Identifying electrochemical processes by distribution of relaxation times in proton exchange membrane electrolyzers

Chan, Ai-Lin; Yu, Haoran; Reeves, Kimberly S.; Alia, Shaun M.

doi:10.1016/j.jpowsour.2024.235850

Identifying electrochemical processes by distribution of relaxation times in proton exchange membrane electrolyzers

Journal Article · Sat Nov 23 00:00:00 EST 2024 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2024.235850· OSTI ID:2480295

^[1]; ^[2]; Reeves, Kimberly S. ^[2]; ^[1]

National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Distribution of relaxation time (DRT) is used to interpret electrochemical impedance spectroscopy (EIS) for proton exchange membrane (PEM) water electrolyzers, with an attempt to separate overlapped relaxation processes in Nyquist plots. By varying operating conditions and catalyst loadings, four main relaxation peaks arising from EIS can be identified and successfully separated from low to high frequencies as (P1) mass transport, (P2) oxygen evolution reaction kinetics, (P3) reaction kinetics (with faster time constant than P2), and (P4) ionic transport. Here, the shape, height, and frequency of the DRT peaks change with different membrane electrode assembly (MEA) configurations. Electron microscopy reveals distinct features from the cross-sectioned MEAs which verify critical DRT results in that increasing the iridium (Ir)-anode loading from 0.2 mgIr/cm² to 1.5 mgIr/cm² reduces kinetic losses due to higher site-access; a thick and compacted anode, however, also triggers higher ohmic resistances from membrane/catalyst layer hydration and increases transport losses due to longer ionomer pathways. DRT provides higher resolution to EIS for deconvoluting processes with different relaxation times and the quantification of DRT peaks improves the accounting of total losses from each process.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725; AC36-08GO28308

OSTI ID:: 2480295

Alternate ID(s):: OSTI ID: 2502145

Report Number(s):: NREL/JA--5900-90793; MainId:92571; UUID:9e9f1625-5c80-4137-96d2-a5ae8b34780f; MainAdminId:74268

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 628; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Identifying electrochemical processes by distribution of relaxation times in proton exchange membrane electrolyzers

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