Editors' Choice—Connecting Fuel Cell Catalyst Nanostructure and Accessibility Using Quantitative Cryo-STEM Tomography
Abstract
Further reduction of Pt in hydrogen fuel cells is hampered by reactant transport losses near the catalyst surface, especially for degraded catalysts. Strategically mitigating these performance losses requires an improved understanding of the catalyst nanostructure, which controls local transport and catalyst durability. We apply cryo-tomography in a scanning transmission electron microscope (STEM) to quantify the three-dimensional structure of carbon-supported Pt catalysts and correlate to their electrochemical accessibility. We present results for two carbon supports: Vulcan, a compact support with a large majority of Pt observed on the exterior, and HSC, a porous support with a majority of Pt observed within interior carbon pores, which have relatively constrictive openings. Increasing Pt content shifts the Pt distribution to the exterior on both carbon supports. By correlating to the electrochemical surface area, we find that all Pt surface area is accessible to protons in liquid. However, the interior Pt fraction quantitatively tracks Pt utilization losses at low humidity, indicating that the interior Pt is inaccessible to the proton-conducting ionomer, likely because narrow carbon pore openings block ionomer infiltration. These results imply different proton transport mechanisms for interior and exterior Pt, and quantitatively describe the catalyst structure, supporting development of transport and durability models.
- Authors:
- Publication Date:
- Research Org.:
- General Motors Co., Warren, MI (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office (HFTO)
- OSTI Identifier:
- 1423148
- Alternate Identifier(s):
- OSTI ID: 1509886
- Grant/Contract Number:
- EE0007271
- Resource Type:
- Published Article
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Name: Journal of the Electrochemical Society Journal Volume: 165 Journal Issue: 3; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Carbon support; Nanostructure; Transport
Citation Formats
Padgett, Elliot, Andrejevic, Nina, Liu, Zhongyi, Kongkanand, Anusorn, Gu, Wenbin, Moriyama, Koji, Jiang, Yi, Kumaraguru, Swami, Moylan, Thomas E., Kukreja, Ratandeep, and Muller, David A. Editors' Choice—Connecting Fuel Cell Catalyst Nanostructure and Accessibility Using Quantitative Cryo-STEM Tomography. United States: N. p., 2018.
Web. doi:10.1149/2.0541803jes.
Padgett, Elliot, Andrejevic, Nina, Liu, Zhongyi, Kongkanand, Anusorn, Gu, Wenbin, Moriyama, Koji, Jiang, Yi, Kumaraguru, Swami, Moylan, Thomas E., Kukreja, Ratandeep, & Muller, David A. Editors' Choice—Connecting Fuel Cell Catalyst Nanostructure and Accessibility Using Quantitative Cryo-STEM Tomography. United States. https://doi.org/10.1149/2.0541803jes
Padgett, Elliot, Andrejevic, Nina, Liu, Zhongyi, Kongkanand, Anusorn, Gu, Wenbin, Moriyama, Koji, Jiang, Yi, Kumaraguru, Swami, Moylan, Thomas E., Kukreja, Ratandeep, and Muller, David A. Thu .
"Editors' Choice—Connecting Fuel Cell Catalyst Nanostructure and Accessibility Using Quantitative Cryo-STEM Tomography". United States. https://doi.org/10.1149/2.0541803jes.
@article{osti_1423148,
title = {Editors' Choice—Connecting Fuel Cell Catalyst Nanostructure and Accessibility Using Quantitative Cryo-STEM Tomography},
author = {Padgett, Elliot and Andrejevic, Nina and Liu, Zhongyi and Kongkanand, Anusorn and Gu, Wenbin and Moriyama, Koji and Jiang, Yi and Kumaraguru, Swami and Moylan, Thomas E. and Kukreja, Ratandeep and Muller, David A.},
abstractNote = {Further reduction of Pt in hydrogen fuel cells is hampered by reactant transport losses near the catalyst surface, especially for degraded catalysts. Strategically mitigating these performance losses requires an improved understanding of the catalyst nanostructure, which controls local transport and catalyst durability. We apply cryo-tomography in a scanning transmission electron microscope (STEM) to quantify the three-dimensional structure of carbon-supported Pt catalysts and correlate to their electrochemical accessibility. We present results for two carbon supports: Vulcan, a compact support with a large majority of Pt observed on the exterior, and HSC, a porous support with a majority of Pt observed within interior carbon pores, which have relatively constrictive openings. Increasing Pt content shifts the Pt distribution to the exterior on both carbon supports. By correlating to the electrochemical surface area, we find that all Pt surface area is accessible to protons in liquid. However, the interior Pt fraction quantitatively tracks Pt utilization losses at low humidity, indicating that the interior Pt is inaccessible to the proton-conducting ionomer, likely because narrow carbon pore openings block ionomer infiltration. These results imply different proton transport mechanisms for interior and exterior Pt, and quantitatively describe the catalyst structure, supporting development of transport and durability models.},
doi = {10.1149/2.0541803jes},
journal = {Journal of the Electrochemical Society},
number = 3,
volume = 165,
place = {United States},
year = {Thu Feb 08 00:00:00 EST 2018},
month = {Thu Feb 08 00:00:00 EST 2018}
}
https://doi.org/10.1149/2.0541803jes
Web of Science
Figures / Tables:
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