CN106345504A - 微波强化活性炭负载TiO2光催化剂制备及降解方法 - Google Patents
微波强化活性炭负载TiO2光催化剂制备及降解方法 Download PDFInfo
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Abstract
本发明属于新材料技术领域,涉及一种催化剂,特别是一种用于去除萘的微波强化活性炭负载TiO2光催化剂制备及降解方法。该方法以钛酸丁酯为钛源,硝酸铈或硝酸镧、尿素、磷酸为掺杂剂,煤基活性炭为载体,通过微波辐射,制备微波强化活性炭负载TiO2光催化剂。该方法采用微波法制备,工艺简单,原料廉价。即缩短了制备时间,又节省了能源,从而降低制备光催化剂的成本,光催化剂为纳米颗粒状,易于回收及分离,在可见光下对萘的催化降解有显著的效果,降解率可达99.28%,并且不产生二次污染,具有良好的经济效益和环境效益。
Description
技术领域
本发明属于新材料技术领域,涉及一种催化剂,特别是一种用于去除萘的微波强化活性炭负载TiO2光催化剂制备及降解方法。
背景技术
萘是由两个苯环直接相连组成的一种有机化合物,分子式C10H8,白色,易挥发并有特殊气味的晶体。是一类很强致癌性、在环境中具有持久性、具有生物富集性、难降解性、结构稳定性,能够随着大气和水等环境介质进行长距离迁移的化合物质,对人体健康和生态环境存在很大的危害,因此,开发高效的方法以去除环境中的萘具有重要的现实意义。
目前,生物处理、反渗透、萃取以及吸附法被广泛用于去除萘,然而这些方法所需时间长,处理工艺复杂,并产生二次污染。光催化降解技术由于其便宜,易操作的特点,成为去除萘的可选技术,其中TiO2光催化剂以其无毒无害、化学稳定性、高活性等特性被广泛应用。Dariani等[Photocatalytic reaction and degradation of methylene blue onTiO2nano-sized particles,2016]用TiO2纳米颗粒降解亚甲基蓝,结果表明在紫外灯下1h,10nm的TiO2对亚甲基蓝的降解率达到90%以上,2h可以降解完全。Juang等[Comparativestudy on photocatalytic degradation of methomyl and parathion over UV-irradiated TiO2particles in aqueous solutions]报道了在紫外灯下TiO2对灭多威和对硫磷的降解,结果表明灭多威的降解速率高于对硫磷,这是因为对硫磷的分子结构更复杂。然而,TiO2光催化剂存在禁带宽度大、可见光利用率低、回收困难等缺点,大大限制了其在实际中的应用。近年来有研究者,提出针对TiO2光催化材料的改性以改善对可见光的吸收,提高光量子产率及光催化性能。此外,孔材料负载TiO2能提高光催化剂的吸附能力并有利于回收利用。其中,活性炭因其较大的比表面积和孔体积成为有效的TiO2载体。Liu等[Controlled synthesis of ordered mesoporous TiO2-supported on activatedcarbon and pore-pore synergistic photocatalytic performance,2015]制备了介孔活性炭负载TiO2,结果表明,与单独的TiO2相比活性炭负载TiO2呈现更高的光催化活性。Ragupathy等[Synthesis and characterization of TiO2loaded cashew nut shellactivated carbon and photocatalytic activity on BG and MB dyes under sunlightradiation,2015]报道了腰果壳负载TiO2的合成和特征,结果表明,在太阳光下光催化剂对亮绿和亚甲基蓝的降解率分别可达到99.75%和96.35%。
