金属负载ZSM-5分子筛催化臭氧化苯酚废水
|
摘要
以ZSM-5分子筛为载体,铈(Ce)、锰(Mn)、镍(Ni)、铜(Cu)为活性组分,制备金属负载型催化剂,催化臭氧化处理苯酚废水。采用浸渍法制备催化剂,并对其进行表征。考察了活性组分、臭氧投加量,催化剂质量浓度、pH等因素对苯酚废水的处理效果。结果表明,在废水pH=7、催化剂质量浓度为1.00 g/L、臭氧投加量为44.0 mg/min、反应时间为60 min的条件下,Ce-ZSM-5的催化效果最好,COD去除率为85.74%。加入Ce-ZSM-5后,可节约大约80%的臭氧量。催化剂在使用7次后,虽然降解效果有小幅度下降,但COD去除效率仍然保持在70%,证明其稳定性良好。
ZSM-5 molecular sieve was used as carrier, cerium(Ce), manganese(Mn), nickel(Ni) and copper(Cu) were used as active components to prepare metal-supported catalyst to catalyze ozonation treatment of phenol wastewater. The catalyst was prepared by impregnation method and characterized. The effects of active components, ozone dosage, catalyst concentration and pH on the treatment of phenol wastewater were investigated. The results showed that Ce-ZSM-5 had the best catalytic effect and COD removal rate under the conditions of pH=7, catalyst concentration of 1.00 g/L, ozone dosage of 44.0 mg/min and reaction time of 60 min. It is 85.74%. When Ce-ZSM-5 is added, about 80% of the ozone can be saved. It shows good stability which the COD removal ratio reached about 70% after the catalyst repeatedly used for 7 times.
ZSM-5 molecular sieve was used as carrier, cerium(Ce), manganese(Mn), nickel(Ni) and copper(Cu) were used as active components to prepare metal-supported catalyst to catalyze ozonation treatment of phenol wastewater. The catalyst was prepared by impregnation method and characterized. The effects of active components, ozone dosage, catalyst concentration and pH on the treatment of phenol wastewater were investigated. The results showed that Ce-ZSM-5 had the best catalytic effect and COD removal rate under the conditions of pH=7, catalyst concentration of 1.00 g/L, ozone dosage of 44.0 mg/min and reaction time of 60 min. It is 85.74%. When Ce-ZSM-5 is added, about 80% of the ozone can be saved. It shows good stability which the COD removal ratio reached about 70% after the catalyst repeatedly used for 7 times.
引文
[1]马健伟,任淑鹏,初阳,等.高级氧化技术处理含酚废水的研究进展[J].当代化工,2018,47(6):1276-1278.
[2]黄太彪,李刘柱,高嵩,等.含酚废水处理研究进展[J].工业用水与废水,2016,47(4):12-15.
[3]王郑,程星星,黄雷,等.催化臭氧化技术在水处理中的应用研究进展[J].应用化工,2017,46(6):1215-1217.
[4]朱秋实,陈进富,姜海洋,等.臭氧催化氧化机理及其技术研究进展[J].化工进展,2014,33(4):1010-1034.
[5] Fajardo A S,Martins R C,Quintaferreira R M. Treatment of a simulated phenolic effluent by heterogeneous catalytic ozonation using Pt/Al2O3[J]. Environmental Technology,2013,34(3):301-311.
[6] Li X,Chen W,Ma L,et al. Industrial wastewater advanced treatment via catalytic ozonation with an Fe-based catalyst[J].Chemosphere,2018,195:336-343.
[7] Dai Q,Wang J,Chen J,et al. Ozonation catalyzed by cerium supported on activated carbon for the degradation of typical pharmaceutical wastewater[J]. Separation and Purification Technology,2014,127:112-120.
[8] Huang Y,Sun Y,Xu Z,et al. Removal of aqueous oxalic acid by heterogeneous catalytic ozonation with MnOx/sewage sludge-derived activated carbon as catalysts[J]. Science of the Total Environment,2017,575:50-57.
[9]刘咏,李妍,赵仕林,等.锰-稀土/Y分子筛复合电催化处理含酚模拟废水[J].中国环境科学,2011,31(5):740-747.
[10] Wang L,Cai H,Li S,et al. Ultra-deep removal of thiophene compounds in diesel oil over catalyst TiO2/Ni-ZSM-5assisted by ultraviolet irradiating[J]. Fuel,2013,105(2):752-756.
[11] Amin N A S,Akhtar J,Rai H K. Screening of combined zeolite-ozone system for phenol and COD removal[J]. Chemical Engineering Journal,2010,158(3):520-527.
[12] Yang P,Xue X,Meng Z,et al. Enhanced catalytic activity and stability of Ce doping on Cr supported HZSM-5 catalysts for deep oxidation of chlorinated volatile organic compounds[J]. Chemical Engineering Journal,2013,234(12):203-210.
