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Micrometer-sized NiOOH hierarchical spheres for enhanced degradation of sulfadiazine via synergistic adsorption and catalytic oxidation in peroxymonosulfate system

Chinese Chemical Letters(2022)

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摘要
As an antibiotic,sulfadiazine has posed a serious threat to humans and ecosystems due to its chronic toxicity.The advanced oxidation processes(AOPs)via heterogeneous catalytic activation of peroxymono-sulfate(PMS)have significant potential for the degradation of antibiotics.However,there are multiple restrictions including non-specifically binding to target contaminants,which would deplete oxidation ca-pacity,and lacking energy effectiveness due to inefficient utilization of reactive oxygen species(ROS).To overcome these obstacles,we adopted the"bait-hook&destroy"strategy in this study.Herein,we syn-thesized a novel micrometer-sized NiOOH hierarchical spheres assembled from nanosheets,which have relatively large specific surface areas and yield specified cavities to"bait-hook"sulfadiazine and PMS onto the surface cavities.This process was further conductive to effective generation of ROS and subsequently"destruction"of sulfadiazine with elevated mass transformation rate.20.4%of sulfadiazine can adsorb to NiOOH surface in less than 30 min(0.0051 min-1),and then sulfadiazine was completely degraded in 90 min intervals in the NiOOH/PMS system.The degradation rate constant(k=0.0537 min-1)was about 5.3,2.5 and 2.2 times higher than that in Ni2O3/PMS,NiO/PMS and Ni(OH)2/PMS system,respectively.This was ascribed to the synergistic catalytic oxidation and adsorption process occurred on the surface of NiOOH.Appreciably,there were both non-radicals(1O2)and radicals(O2·-and SO4·-)involved in the NiOOH/PMS system,and 1O2 was distinguished as the dominated ROS for degradation of sulfadiazine.This study provides a novel strategy via synergistic adsorption and catalytic oxidation,and indicates that the micrometer-sized NiOOH hierarchical sphere as heterogeneous catalyst is an attractive candidate for potential application of the SR-AOPs technology in water treatment.
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关键词
Nickel oxyhydroxide,Peroxymonosulfate,Sulfate radical,Singlet oxygen,Sulfadiazine
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