CuO-Y_2O_3/TS-1催化臭氧降解对苯二甲酸的机理
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摘要
针对对苯二甲酸(TA)水污染问题,通过浸渍法制备CuO-Y_2O_3/TS-1催化剂,利用XRD、SEM、FT-IR、XRF等手段表征催化剂结构、形貌及骨架结构;构建非均相体系催化臭氧氧化降解对苯二甲酸(TA),考察催化剂的催化性能。结果表明:当Cu(NO_3)_2·3H_2O和Y(NO_3)_3·6H_2O浸渍液浓度均为0.5 mg·L~(-1)、臭氧通入量为6.3mg·min~(-1)、催化剂投加量为1.0 g和pH=9.0时,反应30 min后,TA降解率高达99.8%。经5次循环后,TA降解率仍稳定在98.2%。进一步研究表明,CuO-Y_2O_3/TS-1催化臭氧降解TA实验符合一级反应动力学方程。
Aiming at the water pollution problem of terephthalic acid(TA), a kind of CuO-Y_2O_3/TS-1 catalyst was prepared by impregnation method. Its structure, morphology and framework structure were characterized by XRD, SEM, FT-IR and XRF. Then a heterogeneous system was built to catalyze ozone oxidation and degrade terephthalic(TA) acid, to investigate the catalytic performance of the catalyst. The results showed that the degree of TA degradation was as high as 99.8% at 30 min reaction when the concentrations of Cu(NO_3)_2·3H_2O and Y(NO_3)_3·6H_2O impregnating solution were both 0.5 mol·L~(-1), the ozone flux was 6.3 mg·min~(-1), the catalyst dosage was 1.0 g, and pH was 9.0. After 5 cycles of reusing catalyst, TA degradation rate was still remained at98.2%. Furthermore, ozone treatment of TA with CuO-Y_2O_3/TS-1 catalyst accorded with the first-order reaction kinetics equation.
Aiming at the water pollution problem of terephthalic acid(TA), a kind of CuO-Y_2O_3/TS-1 catalyst was prepared by impregnation method. Its structure, morphology and framework structure were characterized by XRD, SEM, FT-IR and XRF. Then a heterogeneous system was built to catalyze ozone oxidation and degrade terephthalic(TA) acid, to investigate the catalytic performance of the catalyst. The results showed that the degree of TA degradation was as high as 99.8% at 30 min reaction when the concentrations of Cu(NO_3)_2·3H_2O and Y(NO_3)_3·6H_2O impregnating solution were both 0.5 mol·L~(-1), the ozone flux was 6.3 mg·min~(-1), the catalyst dosage was 1.0 g, and pH was 9.0. After 5 cycles of reusing catalyst, TA degradation rate was still remained at98.2%. Furthermore, ozone treatment of TA with CuO-Y_2O_3/TS-1 catalyst accorded with the first-order reaction kinetics equation.
引文
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[29]姚宁波,李学艳,李青松,等.超声联合过硫酸钠去除水中三氯生[J].环境工程学报,2017,11(6):3439-3445.
[30]NIU J R,QIAN H L,LIU J,et al.Process and mechanism of toluene oxidation using Cu1-y Mn2Cey Ox/sepiolite prepared by the co-precipitation method[J].Journal of Hazardous Materials,2018,357:332-340.
[31]王兵,周鋆,任宏洋,等.MgO催化臭氧氧化降解苯酚机理研究[J].环境科学学报,2016,36(11):4009-4016.
[32]李文姝.过渡金属催化臭氧氧化的方法[J].居舍,2018(1):171.
[33]董清.尖晶石催化臭氧去除水中邻苯二甲酸二丁酯的实验研究[D].哈尔滨:哈尔滨工程大学,2013.
[2]张丽君,丁大喜,钱彦虎,等.精对苯二甲酸产品和方法标准的研究进展[J].化工进展,2018,37(6):2445-2433.
[3]李玥,胡奇,高大文.温度对一体式厌氧流化床膜生物反应器运行效能及微生物群落结构的影响[J].环境科学,2018,39(4):1731-1738.
[4]沈万峰.有机废水的好氧生物处理技术进展研究[J].城市道桥与防洪,2017(9):105-106.
[5]杨忠林,钟中,韩萍芳,等.厌氧折流板反应器处理PTA废水及其相分离特性[J].生物加工过程,2012,10(6):60-64.
[6]马凯丽,李相昆,张杰.温度两级厌氧反应系统对精对苯二甲酸废水的处理[J].环境工程学报,2018,12(2):482-487.
[7]王旺阳,刘聪,袁珮.吸附法去除环境中多环芳烃的研究进展[J].化工进展,2017,36(1):355-363.
