MnFe2O4-CR的制备及其活化过一硫酸盐降解盐酸四环素性能
Preparation of MnFe2O4-CR and its activation performance on peroxymonosulfate for tetracycline hydrochloride degradation
陈丛瑾 1黄丽斌 1范辉 1张强煦 1廖金戈 1陈紫霞1
作者信息
- 1. 广西大学 化学化工学院 广西石化资源加工及过程强化技术重点实验室,广西 南宁 530004
- 折叠
摘要
利用水热法将MnFe2O4负载在生物质汽化炭渣(CR)上,得到了负载型复合催化剂MnFe2O4-CR,通过SEM、XRD、XPS、BET和VSM对MnFe2O4-CR进行了表征,将其用于活化过一硫酸盐(PMS)降解盐酸四环素(TC).考察了不同反应体系、MnFe2O4 与CR质量比、PMS用量、催化剂用量、温度、pH、阴离子(HCO3-、H2PO4-、Cl-、NO3-)和腐植酸(HA)对MnFe2O4-CR/PMS体系降解TC的影响,探究了MnFe2O4-CR的稳定性和循环使用性,并探讨了MnFe2O4-CR/PMS体系中TC可能的降解机理.结果表明,MnFe2O4与CR质量比为1∶2时制备的MnFe2O4-CR催化效果良好,在30℃、30 mg MnFe2O4-CR、40 mg PMS、90 min的条件下,100 mL质量浓度为50 mg/L自然pH的TC溶液中TC的降解率达到91.32%.MnFe2O4-CR可利用其磁性回收,经过5次循环利用,催化PMS降解TC的降解率仍能达到82.90%,表明MnFe2O4-CR具有良好的稳定性和重复使用性.MnFe2O4-CR/PMS 体系中,硫酸根自由基(SO4-·)、·OH、单线态氧(1O2)和过氧自由基(O2-·)是降解 TC 的主要活性氧物种,并提出了相应的催化降解机理.
Abstract
Supported composite catalyst MnFe2O4-CR was prepared from loading MnFe2O4 onto biomass gasification carbon residue(CR)by hydrothermal method,characterized by SEM,XRD,XPS,BET and VSM,and then utilized to activate peroxymonosulfate(PMS)for tetracycline hydrochloride(TC)degradation.The effects of different reaction systems,mass ratio of MnFe2O4 to CR,PMS dosage,catalyst dosage,temperature,pH,anions(HCO3-,H2PO4-,Cl-,NO3-)and humic acid(HA)on degradation of TC in MnFe2O4-CR/PMS system were investigated.The stability and recyclability of MnFe2O4-CR as well as the TC degradation mechanism were further analyzed.The MnFe2O4-CR prepared with a mass ratio of MnFe2O4 to CR of 1∶2 exhibited good catalysis performance,with a degradation rate of TC in 100 mL TC solution with natural pH and with a mass concentration of 50 mg/L reaching 91.32%under the conditions of temperature 30℃,30 mg MnFe2O4-CR,40 mg PMS and 90 min.The MnFe2O4-CR could be recovered by its magnetic properties.After 5 cycles,the TC degradation rate in MnFe2O4-CR/PMS system could still reach 82.90%,demonstrating the good stability and reusability of MnFe2O4-CR.It was also found that SO4-·,·OH,singlet oxygen(1O2)and O2-·were the main reactive oxygen species for TC degradation in MnFe2O4-CR/PMS system,and the corresponding catalytic degradation mechanism was discussed.
关键词
MnFe2O4-CR/盐酸四环素/高级氧化技术/复合催化剂/过一硫酸盐/降解/催化技术Key words
MnFe2O4-CR/tetracycline hydrochloride/advanced oxidation technology/composite catalysts/peroxymonosulfate/degradation/catalysis technology引用本文复制引用
基金项目
国家自然科学基金项目(31660183)
广西石化资源加工及过程强化技术重点实验室主任基金项目(2022Z007)
广西大学2022大学生创新创业训练计划自治区级创新训练一般项目(S202210593278)
出版年
2024
NETL
NSTL
万方数据