[13] Lan B Y,Huang R H,Li L S,et al. Catalytic ozonation of p-chlorobenzoic acid in aqueous solutionusing Fe-MCM-41 as catalyst[J].Chemical Engineering Journal,2013,219:346-354.
[14] Zhao L,Ma J,Liu Z Q,et al. Catalytic ozonation for the degradation of nitrobenzene in aqueous solution by ceramic honeycomb-supported manganese[J].Applied Catalysis B:Environmental,2008,83:256-264.
[15]杨郭,曾凡炎,王淑静. CeO-活性炭催化臭氧化降解水中草酸的研究[J].工业水处理,2016,36(8):55-59.
[16]王群.氧化铈催化臭氧氧化水中有机物及控制溴酸盐研究[D].哈尔滨:哈尔滨工业大学,2010.
[17]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.
[18]姜传佳.活性炭载锰-钯催化剂的制备及其催化分解臭氧性能研究[D].北京:清华大学,2011.
[19] Shukla P R,Wang S,Sun H,et al. Activated carbon supported cobalt catalysts for advanced oxidation of organic contaminants in aqueous solution[J].Applied Catalysis B:Environmental,2010,100(3/4):529-534.
[2]黄太彪,李刘柱,高嵩,等.含酚废水处理研究进展[J].工业用水与废水,2016,47(4):12-15.
[3]王郑,程星星,黄雷,等.催化臭氧化技术在水处理中的应用研究进展[J].应用化工,2017,46(6):1215-1217.
[4]朱秋实,陈进富,姜海洋,等.臭氧催化氧化机理及其技术研究进展[J].化工进展,2014,33(4):1010-1034.
[5] Fajardo A S,Martins R C,Quintaferreira R M. Treatment of a simulated phenolic effluent by heterogeneous catalytic ozonation using Pt/Al2O3[J]. Environmental Technology,2013,34(3):301-311.
[6] Li X,Chen W,Ma L,et al. Industrial wastewater advanced treatment via catalytic ozonation with an Fe-based catalyst[J].Chemosphere,2018,195:336-343.
[7] Dai Q,Wang J,Chen J,et al. Ozonation catalyzed by cerium supported on activated carbon for the degradation of typical pharmaceutical wastewater[J]. Separation and Purification Technology,2014,127:112-120.
[8] Huang Y,Sun Y,Xu Z,et al. Removal of aqueous oxalic acid by heterogeneous catalytic ozonation with MnOx/sewage sludge-derived activated carbon as catalysts[J]. Science of the Total Environment,2017,575:50-57.
[9]刘咏,李妍,赵仕林,等.锰-稀土/Y分子筛复合电催化处理含酚模拟废水[J].中国环境科学,2011,31(5):740-747.
[10] Wang L,Cai H,Li S,et al. Ultra-deep removal of thiophene compounds in diesel oil over catalyst TiO2/Ni-ZSM-5assisted by ultraviolet irradiating[J]. Fuel,2013,105(2):752-756.
[11] Amin N A S,Akhtar J,Rai H K. Screening of combined zeolite-ozone system for phenol and COD removal[J]. Chemical Engineering Journal,2010,158(3):520-527.
[12] Yang P,Xue X,Meng Z,et al. Enhanced catalytic activity and stability of Ce doping on Cr supported HZSM-5 catalysts for deep oxidation of chlorinated volatile organic compounds[J]. Chemical Engineering Journal,2013,234(12):203-210.
[13] Lan B Y,Huang R H,Li L S,et al. Catalytic ozonation of p-chlorobenzoic acid in aqueous solutionusing Fe-MCM-41 as catalyst[J].Chemical Engineering Journal,2013,219:346-354.
[14] Zhao L,Ma J,Liu Z Q,et al. Catalytic ozonation for the degradation of nitrobenzene in aqueous solution by ceramic honeycomb-supported manganese[J].Applied Catalysis B:Environmental,2008,83:256-264.
[15]杨郭,曾凡炎,王淑静. CeO-活性炭催化臭氧化降解水中草酸的研究[J].工业水处理,2016,36(8):55-59.
[16]王群.氧化铈催化臭氧氧化水中有机物及控制溴酸盐研究[D].哈尔滨:哈尔滨工业大学,2010.
[17]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.
[18]姜传佳.活性炭载锰-钯催化剂的制备及其催化分解臭氧性能研究[D].北京:清华大学,2011.
[19] Shukla P R,Wang S,Sun H,et al. Activated carbon supported cobalt catalysts for advanced oxidation of organic contaminants in aqueous solution[J].Applied Catalysis B:Environmental,2010,100(3/4):529-534.