可见光下氮掺杂罗丹明B分子印迹TiO_2的选择性光催化性能
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摘要
采用溶胶-凝胶法和分子印迹技术,以尿素为氮源、罗丹明B为模板分子制备了氮掺杂罗丹明B分子印迹TiO_2粉末(N-TiO_2-RhB),并对样品进行了XRD、UV-Vis DRS和BET表征。表征结果显示:氮掺杂和分子印迹一定程度改善了样品的孔隙结构和孔径分布,N-TiO_2-RhB的比表面积和孔体积分别为TiO_2的1.9倍和1.5倍;氮掺杂使TiO_2的光吸收带边发生红移,而分子印迹不能改变催化剂的光吸收带边。N-TiO_2-RhB具有最佳的可见光活性和选择性,对罗丹明B的降解率高达92.7%。对罗丹明B、罗丹明6G、甲基紫和甲基绿的降解过程均符合一级反应动力学方程。
Using urea as nitrogen source and Rhodamine B as template molecule,Rhodamine B molecular imprinting N-doped titanium dioxide(N-TiO_2-RhB) powder was prepared by sol-gel method and molecular imprinting technique,and characterized by XRD,UV-Vis DRS and BET. The results showed that:The pore structure and pore size distribution of the sample were improved by doping and molecular imprinting;The specific area and pore volume of N-TiO_2-RhB were 1.9 and 1.5 times as large as TiO_2;N-doping led to red shift of TiO_2 absorption edge,while molecular imprinting can't change the optical absorption edge of the catalyst. N-TiO_2-RhB had the best photocatalytic activity and selectivity under visible-light,the degradation rate of Rhodamine B was up to 92.7% by it. The degradation processes of Rhodamine B,Rhodamine 6G,methyl violet and methyl green all accorded with the first order reaction kinetics equation.
Using urea as nitrogen source and Rhodamine B as template molecule,Rhodamine B molecular imprinting N-doped titanium dioxide(N-TiO_2-RhB) powder was prepared by sol-gel method and molecular imprinting technique,and characterized by XRD,UV-Vis DRS and BET. The results showed that:The pore structure and pore size distribution of the sample were improved by doping and molecular imprinting;The specific area and pore volume of N-TiO_2-RhB were 1.9 and 1.5 times as large as TiO_2;N-doping led to red shift of TiO_2 absorption edge,while molecular imprinting can't change the optical absorption edge of the catalyst. N-TiO_2-RhB had the best photocatalytic activity and selectivity under visible-light,the degradation rate of Rhodamine B was up to 92.7% by it. The degradation processes of Rhodamine B,Rhodamine 6G,methyl violet and methyl green all accorded with the first order reaction kinetics equation.
引文
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[2]Zhang Zhonghai,Yu Yanjie,Wang Peng.Hierarchical top-porous/bottom-tubular Ti O2 nanostructures decorated with Pd nanoparticles for efficient photoelectrocatalytic decomposition of synergistic pollutants[J].ACS Appl Mater Interf,2012,4(2):990-996.
[3]康巧梅,洪臣熙.La2O3-Ti O2的制备及其光催化性能[J].化工环保,2015,35(4):432-437.
[4]Tian Fei,Wu Zhansheng,Yan Yujun,et al.Synthesis of visible-light-responsive Cu and N-codoped AC/Ti O2photocatalyst through microwave irradiation[J].Nanoscal Res Lett,2016,10(11):292-296.
[5]杜聪聪,李石,李萌,等.Mn-N/Ti O2光催化剂的制备及甲基橙的降解[J].化工环保,2015,35(6):625-629.
[6]艾翠玲,郭锐敏,邵享文.Cd S-Ti O2复合光催化剂可见光下降解黄连素[J].环境化学,2013,32(3):366-373.
[7]Pan Lun,Zou Jijun,Liu Xinyu,et al.Visible-light-induced photodegradation of rhodamine B over hierarchical Ti O2:Effects of storage period and water-mediated adsorption switch[J].Ind Eng Chem Res,2012,51(39):12782-12786.
[8]Manoj A L,Walid A D.Selective adsorption and photocatalysis of low-temperature base-modified anatase nanocrystals[J].RSC Adv,2012,2:447-452.
[9]Nakamura K J,Ide Y,Ogawa M.Molecular recognitive photocatalytic decomposition on mesoporous silica coated Ti O2 particle[J].Mater Lett,2011,65(1):24-26.
[10]罗利军,王娟,潘学军,等.二氧化钛选择性光催化降解有机污染物研究进展[J].化学通报,2013,76(4):332-337.
[11]Dovrat S,Yaron P.Preferential photodegradation of contaminants by molecular imprinting on titanium dioxide[J].Appl Catal B:Environ,2010,95:169-178.
[12]Shen Xiantao,Zhu Li,Hua liu,et al.Synthesis of molecular imprinted polymer coated photocatalysts with high selectivity[J].Chem Commun,2007(11):1163-1165.
[13]Qin Haoli,Gu Guobang,Liu Song.Preparation of nitrogen-doped titania using sol-gel technique and its photocatalytic activity[J].Mater Chem Phys,2008,112(2):346-352.
[14]秦好丽,安娅,古国榜.可见光下氮掺杂二氧化钛对有机污染物的降解动力学研究[J].生态环境学报,2010,19(3):513-517.
[15]索丹霞,刘桂超,彭婷婷,等.N掺杂锐钛矿结构Ti O2光催化性能研究[J].上海工程技术大学学报,2015,29(1):27-31.
[16]辛勤,罗孟飞.现代催化研究方法[M].北京:科学出版社,2008:17-22.
[17]曹雪萍,徐辉,李丹,等.HCl加入量对介孔N掺杂Ti O2材料结构及光催化性能的影响[J].南京工业大学学报:自然科学版,2012,34(4):39-42.
[18]Xu Pingping,Xu Wangzhen,Zhang Xiaojie,et al.Molecularly-imprinted material for dibenzothiophene recognition prepared by surface imprinting methods[J].Ads Sci Technol,2009,27(10):975-987.
[19]Asahi R,Morikawa T,Irie H,et al.Nitrogen-doped titanium as visible-light-sensitive photocatalyst:Designs,developments and prospects[J].Chem Rev,2014,114(19):9824-9852.
[20]王思旋.二氧化钛分子印迹光催化剂的制备和选择性光催化作用[D].武汉:华中师范大学,2013.
[21]魏声培,安娅,秦好丽.水杨酸分子印迹掺氮Ti O2粉末的制备及其在可见光下的选择性光催化研究[J].华南农业大学学报,2016,4(2):102-110.
[22]苗智颖.溶胶-凝胶分子印迹聚合物和金属纳米材料的制备及其在传感器中的应用研究[D].天津:南开大学,2014.