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Title: N- and S-doped mesoporous carbon as metal-free cathode catalysts for direct biorenewable alcohol fuel cells

Abstract

Nitrogen and sulfur were simultaneously doped into the framework of mesoporous CMK-3 as metal-free catalysts for direct biorenewable alcohol fuel cells. Glucose, NH3, and thiophene were used as carbon, nitrogen and sulfur precursors, respectively, to prepare mesoporous N-S-CMK-3 with uniform mesopores and extra macropores, resulting in good O2 diffusion both in half cell and alcohol fuel cell investigations. Among all investigated CMK-3 based catalysts, N-S-CMK-3 prepared at 800 °C exhibited the highest ORR activity with the onset potential of 0.92 V vs. RHE, Tafel slope of 68 mV dec-1, and 3.96 electron transfer number per oxygen molecule in 0.1 M KOH. In addition, the alkaline membrane-based direct alcohol fuel cell (DAFC) with N-S-CMK-3 cathode displayed 88.2 mW cm-2 peak power density without obvious O2 diffusion issue, reaching 84% initial performance of that with a Pt/C cathode. The high catalyst durability and fuel-crossover tolerance led to stable performance of the N-S-CMK-3 cathode DAFC with 90.6 mW cm-2 peak power density after 2 h operation, while the Pt/C cathode-based DAFC lost 36.9% of its peak power density. In conclusion, the high ORR activity of N-S-CMK-3 can be attributed to the synergistic effect between graphitic-N and S (C–S–C structure), suggesting great potential tomore » use N-S-CMK-3 as an alternative to noble metal catalysts in the fuel cell cathode.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [2]
  1. Iowa State Univ., Ames, IA (United States). Chemical and Biological Engineering, Biorenewables Research Laboratory
  2. (United States)
Publication Date:
Research Org.:
Ames Lab., Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1355355
Report Number(s):
IS-J-8904
Journal ID: ISSN 2050-7488
Grant/Contract Number:  
AC02-07CH11358; CBET1159448; CBET 1501113
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Qiu, Yang, Huo, Jiajie, Jia, Fan, Shanks, Brent. H., Li, Wenzhen, and Ames Lab., Ames, IA. N- and S-doped mesoporous carbon as metal-free cathode catalysts for direct biorenewable alcohol fuel cells. United States: N. p., 2015. Web. doi:10.1039/c5ta06039g.
Qiu, Yang, Huo, Jiajie, Jia, Fan, Shanks, Brent. H., Li, Wenzhen, & Ames Lab., Ames, IA. N- and S-doped mesoporous carbon as metal-free cathode catalysts for direct biorenewable alcohol fuel cells. United States. doi:10.1039/c5ta06039g.
Qiu, Yang, Huo, Jiajie, Jia, Fan, Shanks, Brent. H., Li, Wenzhen, and Ames Lab., Ames, IA. Fri . "N- and S-doped mesoporous carbon as metal-free cathode catalysts for direct biorenewable alcohol fuel cells". United States. doi:10.1039/c5ta06039g. https://www.osti.gov/servlets/purl/1355355.
@article{osti_1355355,
title = {N- and S-doped mesoporous carbon as metal-free cathode catalysts for direct biorenewable alcohol fuel cells},
author = {Qiu, Yang and Huo, Jiajie and Jia, Fan and Shanks, Brent. H. and Li, Wenzhen and Ames Lab., Ames, IA},
abstractNote = {Nitrogen and sulfur were simultaneously doped into the framework of mesoporous CMK-3 as metal-free catalysts for direct biorenewable alcohol fuel cells. Glucose, NH3, and thiophene were used as carbon, nitrogen and sulfur precursors, respectively, to prepare mesoporous N-S-CMK-3 with uniform mesopores and extra macropores, resulting in good O2 diffusion both in half cell and alcohol fuel cell investigations. Among all investigated CMK-3 based catalysts, N-S-CMK-3 prepared at 800 °C exhibited the highest ORR activity with the onset potential of 0.92 V vs. RHE, Tafel slope of 68 mV dec-1, and 3.96 electron transfer number per oxygen molecule in 0.1 M KOH. In addition, the alkaline membrane-based direct alcohol fuel cell (DAFC) with N-S-CMK-3 cathode displayed 88.2 mW cm-2 peak power density without obvious O2 diffusion issue, reaching 84% initial performance of that with a Pt/C cathode. The high catalyst durability and fuel-crossover tolerance led to stable performance of the N-S-CMK-3 cathode DAFC with 90.6 mW cm-2 peak power density after 2 h operation, while the Pt/C cathode-based DAFC lost 36.9% of its peak power density. In conclusion, the high ORR activity of N-S-CMK-3 can be attributed to the synergistic effect between graphitic-N and S (C–S–C structure), suggesting great potential to use N-S-CMK-3 as an alternative to noble metal catalysts in the fuel cell cathode.},
doi = {10.1039/c5ta06039g},
journal = {Journal of Materials Chemistry. A},
number = 1,
volume = 4,
place = {United States},
year = {2015},
month = {11}
}

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