Immunity of the Fe-N-C catalysts to electrolyte adsorption: phosphate but not perchloric anions

Yang Hu, Jens Oluf Jensen, Chao Pan, Lars Nilausen Cleemann, Illia Shypunov, Qingfeng Li*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Non-precious metal catalysts (NPMCs), particularly the type based on carbon-supported FeNx functionalities (Fe-N-C) are a very promising material for replacing the rare and costly platinum-based catalysts in polymer electrolyte membrane fuel cells (PEMFCs). Evaluation of these materials is most often carried out, like for Pt-based catalysts, in dilute perchloric acid by assuming its non-adsorbing nature on the active sites. The assumption is however not true. In this work, a typical Fe-N-C catalyst was first synthesized by high-pressure pyrolysis in the presence of carbon support and thoroughly characterized in terms of morphology, structure and active site distribution. The subsequent electrochemical characterization of the catalyst shows strong adsorption and poisoning effect of, in addition to the known Cl-, perchloric anions on the oxygen reduction reaction (ORR) activity. On the contrary phosphate anions exhibit negligible poisoning effect on the catalyst activity. At 0.8 V vs. RHE, the ORR activity of the catalyst is found to decrease in the order of H3PO4 (8.6 mA mg-1) > H2SO4 (5.3 mA mg-1 ) > HClO4 (3.1 mA mg-1) > HCl (0.7 mA mg-1). The results suggest potential applications of NPMC in high-temperature PEMFCs based on phosphoric acid doped polymer membranes, where high loading platinum catalysts are currently used. As demonstrated in the low current density range of high-temperature PEMFCs, the catalyst shows a comparable performance to the Pt/C catalysts.
Original languageEnglish
JournalApplied Catalysis B: Environmental
Volume234
Pages (from-to)357-364
ISSN0926-3373
DOIs
Publication statusPublished - 2018

Keywords

  • Oxygen reduction
  • Catalyst
  • Fuell cell
  • Anion
  • Poison

Cite this

@article{02ec711ec8e845f1b2f6ff68ae42d46e,
title = "Immunity of the Fe-N-C catalysts to electrolyte adsorption: phosphate but not perchloric anions",
abstract = "Non-precious metal catalysts (NPMCs), particularly the type based on carbon-supported FeNx functionalities (Fe-N-C) are a very promising material for replacing the rare and costly platinum-based catalysts in polymer electrolyte membrane fuel cells (PEMFCs). Evaluation of these materials is most often carried out, like for Pt-based catalysts, in dilute perchloric acid by assuming its non-adsorbing nature on the active sites. The assumption is however not true. In this work, a typical Fe-N-C catalyst was first synthesized by high-pressure pyrolysis in the presence of carbon support and thoroughly characterized in terms of morphology, structure and active site distribution. The subsequent electrochemical characterization of the catalyst shows strong adsorption and poisoning effect of, in addition to the known Cl-, perchloric anions on the oxygen reduction reaction (ORR) activity. On the contrary phosphate anions exhibit negligible poisoning effect on the catalyst activity. At 0.8 V vs. RHE, the ORR activity of the catalyst is found to decrease in the order of H3PO4 (8.6 mA mg-1) > H2SO4 (5.3 mA mg-1 ) > HClO4 (3.1 mA mg-1) > HCl (0.7 mA mg-1). The results suggest potential applications of NPMC in high-temperature PEMFCs based on phosphoric acid doped polymer membranes, where high loading platinum catalysts are currently used. As demonstrated in the low current density range of high-temperature PEMFCs, the catalyst shows a comparable performance to the Pt/C catalysts.",
keywords = "Oxygen reduction, Catalyst, Fuell cell, Anion, Poison",
author = "Yang Hu and Jensen, {Jens Oluf} and Chao Pan and Cleemann, {Lars Nilausen} and Illia Shypunov and Qingfeng Li",
year = "2018",
doi = "10.1016/j.apcatb.2018.03.056",
language = "English",
volume = "234",
pages = "357--364",
journal = "Applied Catalysis B: Environmental",
issn = "0926-3373",
publisher = "Elsevier",

}

Immunity of the Fe-N-C catalysts to electrolyte adsorption: phosphate but not perchloric anions. / Hu, Yang; Jensen, Jens Oluf; Pan, Chao; Cleemann, Lars Nilausen; Shypunov, Illia; Li, Qingfeng.

