摘要
以玉米秸秆为生物炭原料,在600℃高温缺氧条件下煅烧成炭,并利用共沉淀法在其上负载Fe_3O_4,制得Fe_3O_4@玉米秸秆炭磁性非均相芬顿催化剂。运用XRD、SEM、EDS和TEM技术对材料进行表征,研究其在不同条件下光-类Fenton协同催化降解水中盐酸四环素的性能,考察材料的磁性回收能力和催化稳定性。结果表明,Fe_3O_4纳米颗粒均匀覆盖在炭载体表面,整体形貌上保持玉米秸秆通道状多孔结构。初始pH=7条件下降解盐酸四环素的最佳参数为:溶液初始过氧化氢量为10 mmol/L、Fe_3O_4@玉米秸秆炭催化剂投加量为0.3 g/L、反应时间为60 min。材料具有pH为3~7的适用范围和磁性回收能力。催化剂稳定性强,进行5次重复实验后仍可保持98%的降解率。
The maize straws were used as biological carbon material, calcined at 600 ℃ under high temperature and anoxic conditions and Fe_3O_4 was loaded on it by co-precipitation method to prepare Fe_3O_4@maize straws carbon magnetic heterogenous Fenton catalyst. The materials were characterized by XRD, SEM, EDS and TEM. The photo-Fenton-like degradation of tetracycline hydrochloride in water was studied under different conditions. The magnetic recovery and catalytic stability of the materials were investigated. The results show that the Fe_3O_4 nano-particles uniformly cover the surface of the carbon support and the overall morphology maintains the channel-like porous structure of maize straws. The optimal parameters for the tetracycline hydrochloride degradation under the initial pH 7 condition are as the initial amount of H_2O_2 in the solution 10 mmol/L,the dosage of Fe_3O_4@maize straws carbon 0.3 g/L and the reaction time 60 min. The material has a pH range of 3 to 7 and magnetic recovery. It has strong catalytic stability and can maintain a 98% degradation rate after 5 repeated experiments.
引文
[1]蒋胜韬,祝建中,管玉江,等.Si-FeOOH/H2O2类芬顿降解盐酸四环素废水的效能及其机理[J].化工学报,2015,66(10):4244-4251.
[2]Babak Kakavandi,Ali Esrafili,Anoushiravan Mohseni Bandpi,et al.Magnetic Fe3O4@C nanoparticles as adsorbents for removal of amoxicillin from aqueous solution[J].Water Science&Technology,2014,69(1):147-155.
[3]魏雅男.铁基MOF/蚕沙气凝胶复合材料及类芬顿超声/光协同催化降解农药噻虫嗪[D].南宁:广西大学,2017.
[4]易龙生,刘超,何磊.载铁活性炭非均相Fenton催化剂的制备及应用[J].环境污染与防治,2018,40(3):329-333,338.
[5]郭彦青.非均相UV/类Fenton工艺处理高浓度难降解有机废水的研究[D].呼和浩特:内蒙古大学,2017.
[6]Babak Kakavandi,Afshin Takdastan,Nemat Jaafarzadeh,et al.Application of Fe3O4@C catalyzing heterogeneous UV-Fenton system for tetracycline removal with a focus on optimization by a response surface method[J].Journal of Photochemistry and Photobiology A:Chemistry,2016,314(1):178-188.
[7]张志红,赵秀峰,杨丽.纳米Fe3O4异相催化光/Fenton反应降解有机染料[J].环境污染与防治,2013,35(9):112.
[8]Li Keyan,Zhao Yongqin,Michael J Janik,et al.Facile preparation of magnetic mesoporous Fe3O4/C/Cu composites as high performance Fenton-like catalysts[J].Applied Surface Science,2017,396(1):1383-1392.
[9]赵文峰,曹利,黄学敏.微波制备秸秆活性炭及其对甲苯吸附性能的研究[J].环境科学与技术,2014,37(10):108-111,116.
[10]饶砚迪,盛义平,刘琦,等.Fe3O4-x TiO2复合光催化剂的制备及其对染料废水的处理效果[J].化工环保,2018,38(2):180-184.
[11]Xia Hui,Wan Yunhai,Yuan Guoliang,et al.Fe3O4/carbon core-shell nanotubes as promising anode materials for lithium-ion batteries[J].Journal of Power Sources,2013,241(1):486-493.
[12]沙大巍.改性TiO2复合材料的制备及其可见光光催化性能的研究[D].镇江:江苏大学,2017.
[13]Mohamed Mokhtar Mohamed,WA Bayoumy,ME Goher,et al.Optimization ofα-Fe2O3@Fe3O4incorporated N-TiO2as super effective photocatalysts under visible light irradiation[J].Applied Surface Science,2017,412(1):668-82.
[14]白翠萍.类Fenton高级氧化技术处理染料废水的研究[D].武汉:武汉理工大学,2012.
[15]梁大鑫,张巨擘,郑恺,等.磁性Fe3O4微球的溶剂热法合成及光芬顿性能优化[J].哈尔滨工业大学学报,2017,49(8):90-97.
[16]殷芳芳,顾升波.UV-Fenton法降解垃圾渗滤液中COD的动力学研究[J].给水排水,2017,53(S1):69-71.
[17]矫彩山,王中伟,彭美媛,等.铁炭微电解-Fenton试剂氧化法预处理广灭灵及丙草胺废水[J].化工环保,2007,1(4):349-352.
[18]黄智淼,林君,张洋,等.钛铁矿制四氧化三铁/二氧化钛及其光催化性能[J].无机盐工业,2018,50(3):69-73.