Abstract
Abstract Metal organic frameworks (MOFs) are rarely reported to be grown at the templates due to the strong inherent driving force for crystallization. Herein, we report a pathway to successfully synthesize Zeolitic imidazolate framework-67 (ZIF-67) grown at the unmodified SiO2 spheres from amorphous precursors, and further construct Pudding-typed electrocatalysts, where cobalt sulfides (CoSx) nanocrystals are embedded into nitrogen and sulfur dual-doped hollow carbon spheres (N, S-HCS). CoSx/N, S-HCS show good catalytic activity toward the oxygen reduction reaction (ORR), and the optimized performance is achieved with (CoSx/N, S-HCS)700 with the positive half-wave potentials of 0.90 V vs RHE, high selectivity, good long-term stability, and excellent tolerance against methanol-crossover effect in alkaline medium, which are even superior to that of the as-reported MOFs-derived catalysts and commercial Pt/C catalysts. The remarkable catalytic performance is originated from high reactivity of catalytic active sites composed of cobalt sulfides and nitrogen and sulfur dual-doped carbon matrices, and Pudding-typed hollow structure with proper graphitization degree to facilitate fast electron and ion transport and limit the dissolution and agglomeration of active sites during long-term operation.
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