Issue 6, 2020

NH3-Plasma pre-treated carbon supported active iron–nitrogen catalyst for oxygen reduction in acid and alkaline electrolytes

Abstract

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.

Graphical abstract: NH3-Plasma pre-treated carbon supported active iron–nitrogen catalyst for oxygen reduction in acid and alkaline electrolytes

Supplementary files

Article information

Article type
Paper
Submitted
16 dez 2019
Accepted
03 fev 2020
First published
06 fev 2020

Catal. Sci. Technol., 2020,10, 1675-1687

NH3-Plasma pre-treated carbon supported active iron–nitrogen catalyst for oxygen reduction in acid and alkaline electrolytes

R. Mohan, A. Modak and A. Schechter, Catal. Sci. Technol., 2020, 10, 1675 DOI: 10.1039/C9CY02545F

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