CoFe_(2)O_(4)的制备及其活化过一硫酸盐降解磺胺甲噁唑  

Preparation of CoFe_(2)O_(4) and its peroxymonosulfate activation for degradation of sulfamethoxazole

作　　者：李英豪 郑向前 高晓亚[1,4] 朱文杰 罗永明[1,2,4] 陆继长 LI Yinghao;ZHENG Xiangqian;GAO Xiaoya;ZHU Wenjie;LUO Yongming;LU Jichang(Faculty of Environmental Science and Engineering,Kunming University of Science and Technology,Kunming 650500,Yunnan,China;Faculty of Chemical Engineering,Kunming University of Science and Technology,Kunming 650500,Yunnan,China;Xishuangbanna Prefecture Comprehensive Testing Center for Quality and Technical Supervision,Jinghong 666100,Yunnan,China;Key Laboratory for Odorous Volatile Organic Compounds Pollutants Control of Yunnan Province Colleges and Universities,Kunming 650500,Yunnan,China)

机构地区：[1]昆明理工大学环境科学与工程学院,云南昆明650500 [2]昆明理工大学化学工程学院,云南昆明650500 [3]西双版纳州质量技术监督综合检测中心,云南景洪666100 [4]云南省高校恶臭挥发性有机物控制重点实验室,云南昆明650500

出　　处：《精细化工》2022年第5期1020-1027,共8页Fine Chemicals

基　　金：国家自然科学基金(42030712,21966018,22106055);云南省基础研究计划重点项目(202101AS070026);云南省基础研究专项青年项目(202101AU070025,202105AE160019);云南省万人计划青年项目(YNWR-QNBJ-2018-067)。

摘　　要：以六水合硝酸钴和七水合硫酸亚铁为原料,采用共沉淀法在不同煅烧温度下成功合成了一系列铁酸钴材料(CoFe_(2)O_(4)-X,X代表煅烧温度,分别为450、550和650℃)。通过SEM、XRD、BET、XPS对其结构进行了表征,并将其用于活化过一硫酸盐(PMS)降解磺胺甲唑(SMX)。考察了催化剂投加量、PMS用量、pH、无机阴离子种类和反应温度对降解SMX性能的影响。结果表明,CoFe_(2)O_(4)-550具有最佳的催化性能,在最佳反应条件(SMX初始质量浓度为10 mg/L,CoFe_(2)O_(4)-550投加量为0.3 g/L,PMS质量浓度为1.5 g/L)下,20 min内,SMX的降解率可达95%,且总有机碳(TOC)降解率可达80%。同时,CoFe_(2)O_(4)-550/PMS反应体系具有较广的pH适用范围(p H=5~9)。CoFe_(2)O_(4)-550催化剂可磁性回收,经3次使用后,其对SMX的降解率仍能达到83%,表明CoFe_(2)O_(4)-550具有良好的稳定性和重复使用性。在该降解反应过程中产生了大量的SO_(4)^(-)·和·OH,并提出了相应的催化降解机理。Using cobalt nitrate hexahydrate and ferrous sulfate heptahydrate as raw materials,a series of cobalt ferrite materials(CoFe_(2)O_(4)-X,X represents calcination temperature,which are 450,550 and 650℃,respectively)were successfully synthesized by a simple co-precipitation method.They were characterized by SEM,XRD,BET and XPS,and used for activation peroxymonosulfate(PMS)to degrade sulfamethoxazole(SMX).The effects of catalyst dosage,PMS dosage,pH,inorganic ion species and reaction temperature on the degradation of SMX were investigated.The results showed that CoFe_(2)O_(4)-550 exhibited the best catalytic performance.Under the optimal reaction conditions(SMX initial mass concentration of 10 mg/L,CoFe_(2)O_(4)-550 dosage of 0.3 g/L and PMS mass concentration of 1.5 g/L),the degradation rate of SMX could reach 95%within 20 min and total organic carbon(TOC)removal rate was 80%.At the same time,CoFe_(2)O_(4)-550/PMS reaction system had excellent catalytic performance at a wide pH range(pH=5~9).CoFe_(2)O_(4)-550 could be recovered magnetically,and the removal rate of SMX could still reach 83%after three reaction cycles,indicating that CoFe_(2)O_(4)-550 had good stability and reusability.A large amount of SO_(4)^(-)·and·OH radicals were produced during the degradation reaction,and the corresponding catalytic degradation mechanism was proposed.

关 键 词：铁酸钴 过一硫酸盐 磺胺甲唑 降解 催化 水处理技术 

分 类 号：TQ138.1[化学工程—无机化工] X505[环境科学与工程—环境工程] TQ426