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catalytic destruction of chlorobenzene over K-OMS-2: Inhibition of high toxic byproducts via phosphate modification

Journal of Environmental Sciences 2023年第5期127卷 844-854页

作者： Yunpeng Long Jiajia Liu Meiling Chen Renna Li Xiaole Weng Zhongbiao Wu Key Laboratory of Environment Remediation and Ecological Health Ministry of EducationCollege of Environmental and Resource SciencesZhejiang UniversityHangzhou 310058China Zhejiang Provincial Engineering Research Center of Industrial Boiler and Furnace Flue Gas Pollution Control Zhejiang University-Hangzhou Global Scientific and Technological Innovation CenterHangzhou 311200China

In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing great risk to atmospheric environment and human health.To solve these problems,this work applied phosphate to modify K-OMS-2 catalysts.The physicochemical properties of catalysts were determined by using X-ray powder diffraction(XRD),scanning electron microscope(SEM),X-ray photoelectron spectroscopy(XPS),hydrogen temperature programmed reduction(H_(2)-TPR),pyridine adsorption Fouriertransform infrared(Py-IR)and water temperature programmed desorption(H_(2)O-TPD),and chlorobenzene was selected as a model pollutant to explore the catalytic performance and byproduct inhibition function of phosphating.Experimental results revealed that 1 wt.%phosphate modification yielded the best catalytic activity for chlorobenzene destruction,with the 90%conversion(T90)at approximately 247℃.The phosphating significantly decreased the types and yields of polychlorinated byproducts in effluent.After phosphating,we observed significant hydroxyl groups on catalyst surface,and the active centerwas transformed into Mn(IV)-O…H,which promoted the formation of HCl,and enhanced the dechlorination process.Furthermore,the enriched Lewis acid sites by phosphating profoundly enhanced the deep oxidation ability of the catalyst,which promoted a rapid oxidation of reaction intermediates,so as to reduce byproducts generation.This study provided an effective strategy for inhibiting the toxic byproducts for the catalytic destruction of chlorinated organics.

关键词： catalytic destruction Chlorinated organics Phosphoric modification K-OMS-2 Secondary pollution

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