Sulfur-doped porous carbon nanosheets have been prepared by pyrolysis of graphene-coupled conjugated microporous polymers under an inert atmosphere. The obtained carbon nanosheets exhibited large specific surface areas up to 642 m2 g−1 and high sulfur weight content up to 7.11%. These highly porous carbon nanosheets have been studied as metal-free oxygen reduction electrocatalysts in alkaline environments and they were found to undergo oxygen reduction via a major 4-electron transfer pathway. They were then examined as substitutes for Pt–carbon electrocatalysts in PhotoFuelCells functioning in the presence of ethanol as a model fuel. It has been shown that sulfur doped porous carbon nanosheets yield functional cells with approximately the same characteristics as those employing Pt–carbon electrocatalysts, therefore, they mark a new class of metal-free catalysts.
The development of low-Pt bifunctional electrocatalysts with excellent performance for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) is critical for the advancement of the hydrogen economy. Here, we have integrated low-loading Pt and Co metals into N, S doped porous carbon nanosheets to obtain composite catalysts encapsulating PtCo alloy nanoparticles (PtCo2@Co 9 S 8 / N -CNS and PtCo2@ N -CNS). The acquired PtCo nanoparticles, with dimensions of about 2.5 nm, are uniformly distributed and firmly anchored in N, S doped carbon nanosheets with large specific surface areas and rich pore structure, forming multiple active centers and effectively preventing the aggregation of metal nanoparticles. The PtCo2@Co 9 S 8 / N -CNS and PtCo2@ N -CNS display high ORR catalytic mass activity of 1.65 A mg Pt -1 and 1.01 A mg Pt -1 in 0.1 M HClO 4 . The PtCo2@ N -CNS catalyst exhibits excellent HER performance in 0.5 M H 2 SO 4 , with a mass activity (at 50 mV) 4.3 times higher than that of Pt/C. The PtCo2@Co 9 S 8 / N -CNS and PtCo2@ N -CNS also exhibit stronger ORR and HER stability than Pt/C after accelerated durability tests. The superior catalytic activity performance of catalysts can be attributed to the synergistic effect of multiple active centers of PtCo, Co 9 S 8 and Co-N in the catalysts. The confinement of PtCo nanoparticles by Co metal and N, S doped porous nanosheets derived from graphitic carbon nitride (g-C 3 N 4 ) as the template, which can effectively prevent the corrosion and migration of the catalysts under acidic conditions, enhances the catalytic stability of the materials. This study provides a new perspective for the development of economical and efficient bifunctional low-Pt catalysts.
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