Abstract
It is still a challenge to synthesize non-precious-metal catalysts with high activity and stability for the oxygen reduction reaction (ORR) to replace the state-of-the art Pt/C catalyst. Herein, a Fe, N, S co-doped porous carbon (Fe-NS/PC) is developed by using g-C3N4 and 2,4,6-tri(2-pyridyl)-1,3,5-triazine (TPTZ) as binary nitrogen precursors. The interaction of binary nitrogen precursors not only leads to the formation of more micropores, but also increases the doping amount of both iron and nitrogen dispersed in the carbon matrix. After a second heat-treatment, the best Fe/NS/C-g-C3N4/TPTZ-1000 catalyst exhibits excellent ORR performance with an onset potential of 1.0 V vs. reversible hydrogen electrode (RHE) and a half-wave potential of 0.868 V (RHE) in alkaline medium. The long-term durability is even superior to the commercial Pt/C catalyst. In the meantime, an assembled Zn-air battery with Fe/NS/C-g-C3N4/TPTZ-1000 as the cathode shows a maximal power density of 225 mW·cm−2 and excellent durability, demonstrating the great potential of practical applications in energy conversion devices.
Highlights
The oxygen reduction reaction (ORR) plays an important role in the energy efficiency of polymer electrolyte membrane fuel cells (PEMFCs) and metal-air batteries (MABs)
We have developed a facile method to synthesize Fe, N, S co-doped porous carbon materials (Fe-NS/PC) as efficient ORR catalysts with g-C3 N4 and 2,4,6-tri(2-pyridyl)-1,3,5-triazine (TPTZ) as binary nitrogen precursors
Catalysts using g-C3 N4 and TPTZ separated as single nitrogen precursor and together as binary nitrogen precursors, denoted as Fe/NS/C-g-C3 N4, Fe/NS/C-TPTZ, and Fe/NS/C-g-C3 N4 /TPTZ, respectively
Summary
The oxygen reduction reaction (ORR) plays an important role in the energy efficiency of polymer electrolyte membrane fuel cells (PEMFCs) and metal-air batteries (MABs). High surface area and porous structure are beneficial to increase the number of accessible active sites and facilitate the mass transport of the ORR relevant species approaching the internal active sites of catalysts [13,14]. The use of binary nitrogen precursors has been developed as an effective synthetic strategy to improve the porosity and heteroatoms doping contents, to improve the ORR activity. The superior ORR activity can be ascribed to the increased content of pyridinic nitrogen doped into the carbon matrix. We have developed a facile method to synthesize Fe, N, S co-doped porous carbon materials (Fe-NS/PC) as efficient ORR catalysts with g-C3 N4 and 2,4,6-tri(2-pyridyl)-1,3,5-triazine (TPTZ) as binary nitrogen precursors.
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