Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis

Yechuan Chen; Rohan Gokhale; Alexey Serov; Kateryna Artyushkova; Plamen Atanassov

doi:10.1016/j.nanoen.2017.05.059

Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis

Yechuan Chen, Rohan Gokhale, Alexey Serov, Kateryna Artyushkova, Plamen Atanassov

Research output: Contribution to journal › Article › peer-review

88 Scopus citations

Abstract

Among several candidates considered to replace expensive platinum based catalysts for oxidation reduction reaction (ORR) in fuel cells, iron-nitrogen-carbon (Fe-N-C) composites attract the most interest. In this work, we design a novel method to prepare Fe-N-C catalysts for ORR in both acid and alkaline media. It involves initial polymerization of different amino-pyridines to form a C-N-C backbone, followed by their high-temperature pyrolysis on silica template, HF etching and second heat treatment in ammonia. Polymerization of 2-amino-6-methylpyridine and 2,6-diaminopyridine was done by in-situ and ex-situ templating methods. The catalysts synthesized by this method possess half-wave potentials of ~ 0.88 V versus RHE in O₂ saturated 1 M KOH electrolyte, and the best catalyst based on 2-amino-6-methylpyridine was seen to achieve an E_1/2 greater than 0.7 V in the O₂ saturated 0.5 M sulfuric acid electrolyte. Importantly, the catalysts prepared by this novel method exhibit remarkably low peroxide yield in both acid and base media (< 4% and < 1.3%, respectively) as revealed by rotating ring disk electrode (RRDE) studies.

Original language	English
Pages (from-to)	201-209
Number of pages	9
Journal	Nano Energy
Volume	38
DOIs	https://doi.org/10.1016/j.nanoen.2017.05.059
State	Published - Aug 2017
Externally published	Yes

Funding

The authors would like to acknowledge the projects, Daihatsu Motor Company “Novel Electrocatalysts for Oxygen Reduction in Alkaline Media” and US Department of Energy EERE “High-Performance Platinum Group Metal Free Membrane Electrode Assemblies Through Control of Interfacial Processes” [grant number DE-FOA-0000966]. In addition, the acknowledgment for the usage of Raman spectrometer will be given to U.S. Army Research Office “Nanomaterials Characterization Facility: Confocal Raman Microscope/Atomic Force Microscopy - WITec Alpha 300R” [grant number W911NF1410092].

Funders	Funder number
Daihatsu Motor Company
US Department of Energy EERE	DE-FOA-0000966
Army Research Office	W911NF1410092

Keywords

Oxygen reduction reaction
Polymerization pyrolysis
Silica template

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.nanoen.2017.05.059

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title = "Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis",

abstract = "Among several candidates considered to replace expensive platinum based catalysts for oxidation reduction reaction (ORR) in fuel cells, iron-nitrogen-carbon (Fe-N-C) composites attract the most interest. In this work, we design a novel method to prepare Fe-N-C catalysts for ORR in both acid and alkaline media. It involves initial polymerization of different amino-pyridines to form a C-N-C backbone, followed by their high-temperature pyrolysis on silica template, HF etching and second heat treatment in ammonia. Polymerization of 2-amino-6-methylpyridine and 2,6-diaminopyridine was done by in-situ and ex-situ templating methods. The catalysts synthesized by this method possess half-wave potentials of ~ 0.88 V versus RHE in O2 saturated 1 M KOH electrolyte, and the best catalyst based on 2-amino-6-methylpyridine was seen to achieve an E1/2 greater than 0.7 V in the O2 saturated 0.5 M sulfuric acid electrolyte. Importantly, the catalysts prepared by this novel method exhibit remarkably low peroxide yield in both acid and base media (< 4% and < 1.3%, respectively) as revealed by rotating ring disk electrode (RRDE) studies.",

keywords = "Oxygen reduction reaction, Polymerization pyrolysis, Silica template",

author = "Yechuan Chen and Rohan Gokhale and Alexey Serov and Kateryna Artyushkova and Plamen Atanassov",

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doi = "10.1016/j.nanoen.2017.05.059",

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T1 - Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis

AU - Chen, Yechuan

AU - Gokhale, Rohan

AU - Serov, Alexey

AU - Artyushkova, Kateryna

AU - Atanassov, Plamen

PY - 2017/8

Y1 - 2017/8

N2 - Among several candidates considered to replace expensive platinum based catalysts for oxidation reduction reaction (ORR) in fuel cells, iron-nitrogen-carbon (Fe-N-C) composites attract the most interest. In this work, we design a novel method to prepare Fe-N-C catalysts for ORR in both acid and alkaline media. It involves initial polymerization of different amino-pyridines to form a C-N-C backbone, followed by their high-temperature pyrolysis on silica template, HF etching and second heat treatment in ammonia. Polymerization of 2-amino-6-methylpyridine and 2,6-diaminopyridine was done by in-situ and ex-situ templating methods. The catalysts synthesized by this method possess half-wave potentials of ~ 0.88 V versus RHE in O2 saturated 1 M KOH electrolyte, and the best catalyst based on 2-amino-6-methylpyridine was seen to achieve an E1/2 greater than 0.7 V in the O2 saturated 0.5 M sulfuric acid electrolyte. Importantly, the catalysts prepared by this novel method exhibit remarkably low peroxide yield in both acid and base media (< 4% and < 1.3%, respectively) as revealed by rotating ring disk electrode (RRDE) studies.

AB - Among several candidates considered to replace expensive platinum based catalysts for oxidation reduction reaction (ORR) in fuel cells, iron-nitrogen-carbon (Fe-N-C) composites attract the most interest. In this work, we design a novel method to prepare Fe-N-C catalysts for ORR in both acid and alkaline media. It involves initial polymerization of different amino-pyridines to form a C-N-C backbone, followed by their high-temperature pyrolysis on silica template, HF etching and second heat treatment in ammonia. Polymerization of 2-amino-6-methylpyridine and 2,6-diaminopyridine was done by in-situ and ex-situ templating methods. The catalysts synthesized by this method possess half-wave potentials of ~ 0.88 V versus RHE in O2 saturated 1 M KOH electrolyte, and the best catalyst based on 2-amino-6-methylpyridine was seen to achieve an E1/2 greater than 0.7 V in the O2 saturated 0.5 M sulfuric acid electrolyte. Importantly, the catalysts prepared by this novel method exhibit remarkably low peroxide yield in both acid and base media (< 4% and < 1.3%, respectively) as revealed by rotating ring disk electrode (RRDE) studies.

KW - Oxygen reduction reaction

KW - Polymerization pyrolysis

KW - Silica template

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JO - Nano Energy

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ER -

Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis

Abstract

Funding

Keywords

UN SDGs

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