铁酸镍负载杉木屑生物炭活化过一硫酸盐降解磷酸氯喹  

Preparation of nickel ferrite loaded fir sawdust biochar to activate peroxymonosulfate for chloroquine phosphate degradation

作　　者：王俊辉 张菁玮 孙静 鄢经缘 徐梓淞 江露莹 黄燕 韩彪 张寒冰 郝格日乐[1] 何思静 朱华凤 WANG Junhui;ZHANG Jingwei;SUN Jing;YAN Jingyuan;XU Zisong;JIANG Luying;HUANG Yan;HAN Biao;ZHANG Hanbing;HAO Gerile;HE Sijing;ZHU Huafeng(School of Resources,Environment and Materials,Guangxi University,Nanning 530004,China;Scientific Research Academy of Guangxi Environmental Protection,Nanning 530022,China;Petrochemical Resources Processing and Process Reinforcement Technology Key Laboratory of Guangxi Province,School of Chemistry and Chemical Engineering,Guangxi University,Nanning 530004,China;Guangxi Key Laboratory of Emerging Contaminants Monitoring,Early Warning and Environmental Health Risk Assessment,Guangxi University,Nanning 530004,China)

机构地区：[1]广西大学资源环境与材料学院,南宁530004 [2]广西壮族自治区环境保护科学研究院,南宁530022 [3]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,南宁530004 [4]广西大学广西新污染物监测预警与环境健康评估重点实验室,南宁530004

出　　处：《复合材料学报》2024年第8期4310-4323,共14页Acta Materiae Compositae Sinica

基　　金：国家自然科学基金(52263029);广西自然科学基金(2020GXNSFAA297036);广西石化资源加工及过程强化技术重点实验室主任基金(2022Z005)。

摘　　要：近年来,磷酸氯喹(Chloroquine phosphate,CQP)作为治疗新冠的特效药得到广泛应用,并且由于其具有优异的抗炎症和抗疟疾能力,在疫情结束后仍发挥着重要作用。磷酸氯喹的大量使用对环境造成严重的潜在危害。将废弃的木屑资源化利用,通过共沉淀-无氧煅烧法制备出具有磁回收能力的铁酸镍负载杉木屑生物炭复合材料(Nickel ferrate loaded biochar,NiFe_(2)O_(4)@BC),并研究其活化过一硫酸盐(Peroxymonosulfate,PMS)降解CQP的性能。利用多种表征对NiFe_(2)O_(4)@BC复合材料的组成结构、表面官能团和石墨化程度进行分析,相较于未改性的杉木屑生物炭(Fir sawdust biochar,BC),将具有磁性NiFe_(2)O_(4)的负载在生物炭上,使复合材料的石墨化程度提高,缺陷活性位点也得到增多,对CQP的去除效果得到巨大提高。主要考察了NiFe_(2)O_(4)@BC投加量、PMS浓度、溶液初始pH、共存无机阴离子与腐殖酸在降解CQP过程中的影响。研究表明:当Ni Fe_(2)O_(4)@BC投加量为0.5 g/L,PMS浓度为1.0 mmol/L,CQP浓度为10 mg/L的条件下,CQP去除率在120 min达到89%。在偏酸性或者偏碱的条件下更有利于CQP的降解,腐殖酸(Humic acid,HA)对NiFe_(2)O_(4)@BC活化PMS降解CQP具有促进作用。淬灭实验证实,自由基途径和非自由基途径生成的·OH与^(1)O_(2)主导了NiFe_(2)O_(4)@BC/PMS体系对CQP的降解。在同等条件下,对多种污染物均能达到80%以上的降解效果。此外,NiFe_(2)O_(4)@BC循环使用5次后,活化PMS去除CQP的效率仍能达到74%左右。本文为废弃杉木屑高效、绿色的资源化利用提供了新策略和借鉴意义。In recent years,chloroquine phosphate(CQP)has been widely used as a specific drug for the treatment of COVID-19.Even after the epidemic ended,it still plays an important role because of its anti-inflammatory and antimalaria capabilities.The widespread use of chloroquine phosphate poses serious potential hazards to the environment.Utilizing waste wood chips as resources,a nickel ferrite loaded biochar composite material(NiFe_(2)O_(4)@BC)with magnetic recovery was prepared by co precipitation anaerobic calcination method,and study the performance of activating peroxymonosulfate(PMS)to degrade CQP.The compositional structure,surface functional groups,and degree of graphitization of the NiFe_(2)O_(4)@BC composite were analyzed using various characterizations.Compared with unmodified fir sawdust biochar(BC),the loading of magnetic NiFe_(2)O_(4)on the biochar resulted in an increase in the degree of graphitization of the composite,and an increase in the number of defective active sites,which led to a tremendous increase in the effectiveness of the removal of CQP.The effects of NiFe_(2)O_(4)@BC dosing,PMS concentration,initial pH of the solution,inorganic anions,and humic acid in the degradation of CQP were mainly investigated.Research shows that when NiFe_(2)O_(4)@BC under the conditions of 0.5 g/L dosage,1.0 mmol/L PMS concentration,and 10 mg/L CQP concentration,the CQP removal rate reaches 89%in 120 min.The degradation of CQP is more favorable under acidic or alkaline conditions,and humic acid(HA)has a promoting effect on the degradation of CQP by NiFe_(2)O_(4)@BC-activated PMS.Quenching experiments confirm that•OH and ^(1)O_(2) generated by the radical and non-radical pathways dominated the degradation of CQP by the NiFe_(2)O_(4)@BC/PMS system.Under the same conditions,it can achieve more than 80%degradation effect for many kinds of pollutants.In addition,the efficiency of CQP removal by activated PMS could still reach about 74%after NiFe_(2)O_(4)@BC was recycled 5 times.This study provides new strategies and refe

关 键 词：生物炭 降解 木屑 铁酸镍 磷酸氯喹 过一硫酸盐 

分 类 号：X703[环境科学与工程—环境工程] TB332[一般工业技术—材料科学与工程]