TY - JOUR
T1 - NH3-Plasma pre-treated carbon supported active iron-nitrogen catalyst for oxygen reduction in acid and alkaline electrolytes
AU - Mohan, Roopathy
AU - Modak, Arindam
AU - Schechter, Alex
N1 - Publisher Copyright:
© The Royal Society of Chemistry.
PY - 2020/3/21
Y1 - 2020/3/21
N2 - Metal-nitrogen-carbon (M-N-C) catalysts synthesized by a conventional high-temperature carbonization method are considered as promising electrocatalysts for the oxygen reduction reaction. Herein, we proposed a new approach for the preparation of M-N-C catalysts through NH3-plasma pretreatment of high surface area black pearl carbon. In this study, a pre-treated carbon support facilitated the formation of an Fe-N-C (FeNC/NH3-C) type model catalyst through pyrolysis, acid-treatment, and an additional pyrolysis step. In contrast to untreated FeNC/C, plasma pre-treated FeNC/NH3-C contains Fe3C and Fe-Nx as active catalytic sites. XPS confirms the presence of a high surface concentration of FeNx (43.6%) on FeNC/NH3-C that promotes low oxygen reduction overpotential (0.80 V vs. RHE in 0.5 M H2SO4 and 1.0 V vs. RHE in 0.1 M KOH). Hence plasma activates the surface and incorporates nitrogen, which forms stable Fe-N coordination for accelerating oxygen reduction. Importantly, FeNC/NH3-C shows a lower peroxide yield at 0.6 V vs. RHE (<1.0% in 0.5 M H2SO4 and <2% in 0.1 M KOH) that can reduce the detrimental effect of H2O2 on the catalyst support and exhibits high stability, as seen from thousands of potential cycling stability tests of FeNC/NH3-C in acid solutions. Thereby this plasma-based new synthetic approach can promote more active and stable non-precious metal catalysts.
AB - Metal-nitrogen-carbon (M-N-C) catalysts synthesized by a conventional high-temperature carbonization method are considered as promising electrocatalysts for the oxygen reduction reaction. Herein, we proposed a new approach for the preparation of M-N-C catalysts through NH3-plasma pretreatment of high surface area black pearl carbon. In this study, a pre-treated carbon support facilitated the formation of an Fe-N-C (FeNC/NH3-C) type model catalyst through pyrolysis, acid-treatment, and an additional pyrolysis step. In contrast to untreated FeNC/C, plasma pre-treated FeNC/NH3-C contains Fe3C and Fe-Nx as active catalytic sites. XPS confirms the presence of a high surface concentration of FeNx (43.6%) on FeNC/NH3-C that promotes low oxygen reduction overpotential (0.80 V vs. RHE in 0.5 M H2SO4 and 1.0 V vs. RHE in 0.1 M KOH). Hence plasma activates the surface and incorporates nitrogen, which forms stable Fe-N coordination for accelerating oxygen reduction. Importantly, FeNC/NH3-C shows a lower peroxide yield at 0.6 V vs. RHE (<1.0% in 0.5 M H2SO4 and <2% in 0.1 M KOH) that can reduce the detrimental effect of H2O2 on the catalyst support and exhibits high stability, as seen from thousands of potential cycling stability tests of FeNC/NH3-C in acid solutions. Thereby this plasma-based new synthetic approach can promote more active and stable non-precious metal catalysts.
UR - http://www.scopus.com/inward/record.url?scp=85082752071&partnerID=8YFLogxK
U2 - 10.1039/c9cy02545f
DO - 10.1039/c9cy02545f
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AN - SCOPUS:85082752071
SN - 2044-4753
VL - 10
SP - 1675
EP - 1687
JO - Catalysis Science and Technology
JF - Catalysis Science and Technology
IS - 6
ER -