N-doped hierarchically porous carbon for highly efficient metal-free catalytic activation of peroxymonosulfate in water: A non-radical mechanism.

Metal-free carbo-catalyst has recently emerged as a promising candidate as a substituent for tradition-metal based heterogeneous catalyst for catalytic activation of peroxymonosulfate (PMS). However, most reported carbo-catalysts suffer from low catalytic efficiency and poor stability, thus a high-performance catalyst is urgently desired. In this study, a novel carbo-catalyst (NHPC-800), prepared by using tannic acid and dicyandiamide as renewable carbon/nitrogen feedstocks via a simple pyrolysis route, is reported as an activator of PMS with highly efficient catalytic ability and stability. The as-prepared NHPC-800 possesses as high as 22.4 atom% of nitrogen dopants and a hierarchically porous structure with abundant meso/macropores, accompanied by the abundant edges and wrinkles, which supply sufficient exposed catalytically active centers and fast electrons/mass transportations. Using rhodamine B as a model pollutant, the NHPC-800 shows a highly efficient catalytic ability which is superior to most reported carbo-catalysts and even some state-of-the-art metal catalysts. Based on competitive quenching experiments and electron paramagnetic resonance (EPR) results, a non-radical pathway involving the generation of O is responsible for the degradation of pollutants. Given that the NHPC-800 shows good recycling performance and strong resistance to adventitious interference such as anions and natural organic matters, we believe NHPC-800 can be a promising candidate for practical applications, and this study can provide inspirations for the further development of highly efficient carbo-catalysts.