Toward understanding the utilization of oxygen reduction electrocatalysts under high mass transport conditions and high overpotentials
File(s)Final Submitted MS.docx (532.26 KB) Final submitted Supplementary information.docx (1.61 MB)
Accepted version
Supporting information
Author(s)
Jackson, Colleen
Lin, Xiaoqian
Levecque, Pieter
Kucernak, Anthony
Type
Journal Article
Abstract
There is currently a disconnect between the high electrocatalyst oxygen reduction reaction (ORR) performance measured ex situ, using the rotating disc electrode (RDE), and the in situ membrane electrode assembly (MEA) performance. The disconnect in the electrocatalyst performance raises questions both about the pitfalls of the RDE technique at extrapolating the performance to higher overpotentials and how to improve the in situ catalyst layer performance to meet ambitious fuel cell targets. This work aims to bridge the gap by measuring the ORR ex situ performance under high mass transport conditions, at high overpotentials, using the floating electrode (FE) technique. Here, we determine the performance of three Pt/C electrocatalysts using the FE in 1 M HClO4 and 1 M H2SO4 to show that the MEA activities measured at 80 °C, 150 kPag were substantially lower than the room temperature and pressure performance of the same catalyst in 1 M HClO4 using the RDE and FE methods and also lower than the FE in 1 M H2SO4, implying MEA limitations are not purely due to sulfonate adsorption from the Nafion. Finally, FE and MEA data was modeled which obtained jo values on the FE (oxide free conditions) which were 4–6× larger, at 11–26 μA cm–2, than those measured on the MEA. The difference is interpreted as due to better water removal in the FE system. This work shows that MEA catalyst layers are vastly underutilized, due to poor water transport, and current densities equivalent to 10–16 A cm–2 at 0.65 V for 400 μgPt cm–2 (25–40 A mg–1) are achievable, whereas the current mass activity of MEAs is <40% of this value at 25 and 80 °C, 150 kPag.
Date Issued
2021-12-14
Date Acceptance
2021-11-30
Citation
ACS Catalysis, 2021, 12 (1), pp.200-211
ISSN
2155-5435
Publisher
American Chemical Society
Start Page
200
End Page
211
Journal / Book Title
ACS Catalysis
Volume
12
Issue
1
Copyright Statement
© 2021 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acscatal.1c03908
Sponsor
Engineering & Physical Science Research Council (E
Identifier
https://pubs.acs.org/doi/10.1021/acscatal.1c03908
Grant Number
EP/P024807/1
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Chemistry
oxygen reduction reaction
rotating disc electrode
floating electrode
membrane electrode assembly
kinetic activity
exchange current density
ROTATING-DISC ELECTRODE
GAS-DIFFUSION ELECTRODE
CATALYST LAYER
FUEL-CELLS
PERFORMANCE
CARBON
ALLOY
ORR
0302 Inorganic Chemistry
0305 Organic Chemistry
0904 Chemical Engineering
Publication Status
Published online
Date Publish Online
2021-12-14