One-Pot Synthesis of Fe-N-Containing Carbon Aerogel for Oxygen Reduction Reaction

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ORIGINAL RESEARCH

One-Pot Synthesis of Fe-N-Containing Carbon Aerogel for Oxygen Reduction Reaction Youling Wang 1 & Sandrine Berthon-Fabry 1 Accepted: 11 November 2020 # Springer Science+Business Media, LLC, part of Springer Nature 2020

Abstract Three-dimensional Fe-N-C aerogel catalysts for the oxygen reduction reaction (ORR) are prepared with resorcinol–formaldehyde–melamine and iron precursor using one-pot sol-gel process followed by supercritical drying and heat treatment in nitrogen (N2) and then ammonia (NH3) atmospheres. We studied the effect of the synthesis conditions (Fe precursor and Fe content) of organic aerogel and the heat treatment parameters (including temperature and duration) under N2/NH3 atmosphere on the structural properties and ORR catalytic activities of the resulting Fe-N-C aerogel catalysts. The Fe-N-C aerogel catalysts were characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, and N2-adsorption/desorption, and the ORR activities were studied by the rotating disk electrode method. It was found that the pore structure, the chemical composition, and ultimately the ORR performance were largely affected by the nature of iron precursor, iron content, and the conditions of heat treatment. The catalysts using Iron (III) acetylacetonate as Fe precursor incorporated with 3 wt% of Fe followed by the HT at 800 °C for 1 h under N2 and then 950 °C under NH3 for 30 min showed the highest content of active site (Fe-Nx) and largest mesopore volume, resulting in an enhanced catalytic activity and mass-transport property. Keywords Non-precious metal catalyst . Carbon aerogel . Acidic media . Oxygen reduction reaction

Introduction The oxygen reduction reaction (ORR) is one of the most important reactions in energy storage/conversion systems such as proton-exchange membrane fuel cells (PEMFCs) and metal-air batteries. In PEMFCs, the kinetics of the ORR occurred at the cathode is found to be five times slower than the kinetics at the anode, leading to a high voltage loss through the system and as a result a diminished overall performance. To date, Pt-based catalysts are still considered the most efficient catalysts for the ORR, whereas the high cost, scarcity, and the poor durability of Pt hinder the practical application of PEMFCs [1]. Therefore, developing non-precious metal catalysts (NPMCs) for the ORR is of extreme significance and could be a long-term solution to realize the commercialization of PEMFCs. Among various

* Sandrine Berthon-Fabry [email protected] 1

MINES ParisTech, PSL University, Centre Procédés, Énergies Renouvelables et Systèmes Énergétiques (PERSEE), CS 10207 rue Claude Daunesse 06904, Sophia Antipolis, Cedex, France

NPMCs (e.g., transition metal oxides, carbides, nitrides, chalcogenides, metal-N-C catalysts), Fe-N-C materials have been regarded as the most promising alternative for the ORR in acidic medium [1–4]. In the past decade, much progress has been made in improving the activity and durability of the Fe-