Abstract
Abstract Although Fe–N/C catalysts have received increasing attention in recent years for oxygen reduction reaction (ORR), it is still challenging to precisely control the active sites during the preparation. Herein, we report Fe x N@RGO catalysts with the size of 2–6 nm derived from the pyrolysis of graphene oxide and 1,1′-diacetylferrocene as C and Fe precursors under the NH3/Ar atmosphere as N source. The 1,1′-diacetylferrocene transforms to Fe3O4 at 600°C and transforms to Fe3N and Fe2N at 700°C and 800°C, respectively. The as-prepared Fe x N@RGO catalysts exhibited superior electrocatalytic activities in acidic and alkaline media compared with the commercial 10% Pt/C, in terms of electrochemical surface area, onset potential, half-wave potential, number of electrons transferred, kinetic current density, and exchange current density. In addition, the stability of FGN-8 also outperformed commercial 10% Pt/C after 10000 cycles, which demonstrates the as-prepared Fe x N@RGO as durable and active ORR catalysts in acidic media.
Highlights
Fe–N/C catalysts have received increasing attention in recent years for oxygen reduction reaction (ORR), it is still challenging to precisely control the active sites during the preparation
This study demonstrates a simple strategy to capture FexO particles decomposed from 1,1′-diacetylferrocene in a high-temperature environment by a variety of oxygencontaining functional groups on the GO/Reduced graphene oxide (RGO) surface, and to in situ prepare FexN nanoparticles by reaction with NH3 and Ar atmosphere (NH3/Ar) at high temperature
GO and 1,1′-diacetylferrocene mixtures were heat-treated in NH3/Ar at 600, 700, and 800°C (FGN-6, FGN-7, and FGN-8)
Summary
Abstract: Fe–N/C catalysts have received increasing attention in recent years for oxygen reduction reaction (ORR), it is still challenging to precisely control the active sites during the preparation. The asprepared FexN@RGO catalysts exhibited superior electrocatalytic activities in acidic and alkaline media compared with the commercial 10% Pt/C, in terms of electrochemical surface area, onset potential, half-wave potential, number of electrons transferred, kinetic current density, and exchange current density. The development of non-noble metal (transition metal, carbon-based) electrocatalytic materials suitable for acidic and alkaline hydrolytic materials with high activity and stability as the negative electrode of fuel and metal–air batteries has become a potential strategy [11,12,13]. According to the characterization results, the asprepared catalysts showed premium ORR catalytic activity in both acidic and alkaline media when compared with the commercial Pt/C catalyst and rank among the top FexN-based electrocatalysts, as shown in the Supporting Information (Table S1). The electrochemical surface area (ECSA) ratio of FGN-8 versus Pt/C increased from 4.33 to 7.66 after 10,000 cycles, which indicates its excellent cycling stability in an acidic electrolyte
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