通过水热法合成纯硅介孔分子筛SBA-15,并采用等体积浸渍法制备Ce负载SBA-15分子筛催化剂(Ce/SBA-15),将其应用于催化臭氧氧化环丙沙星(CIP).小角X射线衍射(XRD)、透射电镜(TEM)表征结果表明,Ce/SBA-15保持了纯硅SBA-15有序的介孔结构.Ce/SBA-15催化臭氧氧化环丙沙星(CIP)结果显示,催化剂有良好的活性,对环丙沙星的矿化率为63.3％,比单独臭氧氧化高出22.9％;随着铈负载量增加,催化剂活性呈现先增大后减小趋势,负载量为2％时催化效果最佳;TOC去除率随着反应温度增加而提高;溶液初始pH对反应有显著的影响,pH=5.01时TOC去除率最大.以水杨酸作为羟基自由基(·OH)捕获剂,用比色法测定·OH产量为0.0072 mmol· L-1.溶液中投加1 mmol· L-1磷酸根时,催化臭氧氧化中TOC去除率降低了25.8％,催化效果受到明显抑制,表明·OH的生成发生在Ce/SBA-15表面.
Cerium-loaded SBA-15 (Ce/SBA-15) was synthesized successfully by a hydrothermal method and was used as a catalyst for the ozonation of ciprofloxacin (CIP) in aqueous solution.The catalyst was characterized by low angle X-ray diffraction (XRD) and transmission electron microscopy (TEM).Characterizations results suggested that the prepared samples retained a highly regulated mesopores of hexagonal structure.The catalytic ozonation reaction results showed that Ce/SBA-15 had good catalytic activity,through which TOC removal rate of CIP reached 63.3％,22.9％ higher than ozonation reaction alone.And the catalytic activity of the samples increased with metal loading amount from 0.5％ to 2％.However,it showed a decreased trend as the metal loading amount further increased.What's more,TOC removal increased with temperature.The initial pH of the solution also had a significant effect on the reaction,and the removal rate of TOC reached the highest at pH 5.01.Salicylic acid was employed as · OH scavenger to qualify · OH by using UV-Vis Spectroscopy.When 1 mmol ·L-1 phosphate was added into the reaction solution,TOC removal was inhibited by 25.8％.The result indicted that hydroxyl radical (·OH) was be generated on the surface of Ce/SBA-15.
参考文献
| [1] | Xin Yang;Riley C. Flowers;Howard S. Weinberg;Philip C. Singer.Occurrence and removal of Pharmaceuticals and personal care products (PPCPs) in an advanced wastewater reclamation plant[J].Water research: A journal of the international water association,201116(16):5218-5228. |
| [2] | Ayrton F.Martins;Tibirica G Vasconcelos;Danielle M.Henriques.Concentration of Ciprofloxacin in Brazilian Hospital Effluent and Preliminary Risk Assessment:A Case Study[J].Clean - Soil, Air, Water: A Journal of Sustainability and Environmental Safety,20083(3):264-269. |
| [3] | 邓曹林;王京刚;王颖;方嘉声.石墨烯改性Al-MCM-41介孔分子筛负载铁芬顿催化剂降解苯酚?[J].环境化学,2015(6):1185-1192. |
| [4] | Lei Zhao;Jun Ma;Zhizhong Sun.Mechanism of heterogeneous catalytic ozonation of nitrobenzene in aqueous solution with modified ceramic honeycomb[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,20093/4(3/4):326-334. |
| [5] | Jun Ma;Minghao Sui;Tao Zhang;Chunyu Guan.Effect of pH on MnO_x/GAC catalyzed ozonation for degradation of nitrobenzene[J].Water research: A journal of the international water association,20055(5):779-786. |
| [6] | Tanya Tsoncheva;Mikael Jarn;Daniela Paneva.Copper and chromium oxide nanocomposites supported on SBA-15 silica as catalysts for ethylacetate combustion: Effect of mesoporous structure and metal oxide composition[J].Microporous and mesoporous materials: The offical journal of the International Zeolite Association,20111/3(1/3):56-64. |
| [7] | Roberto Rosal;Maria S. Gonzalo;Antonio Rodriguez.Catalytic ozonation of atrazine and linuron on MnO_x/Al2O3 and MnO_x/SBA-15 in a fixed bed reactor[J].Chemical engineering journal,20103(3):806-812. |
| [8] | A.L Petre;J.B. Carbajo;R. Rosal.CuO/SBA-15 catalyst for the catalytic ozonation of mesoxalic and oxalic acids. Water matrix effects[J].Chemical engineering journal,2013:164-173. |
| [9] | P.C.C.Faria;J.J.M.Orfao;M.F.R.Pereira.A novel ceria-activated carbon composite for the catalytic ozonation of carboxylic acids[J].Catalysis Communications,200811/12(11/12):2121-2126. |
| [10] | Rui C. Martins;Rosa M. Quinta-Ferreira.Catalytic ozonation of phenolic acids over a Mn-Ce-O catalyst[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,20091/2(1/2):268-277. |
| [11] | Urs von Gunten.Ozonation of drinking water: Part Ⅰ. Oxidation kinetics and product formation[J].Water research: A journal of the international water association,20037(7):1443-1467. |
| [12] | Laisheng Li;Weiying Ye;Qiuyun Zhang;Fengqiang Sun;Ping Lu;Xukai Li.Catalytic ozonation of dimethyl phthalate over cerium supported on activated carbon[J].Journal of hazardous materials,20091(1):13-21. |
| [13] | Tao Zhang;Chunjuan Li;Jun Ma.Surface hydroxyl groups of synthetic α-FeOOH in promoting ~·OH generation from aqueous ozone: Property and activity relationship[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,20081/2(1/2):131-137. |
| [14] | LEI ZHAO;ZHIZHONG SUN;JUN MA.Novel Relationship between Hydroxyl Radical Initiation and Surface Group of Ceramic Honeycomb Supported Metals for the Catalytic Ozonation of Nitrobenzene in Aqueous Solution[J].Environmental Science & Technology: ES&T,200911(11):4157-4163. |
| [15] | Hui Zhao;Yuming Dong;Guangli Wang.Novel magnetically separable nanomaterials for heterogeneous catalytic ozonation of phenol pollutant: NiFe2O4 and their performances[J].Chemical engineering journal,2013:295-302. |
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