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Title: Iron-based sulfur and nitrogen dual doped porous carbon as durable electrocatalysts for oxygen reduction reaction

Abstract

The widespread use of fuel cell technology is hampered by the use of expensive and scarce platinum metal in electrodes which is required to facilitate the sluggish oxygen reduction reaction (ORR). In this work, a viable synthetic approach was developed to prepare iron-based sulfur and nitrogen dual doped porous carbon (Fe@SNDC) for use in ORR. Benzimidazole, a commercially available monomer, was used as a precursor for N doped carbon and calcined with potassium thiocyanate at different temperatures to tune the pore size, nitrogen content and different types of nitrogen functionality such as pyridinic, pyrrolic and graphitic. The Fe@SNDC–950 with high surface area, optimum N content of about 5 at% and high amount of pyridinic and graphitic N displayed an onset potential and half-wave potential of 0.98 and 0.83 V vs RHE, respectively, in 0.1 M KOH solution. The catalyst also exhibits similar oxygen reduction reaction performance compared to Pt/C (20 wt%) in acidic media. Furthermore, when compared to commercially available Pt/C (20 wt%), Fe@SNDC–950 showed enhanced durability over 6 h and poison tolerance in case of methanol crossover with the concentration up to 3.0 M in oxygen saturated alkaline electrolyte. Finally, our study demonstrates that the presence of N andmore » S along with Fe-N moieties synergistically served as ORR active sites while the high surface area with accessible pores allowed for efficient mass transfer and interaction of oxygen molecules to the active sites contributing to the ORR activity of the catalyst.« less

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [1]
  1. Virginia Commonwealth Univ., Richmond, VA (United States)
Publication Date:
Research Org.:
Virginia Commonwealth Univ., Richmond, VA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
OSTI Identifier:
1977206
Grant/Contract Number:  
SC0002576
Resource Type:
Accepted Manuscript
Journal Name:
International Journal of Hydrogen Energy
Additional Journal Information:
Journal Volume: 47; Journal Issue: 9; Journal ID: ISSN 0360-3199
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; Chemistry; Electrochemistry; Energy & Fuels; Oxygen reduction reaction (ORR); Iron-based sulfur and nitrogen dual doped porous carbon; Fuel cell; Electrocatalyst

Citation Formats

Choudhury, Fatema Akthar, Norouzi, Nazgol, Amir, Kaiynat, Demir, Muslum, and El-Kaderi, Hani M. Iron-based sulfur and nitrogen dual doped porous carbon as durable electrocatalysts for oxygen reduction reaction. United States: N. p., 2021. Web. doi:10.1016/j.ijhydene.2021.12.020.
Choudhury, Fatema Akthar, Norouzi, Nazgol, Amir, Kaiynat, Demir, Muslum, & El-Kaderi, Hani M. Iron-based sulfur and nitrogen dual doped porous carbon as durable electrocatalysts for oxygen reduction reaction. United States. https://doi.org/10.1016/j.ijhydene.2021.12.020
Choudhury, Fatema Akthar, Norouzi, Nazgol, Amir, Kaiynat, Demir, Muslum, and El-Kaderi, Hani M. Sun . "Iron-based sulfur and nitrogen dual doped porous carbon as durable electrocatalysts for oxygen reduction reaction". United States. https://doi.org/10.1016/j.ijhydene.2021.12.020. https://www.osti.gov/servlets/purl/1977206.
@article{osti_1977206,
title = {Iron-based sulfur and nitrogen dual doped porous carbon as durable electrocatalysts for oxygen reduction reaction},
author = {Choudhury, Fatema Akthar and Norouzi, Nazgol and Amir, Kaiynat and Demir, Muslum and El-Kaderi, Hani M.},
abstractNote = {The widespread use of fuel cell technology is hampered by the use of expensive and scarce platinum metal in electrodes which is required to facilitate the sluggish oxygen reduction reaction (ORR). In this work, a viable synthetic approach was developed to prepare iron-based sulfur and nitrogen dual doped porous carbon (Fe@SNDC) for use in ORR. Benzimidazole, a commercially available monomer, was used as a precursor for N doped carbon and calcined with potassium thiocyanate at different temperatures to tune the pore size, nitrogen content and different types of nitrogen functionality such as pyridinic, pyrrolic and graphitic. The Fe@SNDC–950 with high surface area, optimum N content of about 5 at% and high amount of pyridinic and graphitic N displayed an onset potential and half-wave potential of 0.98 and 0.83 V vs RHE, respectively, in 0.1 M KOH solution. The catalyst also exhibits similar oxygen reduction reaction performance compared to Pt/C (20 wt%) in acidic media. Furthermore, when compared to commercially available Pt/C (20 wt%), Fe@SNDC–950 showed enhanced durability over 6 h and poison tolerance in case of methanol crossover with the concentration up to 3.0 M in oxygen saturated alkaline electrolyte. Finally, our study demonstrates that the presence of N and S along with Fe-N moieties synergistically served as ORR active sites while the high surface area with accessible pores allowed for efficient mass transfer and interaction of oxygen molecules to the active sites contributing to the ORR activity of the catalyst.},
doi = {10.1016/j.ijhydene.2021.12.020},
journal = {International Journal of Hydrogen Energy},
number = 9,
volume = 47,
place = {United States},
year = {Sun Dec 26 00:00:00 EST 2021},
month = {Sun Dec 26 00:00:00 EST 2021}
}

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