High-Performance Supercomputing for Pore-Scale Simulations of Electrochemical Reactions and Transport Processes in PGM-Free Electrodes

Laboratory: Argonne National Laboratory (ANL)
Capability Expert: Rajesh K. Ahluwalia, walia@anl.gov, 630-252-5979
Capability Details:
Title:   High-Performance Supercomputing for Pore-Scale Simulations of Electrochemical Reactions and Transport Processes in PGM-Free Electrodes
Class:   Computational tool and simulations
Description:   We are developing pore-scale models, with nm to mm resolution, using high-performance computing to simulate electrochemical reactions, species transport, and liquid water movement in thick PGM-free electrodes. The simulations are conducted on primitive hybrid electrode microstructures that define the distributions and connectivity of primary and secondary pores, active electrochemical reaction sites, solids, and ionomer.
Capability Bounds:   The models are most fundamental but require supporting experimental data that are specific to catalysts and electrode structures.
Unique Aspects:   Models are most useful in identifying the aspects of electrode structures that limit the performance of thick PGM-free electrodes under different conditions and in guiding improvements needed to overcome these limitations.
Availability:   Models are under initial development for thinner low-PGM electrodes and modeling even these thinner electrodes requires access to high performance computers with >100 million nodes and >100,000 core-hours.
References:   C. Cetinbas, R.K. Ahluwalia, N. Kariuki, V. De Andrade, D. Fongalland, L. Smith, J. Sharman, P. Ferreira, S. Rasouli, and D.J. Myers, “Hybrid approach combining multiple characterization techniques and simulations for microstructural analysis of proton exchange membrane fuel cell electrodes,” J. Power Sources 344 (2017), pp 62-72.C. Cetinbas, X. Wang, R.K. Ahluwalia, N. Kariuki, R.P. Winarski, Z. Wang, J. Sharman, and
D.J. Myers, “Microstructural analysis and transport resistances of low-platinum PEFC electrodes,” J. Electrochem. Soc. 164 (2017), F1596-F1607.
Benefit:   This capability is important to the mission of ElectroCat consortium since knowledge of kinetic and transport processes that limit the electrochemical performance are crucial in the development of novel PGM-free catalysts and electrodes.
Robustness:   The models are robust but require supporting experimental data for PGM-free catalysts and electrodes of interest. The models have been previously used only for low-PGM Pt/C and PtCo/C catalysts.
Dynamics of liquid water invasion
Vertical bar chart showing saturation in blue and pore scale in red
Pore-scale saturation profiles