近些年来,微波技术成为制备光催化剂一种有效的加热技术,中国专利[申请号:201410264807]利用微波加热合成了活性炭。肖等[申请号:201410142529]研究表明微波辅助加热能够缩短加热的时间,显著提高光催化剂的光催化活性。与传统加热方式比较,微波技术能够极大地提高一些化学反应速率、减少反应时间、简化后处理程序。
发明内容
为了解决上述问题,本发明的目的在于提供一种在可见光下对萘表现出降解效率高,速率快,所需时间短等优点,具有良好的经济和环境效益的微波强化活性炭负载TiO2光催化剂制备及降解方法。
本发明的技术方案是:微波强化活性炭负载TiO2光催化剂的制备方法,该方法包括如下步骤:
步骤1:钛溶胶制备:
1.1)量取一定量的无水乙醇于锥形瓶中,加入钛酸丁酯,持续搅拌35-45min,得溶液A,备用,其中,所述无水乙醇与太酸钛酸丁酯的体积比为1.1-1.2:1;
1.2)量取一定量的无水乙醇于锥形瓶中,加入蒸馏水、冰乙酸、尿素、硝酸铈和磷酸,得溶液B;
1.3)在不断搅拌下将溶液B缓慢滴入溶液A中,室温条件下,继续搅拌35-45min得到浅黄色均匀透明的钛溶胶,其中,溶液B与溶液A质量比为1:1;
步骤2:微波强化制备复合光催化剂:
将预处理后的煤基活性炭浸于步骤1.3制备得到的钛溶胶中密封静置22-26h成半固化状态后,放入烘箱内设置温度100-110℃,烘干12-18小时,将烘干的复合光催化剂置于微波功率650-700W、辐射12-15min,即得到微波强化活性炭负载共掺杂TiO2光催化剂。
进一步,所述步骤1.2中,所述硝酸铈还可以为硝酸镧。
进一步,所述步骤1.2中的无水乙醇、蒸馏水、冰乙酸、尿素、磷酸和硝酸铈或硝酸镧之间的质量比23.7-27.65:6.5-7.0:10.0-14.0:1.0-2.0:0.22-0.72:0.3-1.5。
进一步,所述步骤2中,所述煤基活性炭与钛溶胶的固液比为0.8-0.1:8-10。
进一步,所述波强化活性炭负载共掺杂TiO2光催化剂的平均粒径为9.1-13.5nm,比表面积为500.04-800.49m2/g,总孔容为0.25-0.71cm3/g。
本发明的另一目的提供一种上述方法制备得到的微波强化活性炭负载共掺杂TiO2光催化剂用于降解萘的方法,具体包括以下步骤:
步骤1:先将光催化降解反应在光反应器中进行,为排除外界光源干扰,反应在暗箱中进行,反应器中心置以450-500W氙灯;
步骤2:将50mL浓度为30mg/L的萘溶液加入石英反应器中,并加入0.02g催化剂样品,避光磁力搅拌60min,充分混合使催化剂达到吸附-脱附平衡。打开光源,光稳定5-10min,开始计光照反应时间,光照30-180min取样,样品在4000-5000r/min下离心15-20min,取上清液测定样品在波长为218nm处的吸光度值,通过下式即可计算出萘的降解率:
其中:Co为初始浓度,Ct为一定光照时间后萘的浓度。
在可见光下对萘降解率达到90.06%-99.28%,重复使用8-10次,对萘的降解率依然达到90%以上。
本发明的优点为:
1.本发明光催化剂采用微波法制备,工艺简单,原料廉价。即缩短了制备时间,又节省了能源,从而降低制备光催化剂的成本,是一种经济高效的制备方法。
2.本发明所得到的光催化剂为纳米颗粒状,易于回收及分离,在可见光下对萘的催化降解有很好的效果。
本发明方法制备的Ce-N-P-TiO2/AC光催化剂具有适合催化降解萘分子表面结构、粒径及比表面积,对于在可见光下去除萘具有显著的效果,并且不产生二次污染,具有良好的经济效益和环境效益。
具体实施方式
下面结合具体实施例对本发明的技术方案做进一步说明。
实施例1:
1.溶胶制备
(1)量取30mL无水乙醇于锥形瓶中,加入25mL钛酸丁酯,得溶液A。不断搅拌40min;
(2)不断搅拌下,向30mL无水乙醇中加入6.5mL蒸馏水,11.0mL的冰乙酸,1.71g的尿素,0.94g的硝酸铈,0.9mL浓度为7.35mol/L的磷酸,得溶液B;
(3)在不断搅拌下将溶液B缓慢的滴入溶液A中,继续搅拌40min得到浅黄色均匀透明的溶胶,即得Ce、N、P共掺杂TiO2溶胶。
注:在溶胶制备过程中,除加药品外,过程均密封。
2.微波辅助制备复合光催化剂
将预处理后的煤基活性炭10g浸于钛溶胶中100g密封静置24h成半固化状态后烘干(放入烘箱设置温度100℃,15小时)。将烘干的复合光催化剂置于微波功率650W辐射13min。
