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

  • 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,NiFe2O4@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NiFe2O4@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NiFe2O4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NiFe2O4@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NiFe2O4@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NiFe2O4@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1O2主导了NiFe2O4@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,NiFe2O4@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。

     

    Abstract: 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 anti-malaria 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 (NiFe2O4@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 NiFe2O4@BC composite were analyzed using various characterizations. Compared with unmodified fir sawdust biochar (BC), the loading of magnetic NiFe2O4 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 NiFe2O4@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 NiFe2O4@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 NiFe2O4@BC-activated PMS. Quenching experiments confirm that •OH and 1O2 generated by the radical and non-radical pathways dominated the degradation of CQP by the NiFe2O4@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 NiFe2O4@BC was recycled 5 times. This study provides new strategies and reference significance for the efficient and green resource utilization of discarded fir sawdust.

     

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