废水中盐酸四环素的钡掺杂钨酸铋光催化降解
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摘要
目的探讨钡掺杂钨酸铋(钡-钨酸铋)可见光光催化对盐酸四环素(TCH)的降解特性。方法采用水热法制备钡-钨酸铋可见光光催化剂,研究不同钡掺杂量(钡与铋物质量的比为1∶10~3∶20)时钨酸铋催化剂对TCH的降解效果,同时,考察催化剂投加量(0.2~2.0 g/L)、TCH初始浓度(10~50 mg/L)、溶液初始p H值(3~11)、过氧化氢投加量(1~3 ml)时,钡-钨酸铋可见光催化反应在150 min内对TCH降解性能的影响。通过连续4次重复使用实验评价催化剂的稳定性能。结果钡与铋物质量的比为3∶20时,制备的催化剂表现出了最优的可见光光催化活性。在优化的光催化反应条件(TCH初始浓度为20 mg/L、p H 6.8、催化剂投加量为0.5 g/L)下,钡-钨酸铋对TCH的去除率高达90%以上。另外,投加过氧化氢可加快TCH的降解速率,改性催化剂有良好的稳定性能。结论钡-钨酸铋催化剂可显著提高对TCH的可见光光催化降解效能,具有一定的实际应用价值。
Objective To understand the degradation characteristics of the tetracycline hydrochloride(TCH) by using bariumdoped tungsten acid bismuth(Ba-Bi_2WO_6) as the visible light photocatalyst. Methods Ba-Bi_2WO_6 photocatalyst was prepared by hydrothermal method and the degradation effect of TCH was evaluated by using Bi_2WO_6 photocatalyst doped with different levels of Ba(Ba and Bi mole ratio of 1 ∶10-3∶20). Meanwhile,the influence of degradation characteristics of the tetracycline hydrochloride was analyzed at catalyst amounts(0.2-2.0 g/L),initial concentration of tetracycline hydrochloride(10-50 mg/L),initial p H(3-11) and H2 O2 amounts(1-3 ml) and the experiment was proceeded by the visible light photocatalyst of Ba-Bi_2WO_6 within 150 min. The stability of the catalyst was measured by four consecutive experiments. Results The modified catalyst prepared at mole ratio of 3∶20(Ba∶Bi) showed the best photocatalytic activity. Under the optimal condition of photocatalytic(the TCH concentration of 20 mg/L,p H 6.8,the catalyst dose of 0.5 g/L),the ratio of TCH removal could reach 90%. In addition,H_2O_2 could accelerate the degradation rate of the TCH,and the modified catalyst presented good stability. Conclusion The investigated Ba-doped Bi_2WO_6 can greatly improve the visible photocatalytic degradation efficiency of TCH, which has certain practical value.
Objective To understand the degradation characteristics of the tetracycline hydrochloride(TCH) by using bariumdoped tungsten acid bismuth(Ba-Bi_2WO_6) as the visible light photocatalyst. Methods Ba-Bi_2WO_6 photocatalyst was prepared by hydrothermal method and the degradation effect of TCH was evaluated by using Bi_2WO_6 photocatalyst doped with different levels of Ba(Ba and Bi mole ratio of 1 ∶10-3∶20). Meanwhile,the influence of degradation characteristics of the tetracycline hydrochloride was analyzed at catalyst amounts(0.2-2.0 g/L),initial concentration of tetracycline hydrochloride(10-50 mg/L),initial p H(3-11) and H2 O2 amounts(1-3 ml) and the experiment was proceeded by the visible light photocatalyst of Ba-Bi_2WO_6 within 150 min. The stability of the catalyst was measured by four consecutive experiments. Results The modified catalyst prepared at mole ratio of 3∶20(Ba∶Bi) showed the best photocatalytic activity. Under the optimal condition of photocatalytic(the TCH concentration of 20 mg/L,p H 6.8,the catalyst dose of 0.5 g/L),the ratio of TCH removal could reach 90%. In addition,H_2O_2 could accelerate the degradation rate of the TCH,and the modified catalyst presented good stability. Conclusion The investigated Ba-doped Bi_2WO_6 can greatly improve the visible photocatalytic degradation efficiency of TCH, which has certain practical value.
