hwang, Sooyeon; Wang, Maoyu Journal of the American Chemical Society, Vol. 139, Issue 40 https://doi.org/10.1021/jacs.7b06514	journal	September 2017
Platinum group metal-free catalysts boost cost competitiveness of fuel cell vehicles Thompson, Simon T.; Papageorgopoulos, Dimitrios Nature Catalysis, Vol. 2, Issue 7 https://doi.org/10.1038/s41929-019-0291-x	journal	July 2019
Is the rapid initial performance loss of Fe/N/C non precious metal catalysts due to micropore flooding? Choi, Ja-Yeon; Yang, Lijun; Kishimoto, Takeaki Energy & Environmental Science, Vol. 10, Issue 1 https://doi.org/10.1039/C6EE03005J	journal	January 2017
Advancements in rationally designed PGM-free fuel cell catalysts derived from metal–organic frameworks Barkholtz, Heather M.; Liu, Di-Jia Materials Horizons, Vol. 4, Issue 1 https://doi.org/10.1039/C6MH00344C	journal	January 2017
The Achilles' heel of iron-based catalysts during oxygen reduction in an acidic medium Choi, Chang Hyuck; Lim, Hyung-Kyu; Chung, Min Wook Energy & Environmental Science, Vol. 11, Issue 11 https://doi.org/10.1039/C8EE01855C	journal	January 2018
Highly active atomically dispersed CoN ₄ fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy He, Yanghua; Hwang, Sooyeon; Cullen, David A. Energy & Environmental Science, Vol. 12, Issue 1 https://doi.org/10.1039/C8EE02694G	journal	January 2019
Non-PGM electrocatalysts for PEM fuel cells: effect of fluorination on the activity and stability of a highly active NC_Ar + NH ₃ catalyst Zhang, Gaixia; Yang, Xiaohua; Dubois, Marc Energy & Environmental Science, Vol. 12, Issue 10 https://doi.org/10.1039/C9EE00867E	journal	January 2019
A review on non-precious metal electrocatalysts for PEM fuel cells Chen, Zhongwei; Higgins, Drew; Yu, Aiping Energy & Environmental Science, Vol. 4, Issue 9 https://doi.org/10.1039/c0ee00558d	journal	January 2011
Low cost PC based scanning Kelvin probe Baikie, I. D.; Estrup, P. J. Review of Scientific Instruments, Vol. 69, Issue 11 https://doi.org/10.1063/1.1149197	journal	November 1998
Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst Chung, Hoon T.; Cullen, David A.; Higgins, Drew Science, Vol. 357, Issue 6350 https://doi.org/10.1126/science.aan2255	journal	August 2017
(Invited) Kinetic Models for the Degradation Mechanisms of PGM-Free ORR Catalysts Yin, Xi; Zelenay, Piotr ECS Transactions, Vol. 85, Issue 13 https://doi.org/10.1149/08513.1239ecst	journal	June 2018
Kinetics of Oxygen Reduction on Pt(hkl) Electrodes: Implications for the Crystallite Size Effect with Supported Pt Electrocatalysts Markovic, Nenad Journal of The Electrochemical Society, Vol. 144, Issue 5 https://doi.org/10.1149/1.1837646	journal	January 1997
Measurement of Oxygen Transport Resistance in PEM Fuel Cells by Limiting Current Methods Baker, Daniel R.; Caulk, David A.; Neyerlin, Kenneth C. Journal of The Electrochemical Society, Vol. 156, Issue 9 https://doi.org/10.1149/1.3152226	journal	January 2009
Gravure Coating for Roll-to-Roll Manufacturing of Proton-Exchange-Membrane Fuel Cell Catalyst Layers Mauger, Scott A.; Neyerlin, K. C.; Yang-Neyerlin, Ami C. Journal of The Electrochemical Society, Vol. 165, Issue 11 https://doi.org/10.1149/2.0091813jes	journal	January 2018
Experimental and Theoretical Trends of PGM-Free Electrocatalysts for the Oxygen Reduction Reaction with Different Transition Metals Martinez, Ulises; Holby, Edward F.; Babu, Siddharth Komini Journal of The Electrochemical Society, Vol. 166, Issue 7 https://doi.org/10.1149/2.0201907jes	journal	January 2019
Performance of Polymer Electrolyte Fuel Cell Electrodes with Atomically Dispersed (AD) Fe-C-N ORR Catalyst Ahluwalia, R. K.; Wang, X.; Osmieri, L. Journal of The Electrochemical Society, Vol. 166, Issue 14 https://doi.org/10.1149/2.0851914jes	journal	January 2019
Hydrogen Oxidation and Evolution Reaction Kinetics on Carbon Supported Pt, Ir, Rh, and Pd Electrocatalysts in Acidic Media Durst, Julien; Simon, Christoph; Hasché, Frédéric Journal of The Electrochemical Society, Vol. 162, Issue 1 https://doi.org/10.1149/2.0981501jes	journal	November 2014
Separation Method for Oxygen Mass Transport Coefficient in Gas and Ionomer Phases in PEMFC GDE Reshetenko, Tatyana V.; St-Pierre, Jean Journal of The Electrochemical Society, Vol. 161, Issue 10 https://doi.org/10.1149/2.1021410jes	journal	January 2014
Ink Solvent Dependence of the Ionomer Distribution in the Catalyst Layer of a PEMFC Orfanidi, Alin; Rheinländer, Philipp J.; Schulte, Nicole Journal of The Electrochemical Society, Vol. 165, Issue 14 https://doi.org/10.1149/2.1251814jes	journal	January 2018
Toward Platinum Group Metal-Free Catalysts for Hydrogen/Air Proton-Exchange Membrane Fuel Cells Jaouen, Frédéric; Jones, Deborah; Coutard, Nathan Johnson Matthey Technology Review, Vol. 62, Issue 2 https://doi.org/10.1595/205651318X696828	journal	April 2018
Transition Metal–Nitrogen–Carbon (M–N–C) Catalysts for Oxygen Reduction Reaction. Insights on Synthesis and Performance in Polymer Electrolyte Fuel Cells Osmieri, Luigi ChemEngineering, Vol. 3, Issue 1 https://doi.org/10.3390/chemengineering3010016	journal	February 2019

Similar Records

Elucidating the Role of Ionomer in the Performance of Platinum Group Metal-free Catalyst Layer via in situ Electrochemical Diagnostics

Journal Article · Mon Mar 09 00:00:00 UTC 2020 · Journal of the Electrochemical Society · OSTI ID:1832505

Wang, Guanxiong; Osmieri, Luigi; Star, Andrew G.; +2 more

Novel platinum group metal-free catalyst ink deposition system for combinatorial polymer electrolyte fuel cell performance evaluation

Journal Article · Thu Dec 31 00:00:00 UTC 2020 · Journal of Power Sources · OSTI ID:1661664

Park, Jaehyung; Myers, Deborah J.

Understanding water management in platinum group metal-free electrodes using neutron imaging

Journal Article · Fri Jul 03 00:00:00 UTC 2020 · Journal of Power Sources · OSTI ID:2280564

Komini Babu, Siddharth; Spernjak, Dusan; Mukundan, Rangachary; +8 more

Related Subjects

30 DIRECT ENERGY CONVERSION
combinatorial test
conditioning
electrode layer
non-noble metal catalyst
optimization
segmented fuel cell

Title: Use of a segmented cell for the combinatorial development of platinum group metal-free electrodes for polymer electrolyte fuel cells

Citation Formats

References (55)

Similar Records

Related Subjects