In: Applied Catalysis B: Environmental, Vol. 234, 2018, p. 357-364.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Immunity of the Fe-N-C catalysts to electrolyte adsorption: phosphate but not perchloric anions

AU - Hu, Yang

AU - Jensen, Jens Oluf

AU - Pan, Chao

AU - Cleemann, Lars Nilausen

AU - Shypunov, Illia

AU - Li, Qingfeng

PY - 2018

Y1 - 2018

N2 - Non-precious metal catalysts (NPMCs), particularly the type based on carbon-supported FeNx functionalities (Fe-N-C) are a very promising material for replacing the rare and costly platinum-based catalysts in polymer electrolyte membrane fuel cells (PEMFCs). Evaluation of these materials is most often carried out, like for Pt-based catalysts, in dilute perchloric acid by assuming its non-adsorbing nature on the active sites. The assumption is however not true. In this work, a typical Fe-N-C catalyst was first synthesized by high-pressure pyrolysis in the presence of carbon support and thoroughly characterized in terms of morphology, structure and active site distribution. The subsequent electrochemical characterization of the catalyst shows strong adsorption and poisoning effect of, in addition to the known Cl-, perchloric anions on the oxygen reduction reaction (ORR) activity. On the contrary phosphate anions exhibit negligible poisoning effect on the catalyst activity. At 0.8 V vs. RHE, the ORR activity of the catalyst is found to decrease in the order of H3PO4 (8.6 mA mg-1) > H2SO4 (5.3 mA mg-1 ) > HClO4 (3.1 mA mg-1) > HCl (0.7 mA mg-1). The results suggest potential applications of NPMC in high-temperature PEMFCs based on phosphoric acid doped polymer membranes, where high loading platinum catalysts are currently used. As demonstrated in the low current density range of high-temperature PEMFCs, the catalyst shows a comparable performance to the Pt/C catalysts.

AB - Non-precious metal catalysts (NPMCs), particularly the type based on carbon-supported FeNx functionalities (Fe-N-C) are a very promising material for replacing the rare and costly platinum-based catalysts in polymer electrolyte membrane fuel cells (PEMFCs). Evaluation of these materials is most often carried out, like for Pt-based catalysts, in dilute perchloric acid by assuming its non-adsorbing nature on the active sites. The assumption is however not true. In this work, a typical Fe-N-C catalyst was first synthesized by high-pressure pyrolysis in the presence of carbon support and thoroughly characterized in terms of morphology, structure and active site distribution. The subsequent electrochemical characterization of the catalyst shows strong adsorption and poisoning effect of, in addition to the known Cl-, perchloric anions on the oxygen reduction reaction (ORR) activity. On the contrary phosphate anions exhibit negligible poisoning effect on the catalyst activity. At 0.8 V vs. RHE, the ORR activity of the catalyst is found to decrease in the order of H3PO4 (8.6 mA mg-1) > H2SO4 (5.3 mA mg-1 ) > HClO4 (3.1 mA mg-1) > HCl (0.7 mA mg-1). The results suggest potential applications of NPMC in high-temperature PEMFCs based on phosphoric acid doped polymer membranes, where high loading platinum catalysts are currently used. As demonstrated in the low current density range of high-temperature PEMFCs, the catalyst shows a comparable performance to the Pt/C catalysts.

KW - Oxygen reduction

KW - Catalyst

KW - Fuell cell

KW - Anion

KW - Poison

U2 - 10.1016/j.apcatb.2018.03.056

DO - 10.1016/j.apcatb.2018.03.056

M3 - Journal article

VL - 234

SP - 357

EP - 364

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

SN - 0926-3373

ER -