3.复合光催化剂对萘降解的具体步骤:
光催化降解反应在光反应器中进行,为排除外界光源干扰,反应在暗箱中进行。反应器中心置以500W氙灯,将50mL浓度为30mg/L的萘溶液加入石英反应器中,并加入0.02g催化剂样品,避光磁力搅拌60min,充分混合使催化剂达到吸附-脱附平衡。打开光源,光稳定5min,开始计光照反应时间,光照一定时间取样,样品在5000r/min下离心15min,取上清液测定样品在波长为218nm处的吸光度值。
所得的Ce-N-P-TiO2/AC光催化剂平均粒径为10.8nm,比表面积为690.69m2/g,总孔容为0.64cm3/g,在可见光下对萘降解率可达98.5%,重复使用8次,对萘的降解率依然达到95.6%。
实施例2:
1.Ce、N、P共掺杂TiO2溶胶制备
(1)量取35mL无水乙醇于锥形瓶中,加入30mL钛酸丁酯,得溶液A。不断搅拌40min;
(2)不断搅拌下,向35mL无水乙醇中加入7.0mL蒸馏水,14.0mL的冰乙酸,1.0g的尿素,0.3g的硝酸铈,0.32mL浓度为7.35mol/L的磷酸,得溶液B;
(3)在不断搅拌下将溶液B缓慢的滴入溶液A中,继续搅拌40min得到浅黄色均匀透明的溶胶,即得Ce、N、P共掺杂TiO2溶胶。
注:在溶胶制备过程中,除加药品外,过程均密封。
2.微波辅助制备复合光催化剂
将预处理后的煤基活性炭10g浸于钛溶胶100g中密封静置22h成半固化状态后烘干(放入烘箱设置温度105℃,12小时)。将烘干的复合光催化剂置于微波功率680W辐射15min。
3.复合光催化剂对萘降解的具体步骤:
光催化降解反应在光反应器中进行,为排除外界光源干扰,反应在暗箱中进行。反应器中心置以500W氙灯,将50mL浓度为30mg/L的萘溶液加入石英反应器中,并加入0.02g催化剂样品,避光磁力搅拌60min,充分混合使催化剂达到吸附-脱附平衡。打开光源,光稳定5min,开始计光照反应时间,光照一定时间取样,样品在5000r/min下离心15min,取上清液测定样品在波长为218nm处的吸光度值。
所得的Ce-N-P-TiO2/AC光催化剂平均粒径为11.3nm,比表面积为584.69m2/g,总孔容为0.42cm3/g,在可见光下对萘降解率可达95.5%,重复使用8次,对萘的降解率依然达到93.0%。
实施例3:
1.Ce、N、P共掺杂TiO2溶胶制备
(1)量取33mL无水乙醇于锥形瓶中,加入28mL钛酸丁酯,得溶液A。不断搅拌40min;
(2)不断搅拌下,向33mL无水乙醇中加入6.8mL蒸馏水,12.5mL的冰乙酸,2.0g的尿素,1.5g的硝酸铈,0.6mL浓度为7.35mol/L的磷酸,得溶液B;
(3)在不断搅拌下将溶液B缓慢的滴入溶液A中,继续搅拌40min得到浅黄色均匀透明的溶胶,即得Ce、N、P共掺杂TiO2溶胶。
注:在溶胶制备过程中,除加药品外,过程均密封。
2.微波辅助制备复合光催化剂
将预处理后的煤基活性炭10g浸于钛溶胶80g中密封静置24h成半固化状态后烘干(放入烘箱设置温度110℃左右,18小时)。将烘干的复合光催化剂置于微波功率700W辐射12min。
3.复合光催化剂对萘降解的具体步骤:
光催化降解反应在光反应器中进行,为排除外界光源干扰,反应在暗箱中进行。反应器中心置以500W氙灯,将50mL浓度为30mg/L的萘溶液加入石英反应器中,并加入0.02g催化剂样品,避光磁力搅拌60min,充分混合使催化剂达到吸附-脱附平衡。打开光源,光稳定5min,开始计光照反应时间,光照一定时间取样,样品在5000r/min下离心15min,取上清液测定样品在波长为218nm处的吸光度值。
所得的Ce-N-P-TiO2/AC光催化剂平均粒径为12.9nm,比表面积为525.69m2/g,总孔容为0.28cm3/g,在可见光下对萘降解率可达94.5%,重复使用8次,对萘的降解率依然达到91.5%。
实施例4:
(1)量取33mL无水乙醇于锥形瓶中,加入28mL钛酸丁酯,得溶液A。不断搅拌40min;