引文
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[16]宋晨怡,胡霞林,尹大强.四环素在光催化剂Ti O2上的吸附研究[J].环境化学,2011,30(7):1291-1296.
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[18]冷文华,成少安,刘鸿,等.负载型二氧化钛光催化降解苯胺[J].环境科学学报,2000,20(4):499-503.
[19]周娅.制备Ti O2/Fe2O3/CNTs复合磁性光催化剂及光催化降解四环素类抗生素[D].西安:长安大学,2013.
[2]Zhang HC,Chen WR,Huang CH.Kinetic modeling of oxidation of antibacterial agents by manganese oxide[J].Environ Sci Technol,2008,42:5548-5554.
[3]刘珊珊,杨栋,张坤明,等.天津市某地区自来水中抗生素耐药菌及其相关基因的调查[J].环境与健康杂志,2018,35(2):166-169.
[4]叶必雄,张岚.环境水体及饮用水中抗生素污染现状及健康影响分析[J].环境与健康杂志,2015,32(2):173-178.
[5]朱婷婷,宋战锋,段标标,等.深圳石岩水库抗生素污染特征与健康风险初步评价[J].环境与健康杂志,2013,30(11):1003-1006.
[6]孙刚,袁守军,计峰,等.畜禽粪便中抗生素残留危害及其研究进展[J].环境与健康杂志,2009,26(3):277-279.
[7]Reyes C,Fernandez J,Freer J,et al.Degradation and inactivation of tetracycline by Ti O2photocatalysis[J].J Photochem Photobiol A,2006,184:141-146.
[8]张孝杰.改性Zn S光催化剂的制备及其选择性吸附/光降解环丙沙星行为研究[D].南京:江苏大学,2010.
[9]王春英,单国强,陈鹏,等.光催化剂Bi3.84W0.16O6.24在模拟太阳光下对双酚A的降解[J].中国环境科学,2011,31(12):1977-1982.
[10]Bhatkhande DS,Pangarkar VG,Beenackers AA.Photocatalytic degradation for environmental applications:a review[J].J Chem Thermodyn,2002,77:102-116.
[11]Gaya UI,Abdullah AH.Heterogeneous photocatalytic degradation of organic contaminants over titanium dioxide:a review of fundamentals,progress and problems[J].J Photochem Photobiol C,2008,9:1-12.
[12]梁敏,莫创荣,张金莲,等.复合磁性光催化剂Co0.5Zn0.5Fe2O4/Bi2WO6的制备及其光催化性能[J].化工环保,2016,36(2):183-188.
[13]Li WT,Huang WZ,Zhou H,et al.Synthesis and photo activity enhancement of Ba doped Bi2WO6photocatalyst[J].Mater Res Bull,2015,64:432-437.
[14]冯长根,李鑫,曾庆轩,等.强碱阴离子交换纤维对活性染料的吸附性能研究[J].功能材料,2005,36(10):94-97.
[15]Wei XX,Chen JW,Xie Q,et al.Distinct photolytic mechanisms and products for different dissociation species of ciprofloxacin[J].Environ Sci Technol,2013,47:4284-4290.
[16]宋晨怡,胡霞林,尹大强.四环素在光催化剂Ti O2上的吸附研究[J].环境化学,2011,30(7):1291-1296.
[17]Jiao SJ,Zheng SR,Yin DQ,et al.Aqueous photolysis of tetracycline and toxicity of photolytic products to luminescent bacteria[J].Chemosphere,2008,73:377-382.
[18]冷文华,成少安,刘鸿,等.负载型二氧化钛光催化降解苯胺[J].环境科学学报,2000,20(4):499-503.
[19]周娅.制备Ti O2/Fe2O3/CNTs复合磁性光催化剂及光催化降解四环素类抗生素[D].西安:长安大学,2013.
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