摘要
基于煤矸石大宗固废综合利用以及煤炭产业集聚区多环芳烃有机污染治理的迫切需要,以煤矸石(CG)为原料、氯化钙为活化剂,在绝氧煅烧条件下制备了煤矸石基过一硫酸氢钾复合盐(PMS)催化材料(CG/Ca)。系统研究了氯化钙用量和煅烧温度对苯并[a]芘降解的影响,同时对CG和CG/Ca样品的物相组成、表面形貌、比表面积、孔结构及化学键变化进行了表征,并通过电子顺磁共振(EPR)明晰了降解体系中的活性物种。结果表明,煤矸石与等量的氯化钙在750℃下煅烧90 min后,制备所得的CG/Ca可在30 min内完全去除苯并[a]芘,且其反应速率常数是煅烧煤矸石(CG/Ca-0)的约55倍。此外,CG中含有的硅铝骨架与氯化钙中的Ca^(2+)结合,生成含有Si—O—Ca键的钙铝榴石,孔体积和平均孔径同时增大。CG/Ca在酸性和中性环境(pH=3~7)具有良好的活化性能,且环境中Cl-和H2PO4-阴离子对苯并[a]芘降解的影响有限,说明CG/Ca材料良好的应用前景,体系中·OH、SO_(4)^(•-)、·O_(2)^(-)和^(1)O_(2)均对苯并[a]芘的降解起到促进作用。
Based on the urgent need for the comprehensive utilization of bulk solid waste from coal gangue and the treat-ment of polycyclic aromatic hydrocarbon organic pollution in coal industry areas,coal gangue-based potassium persulfate composite salt(PMS)catalytic materials(CG/Ca)were prepared by using coal gangue(CG)as the raw material and calcium chloride as the activator under anaerobic calcination conditions.The effects of calcium chloride dosage and calcination tem-perature on the degradation of benzo[a]pyrene were systematically studied.The phase composition,surface morphology,spe-cific surface area,pore structure,and chemical bond changes of CG and CG/Ca samples were characterized,and the active species in the degradation system were clarified by electron paramagnetic resonance(EPR).The results showed that after calcining coal gangue with an equal amount of calcium chloride at 750℃for 90 minutes,the prepared CG/Ca could com-pletely remove benzo[a]pyrene within 30 minutes,and its reaction rate constant was about 55 times that of calcined coal gangue(CG/Ca-0).Furthermore,the silicon-aluminum skeleton contained in CG was combined with Ca^(2+)in calcium chlo-ride to form calcium aluminum garnet containing Si—O—Ca bonds,resulting in an increase in pore volume and average pore size simultaneously.CG/Ca exhibited excellent activation performance in acidic and neutral environments(pH=3~7),and the influence of Cl-and H2PO4-anions on the degradation of benzo[a]pyrene was limited in the environment,indicating the promising application prospects of CG/Ca materials.In the system,·OH、SO_(4)^(•-)、·O_(2)^(-)and^(1)O_(2)all promoted the degrada-tion of benzo[a]pyrene.
作者
韩伟
宋永明
刘琪
徐金陵
徐荣
李春全
殷帅军
孙志明
HAN Wei;SONG Yongming;LIU Qi;XU Jinling;XU Rong;LI Chunquan;YIN Shuaijun;SUN Zhiming(Inner Mongolia Mengtai Buliangou Coal Industry Co.,Ltd.,Ordos 010399,China;Huadian Coal Industry Group Co.,Ltd.,Beijing 100035,China;Huadian Coal Industry Group Digital Intelligence Technology Co.,Ltd.,Beijing 102400,China;School of Chemical and Environmental Engineering,China University of Mining and Technology(Beijing),Beijing 100083,China)
出处
《无机盐工业》
北大核心
2025年第1期103-112,共10页
Inorganic Chemicals Industry
基金
华电煤业集团有限公司科技项目(CHDMYKJ21-02-02)
国家重点研发计划课题(2020YFC1806504)。
关键词
煤矸石
过硫酸盐活化
高级氧化技术
苯并[A]芘
氯化钙
coal gangue
persulfate activation
advanced oxidation processes
benzo[a]pyrene
calcium chloride