(2)不断搅拌下,向33mL无水乙醇中加入6.6mL蒸馏水,13.0mL的冰乙酸,1.5g的尿素,0.5g的硝酸镧,0.45mL浓度为7.35mol/L的磷酸,得溶液B;
(3)在不断搅拌下将溶液B缓慢的滴入溶液A中,继续搅拌40min得到浅黄色均匀透明的溶胶,即得La、N、P共掺杂TiO2溶胶。
注:在溶胶制备过程中,除加药品外,过程均密封。
2.微波辅助制备复合光催化剂
将预处理后的煤基活性炭8g浸于钛溶胶80g中密封静置24h成半固化状态后烘干(放入烘箱设置温度110℃,18小时)。将烘干的复合光催化剂置于微波功率670W辐射15min。
3.复合光催化剂对萘降解的具体步骤:
光催化降解反应在光反应器中进行,为排除外界光源干扰,反应在暗箱中进行。反应器中心置以500W氙灯,将50mL浓度为30mg/L的萘溶液加入石英反应器中,并加入0.02g催化剂样品,避光磁力搅拌60min,充分混合使催化剂达到吸附-脱附平衡。打开光源,光稳定5min,开始计光照反应时间,光照一定时间取样,样品在5000r/min下离心15min,取上清液测定样品在波长为218nm处的吸光度值。
所得的La-N-P-TiO2/AC光催化剂平均粒径为9.1nm,比表面积为800.49m2/g,总孔容为0.71cm3/g,在可见光下对萘降解率可达99.28%,重复使用8次,对萘的降解率依然达到96.1%。
Claims (6)
1.微波强化活性炭负载TiO2光催化剂制备方法,其特征在于,该方法包括如下步骤:
步骤1:钛溶胶制备:
1.1)量取一定量的无水乙醇于锥形瓶中,加入钛酸丁酯,持续搅拌35-45min,得溶液A,备用,其中,所述无水乙醇与太酸钛酸丁酯的体积比为1.1-1.2:1;
1.2)量取一定量的无水乙醇于锥形瓶中,加入蒸馏水、冰乙酸、尿素、硝酸铈和磷酸,得溶液B;
1.3)在不断搅拌下将溶液B缓慢滴入溶液A中,室温条件下,继续搅拌35-45min得到浅黄色均匀透明的钛溶胶,其中,溶液B的溶液A质量比为1:1;
步骤2:微波强化制备复合光催化剂:
将预处理后的煤基活性炭浸于步骤1.3制备得到的钛溶胶中密封静置22-26h成半固化状态后,放入烘箱内设置温度100-110℃,烘干12-18小时,将烘干的复合光催化剂置于微波功率650-700W、辐射12-15min,即得到微波强化活性炭负载共掺杂TiO2光催化剂。
2.根据权利要求1所述的方法,其特征在于,所述步骤1.2中,所述硝酸铈还可以为硝酸镧。
3.根据权利要求1或2所述的方法,其特征在于,所述步骤1.2中的无水乙醇、蒸馏水、冰乙酸、尿素、磷酸和硝酸铈或硝酸镧之间的质量比23.7-27.65:6.5-7.0:10.0-14.0:1.0-2.0:0.22-0.72:1.0-2.0:0.22-0.72:0.3-1.5。
4.根据权利要求1或2所述的方法,其特征在于,所述步骤2中,所述煤基活性炭与钛溶胶的固液比为0.8-0.1:8-10。
5.根据权利要求1或2所述的方法,其特征在于,所述波强化活性炭负载共掺杂TiO2光催化剂的平均粒径为9.1-13.5nm,比表面积为500.04-800.49m2/g,总孔容为0.25-0.71cm3/g。
6.一种使用如权利要求1或2任意一项制备得到的微波强化活性炭负载共掺杂TiO2光催化剂降解萘的方法,其特征在于,具体包括以下步骤:
步骤1:先将光催化降解反应在光反应器中进行,为排除外界光源干扰,反应在暗箱中进行,反应器中心置以450-500W氙灯;
步骤2:将50mL浓度为30mg/L的萘溶液加入石英反应器中,并加入0.02g催化剂样品,避光磁力搅拌60min,充分混合使催化剂达到吸附-脱附平衡。打开光源,光稳定5-10min,开始计光照反应时间,光照30-180min取样,样品在4000-5000r/min下离心15-20min,取上清液测定样品在波长为218nm处的吸光度值,通过下式即可计算出萘的降解率:
其中:Co为初始浓度,Ct为一定光照时间后萘的浓度。
在可见光下对萘降解率达到90.06%-99.28%,重复使用8-10次,对萘的降解率依然达到90%以上。
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