Phosphate tolerance of nitrogen-coordinated-iron-carbon (FeNC) catalysts for oxygen reduction reaction: A size-related hindrance effect
Abstract
The greatest challenges facing the large – scale commercialization of the intermediate temperature phosphoric acid fuel cell (PAFC) technology are: (i) the high cost of Pt catalyst that is required to overcome the slow kinetics of oxygen reduction reaction (ORR) on the PAFC cathode, and (ii) deactivation of the Pt catalyst by exposure to the phosphoric acid electrolyte. Inexpensive carbon-based materials, particularly iron- spectroscopy is used to explore the phenomenon of phosphate poisoning nitrogen-coordinated carbon supported catalysts (FeNC), are promising cathodes for PAFCs. The higher ORR activation energy and phosphate poisoning resistance of FeNC present a clear advantage over the Pt-based commercial catalysts that are easily susceptible to deactivation after exposure to phosphate anions. While the immunity of FeNC catalysts to phosphate anion poisoning has been reported previously, this work explores the counter-intuitive and conditional nature of this poisoning resistance based on the properties of the carbon support used in the preparation of the FeNC catalyst. Additionally, a combination of electrochemical measurements with characterization experiments performed using X-ray photoelectron spectroscopy, infrared spectroscopy and in-situ X-ray absorption on FeNC catalysts synthesized from two different carbon supports. Results from these studies reveal a “size-related hindrance effect” wherein the ORR active Fe centersmore »
- Authors:
-
[1];
[1];
[1];
- The Ohio State Univ., Columbus, OH (United States). William G. Lowrie Dept. of Chemical and Biomolecular Engineering
- The Ohio State Univ., Columbus, OH (United States). Dept. of Chemistry and Biochemistry
- Publication Date:
- Research Org.:
- The Ohio State Univ., Columbus, OH (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1849724
- Alternate Identifier(s):
- OSTI ID: 1648155
- Grant/Contract Number:
- FG02-07ER15896; AC02-06CH11357; DE ‐FG02‐ 07ER15896
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Catalysis
- Additional Journal Information:
- Journal Volume: 390; Journal Issue: C; Journal ID: ISSN 0021-9517
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 42 ENGINEERING; Chemistry; Engineering; Oxygen reduction reaction; FeNC catalyst; activation energy; phosphate poisoning; active sites; carbon support
Citation Formats
Jain, Deeksha, Gustin, Vance, Basu, Dishari, Gunduz, Seval, Deka, Dhruba J., Co, Anne C., and Ozkan, Umit S. Phosphate tolerance of nitrogen-coordinated-iron-carbon (FeNC) catalysts for oxygen reduction reaction: A size-related hindrance effect. United States: N. p., 2020.
Web. doi:10.1016/j.jcat.2020.07.012.
Jain, Deeksha, Gustin, Vance, Basu, Dishari, Gunduz, Seval, Deka, Dhruba J., Co, Anne C., & Ozkan, Umit S. Phosphate tolerance of nitrogen-coordinated-iron-carbon (FeNC) catalysts for oxygen reduction reaction: A size-related hindrance effect. United States. https://doi.org/10.1016/j.jcat.2020.07.012
Jain, Deeksha, Gustin, Vance, Basu, Dishari, Gunduz, Seval, Deka, Dhruba J., Co, Anne C., and Ozkan, Umit S. Tue .
"Phosphate tolerance of nitrogen-coordinated-iron-carbon (FeNC) catalysts for oxygen reduction reaction: A size-related hindrance effect". United States. https://doi.org/10.1016/j.jcat.2020.07.012. https://www.osti.gov/servlets/purl/1849724.
@article{osti_1849724,
title = {Phosphate tolerance of nitrogen-coordinated-iron-carbon (FeNC) catalysts for oxygen reduction reaction: A size-related hindrance effect},
author = {Jain, Deeksha and Gustin, Vance and Basu, Dishari and Gunduz, Seval and Deka, Dhruba J. and Co, Anne C. and Ozkan, Umit S.},
abstractNote = {The greatest challenges facing the large – scale commercialization of the intermediate temperature phosphoric acid fuel cell (PAFC) technology are: (i) the high cost of Pt catalyst that is required to overcome the slow kinetics of oxygen reduction reaction (ORR) on the PAFC cathode, and (ii) deactivation of the Pt catalyst by exposure to the phosphoric acid electrolyte. Inexpensive carbon-based materials, particularly iron- spectroscopy is used to explore the phenomenon of phosphate poisoning nitrogen-coordinated carbon supported catalysts (FeNC), are promising cathodes for PAFCs. The higher ORR activation energy and phosphate poisoning resistance of FeNC present a clear advantage over the Pt-based commercial catalysts that are easily susceptible to deactivation after exposure to phosphate anions. While the immunity of FeNC catalysts to phosphate anion poisoning has been reported previously, this work explores the counter-intuitive and conditional nature of this poisoning resistance based on the properties of the carbon support used in the preparation of the FeNC catalyst. Additionally, a combination of electrochemical measurements with characterization experiments performed using X-ray photoelectron spectroscopy, infrared spectroscopy and in-situ X-ray absorption on FeNC catalysts synthesized from two different carbon supports. Results from these studies reveal a “size-related hindrance effect” wherein the ORR active Fe centers in FeNC remain inaccessible to larger anions such as phosphate when the Fe sites are present deeper inside the pores of a carbon support with high porosity. However, FeNC catalyst is poisoned by phosphate anions when synthesized using a carbon support with low porosity. This work helps gain insights into the nature of active sites in FeNC catalysts that will be useful in designing precious-metal free ORR catalysts for intermediate temperature fuel cell technologies.},
doi = {10.1016/j.jcat.2020.07.012},
journal = {Journal of Catalysis},
number = C,
volume = 390,
place = {United States},
year = {Tue Jul 28 00:00:00 EDT 2020},
month = {Tue Jul 28 00:00:00 EDT 2020}
}
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