Abstract
We report the first investigation of dual-doped graphene/perovskite mixtures as catalysts for oxygen reduction. Pairwise combinations of boron, nitrogen, phosphorus and sulfur precursors were co-reduced with graphene oxide and mixed with La0.8Sr0.2MnO3 (LSM) to produce SN-Gr/LSM, PN-Gr/LSM and BN-Gr/LSM catalysts. In addition, the dual-doped graphenes, graphene, LSM, and commercial Pt/C were used as controls. The addition of LSM to the dual-doped graphenes significantly improved their catalytic performance, with optimised composition ratios enabling PN-Gr/LSM to achieve 85% of the current density of commercial Pt/C at −0.6V (vs. Ag/AgCl) at the same loading. The effective number of electrons increased to ca. 3.8, and kinetic analysis confirms the direct 4 electron pathway is favoured over the stepwise (2e+2e) route: the rate of peroxide production was also found to be lowered by the addition of LSM to less than 10%.
Highlights
We report the first investigation of dual-doped graphene/perovskite mixtures as catalysts for oxygen reduction
Research effort continues to focus on the oxygen reduction reaction (ORR) due to its importance in energy device applications and, in particular, the search for more abundant and inexpensive catalyst replacements for the Pt-group materials is attracting increasing attention [1,2,3]
We investigate combining dual-doped graphenes with a perovskite for the first time. These materials exhibit improved electrocatalytic activity due to the synergic effects of the dual-doped graphene/perovskite, and optimisation of the composition obtains the best performance in terms of both current densities and number of electrons transferred in the ORR yields results that approach that of Pt/C
Summary
Research effort continues to focus on the oxygen reduction reaction (ORR) due to its importance in energy device applications (e.g., fuel cells and metal-air batteries) and, in particular, the search for more abundant and inexpensive catalyst replacements for the Pt-group materials is attracting increasing attention [1,2,3]. Dualdoped graphene with B, P or S in combination with N have been demonstrated to be catalytically active towards the oxygen reduction [12,13]. It has been proposed that the presence of carbon greatly improves the conductivity through the catalyst composite [22], whereas other workers suggest an influence of the carbon material on the ORR pathway [14,15]. We investigate combining dual-doped graphenes with a perovskite for the first time These materials exhibit improved electrocatalytic activity due to the synergic effects of the dual-doped graphene/perovskite, and optimisation of the composition obtains the best performance in terms of both current densities and number of electrons transferred in the ORR yields results that approach that of Pt/C
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