[8]张家发,白玲,范浩军,等.超细纤维合成革碱减量废水中对苯二甲酸的分离提纯[J].中国皮革,2016,45(9):29-34.
[9]李杨,朱夔,李晶蕊,等.采用臭氧催化氧化法深度处理石化污水[J].石化技术与应用,2016,34(5):410-413.
[10]牛建瑞,李文亚,李宗泽,等.Cu-Mn/Fe3O4@SiO2@KCC纳米催化剂制备及其催化臭氧化降解对苯二甲酸性能[J].科学技术与工程,2018,18(6):354-360.
[11]臧兴杰.臭氧及同相催化臭氧化降解有机物的动力学研究[D].杭州:浙江工业大学,2009.
[12]刘梦,戚秀芝,张科亭,等.非均相催化臭氧氧化法深度处理染料废水[J].环境污染与防治,2018,40(5):572-576.
[13]孙逊,杨红红.催化臭氧氧化工艺深度处理市政污水厂生化出水[J].中国给水排水,2018,34(1):74-81.
[14]郭瑶,梁娟,闫浩,等.不同载体对催化臭氧氧化降解甲基橙的影响[J].环境工程,2018,36(4):57-61.
[15]许珊珊,林存旺,丁亚磊,等.MgO/活性炭催化臭氧化降解有机物的作用机制[J].环境科学,2018,39(2):838-843.
[16]LOPES R J G,PERDIGOTO M L N,FERREIRAR M Q.Tailored investigation and characterization of heterogeneous(Mn,Cu)/TiO2 catalysts embedded within a ceria-based framework for the wet peroxide oxidation of hazardous pollutants[J].Applied Catalysis B:Environmental,2012,117-118(3):292-301.
[17]王宇轩,王应军,方明珠.活性炭负载CuO催化过硫酸盐去除活性艳红X-3B染料[J].环境工程学报,2016,10(1):230-236.
[18]张坤,崔玉民,张文保,等.Y2O3/WO3光催化降解污水处理厂综合废水的研究[J].稀土,2011,32(1):42-45.
[19]陈坦,陈皓,傅杰,等.CuO/HZSM-5催化溴甲烷芳构化制备芳烃[J].化工学报,2017,68(6):2344-2351.
[20]SASIDHARAN M,BHAUMIK A.Catalytic oxidation of cyclic ethers to lactones over various titanosilicates[J].Journal of Molecular Catalysis A:Chemical,2011,338(1):105-110.
[21]刘艳芳,张智理,许欢欢,等.连续流催化臭氧氧化污水处理厂尾水效能研究[J].给水排水,2017,43(4):29-34.
[22]王清.不同类型沸石分子筛的OH振动红外光谱研究[D].大连:大连理工大学,2011.
[23]朱荣秀.胺类双官能团催化剂催化作用的理论研究[D].济南:山东大学,2007.
[24]CHEN X,KUO D H,SARAGIH A D,et al.The effect of the Cu+/Cu2+ratio on the redox reactions by nanoflower CuNiOScatalysts[J].Chemical Engineering Science,2018,194:105-115.
[25]刘莹,何宏平,吴德礼,等.非均相催化臭氧氧化反应机制[J].化学进展,2016,28(7):1112-1120.
[26]李磊,倪晶晶.臭氧氧化降解对苯二甲酸的试验研究[J].天津化工,2008,22(5):51-54.
[27]BING J,HU C,NIE Y,et al.Mechanism of catalytic ozonation in Fe2O3/Al2O3@SBA-15 aqueous suspension for destruction of ibuprofen[J].Environmental Science&Technology,2015,49(3):1690-1697.
[28]IKHLAQ A,BROWN D R,KASPRZYK H B.Catalytic ozonation for the removal of organic contaminants in water on ZSM-5zeolites[J].Applied Catalysis B:Environmental,2014,154-155:110-122.
[29]姚宁波,李学艳,李青松,等.超声联合过硫酸钠去除水中三氯生[J].环境工程学报,2017,11(6):3439-3445.
[30]NIU J R,QIAN H L,LIU J,et al.Process and mechanism of toluene oxidation using Cu1-y Mn2Cey Ox/sepiolite prepared by the co-precipitation method[J].Journal of Hazardous Materials,2018,357:332-340.
[31]王兵,周鋆,任宏洋,等.MgO催化臭氧氧化降解苯酚机理研究[J].环境科学学报,2016,36(11):4009-4016.
[32]李文姝.过渡金属催化臭氧氧化的方法[J].居舍,2018(1):171.
[33]董清.尖晶石催化臭氧去除水中邻苯二甲酸二丁酯的实验研究[D].哈尔滨:哈尔滨工程大学,2013.
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