固溶体微球光催化剂的超声喷雾制备及其光催化性能研究
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摘要
自从1972年日本科学家Fujishima和Honda发现在TiO_2电极上光解水制氢以来,光催化技术受到了越来越广泛的关注。TiO_2由于其独特的化学稳定性、无毒和廉价等优点,已经在降解水和空气污染物中显示出巨大的潜力。但是由于其禁带宽度较大(3.2eV),只能吸收太阳光中的紫外光部分,而上述波段的光能量仅占太阳光总能量的5%,导致其利用太阳能的效率较低。为了提高TiO_2的量子产率,研究人员采取了很多有效的方法,如金属离子掺杂,非金属掺杂,染料敏化以及形成复合氧化物等,从根本上提高其利用太阳能的效率。
本文通过超声喷雾热解法(USP)制备出一系列Ti_(1-x)Zr_xO_2固溶体(x=0.000,0.045,0.090,0.135和0.180)光催化剂。对所得样品进行了XRD,SEM,TEM,BET以及UV-vis漫反射表征。实验结果表明,所得产物具有核壳状微球结构,球的直径分布在几百个纳米到几个微米的范围之内:由于TiO_2晶格中部分Ti~(4+)被Zr~(4+)取代,固溶体的能带发生了蓝移。以罗丹明B(RhB)为目标污染物,在模拟太阳光照射的条件下,研究了该系列固溶体光催化剂光催化活性差异,并提出了可能的催化反应机理。该制备方法简便省时,易于操作,适合规模化制备固溶体光催化剂。
在制备出Ti_(1-x)Zr_xO_2固溶体高效光催化剂基础之上,本文进一步通过超声喷雾热解法得到具有可见光活性的碳掺杂的Ti_(0.91)Zr_(0.09)O_2固溶体光催化剂,并进行了一系列的表征。实验结果表明,通过碳掺杂,成功地将固溶体的光吸收范围拓展至可见光区域,并能在可见光条件下有效光催化降解罗丹明B。文章分析了不同的反应条件对产物形貌和性能的影响。
Since Fujishama and Honda discovered that hydrogen can be generated from water by TiO_2 electrode in 1972,many efforts have been made to improve the photocatalytic performance of TiO_2.Because of its high photostability,nontoxicity,low cost,and availability,TiO_2 has been widely utilized for photocatalytic decomposition of harmful organic compounds in water and air.However,it can not utilize the solar light efficiently due to its large band gap(3.2eV).In order to enhance the quantum efficiency of TiO_2, many investigations have been made to improve the intrinsic efficiency of TiO_2.These include doping by transition metal elements,nonmetal elements,sensitization,coupling with other semiconductors,and addition of noble metals.
In this thesis,a series of Ti_(1-x)Zr_xO_2 solid solutions photocatalysts(x=0.000,0.045, 0.090,0.135,and 0.180)were directly obtained by an ultrasonic spray pyrolysis method (USP).The resulting samples were characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,nitrogen adsorption,and UV-Vis diffuse reflectance spectroscopy.The characterizations revealed core-shell spherical structures of the resulting solid solutions.We evaluated photocatalytic activities of the solid solutions on degradation of rhodamine B in aqueous solution under simulated solar light.
On the basis of our previous work,visible-light active carbon-doped Ti_(0.91)Zr_(0.09)O_2 solid solution photocatalysts were also directly obtained by USP method.The characterization results revealed that the carbon doping successfully extended the absorption edges of the solid solution to visible light region.These experiments confirmed that the USP method is suitable to synthesize high-efficiency solid solution photocatalysts in a large scale.
本文通过超声喷雾热解法(USP)制备出一系列Ti_(1-x)Zr_xO_2固溶体(x=0.000,0.045,0.090,0.135和0.180)光催化剂。对所得样品进行了XRD,SEM,TEM,BET以及UV-vis漫反射表征。实验结果表明,所得产物具有核壳状微球结构,球的直径分布在几百个纳米到几个微米的范围之内:由于TiO_2晶格中部分Ti~(4+)被Zr~(4+)取代,固溶体的能带发生了蓝移。以罗丹明B(RhB)为目标污染物,在模拟太阳光照射的条件下,研究了该系列固溶体光催化剂光催化活性差异,并提出了可能的催化反应机理。该制备方法简便省时,易于操作,适合规模化制备固溶体光催化剂。
在制备出Ti_(1-x)Zr_xO_2固溶体高效光催化剂基础之上,本文进一步通过超声喷雾热解法得到具有可见光活性的碳掺杂的Ti_(0.91)Zr_(0.09)O_2固溶体光催化剂,并进行了一系列的表征。实验结果表明,通过碳掺杂,成功地将固溶体的光吸收范围拓展至可见光区域,并能在可见光条件下有效光催化降解罗丹明B。文章分析了不同的反应条件对产物形貌和性能的影响。
Since Fujishama and Honda discovered that hydrogen can be generated from water by TiO_2 electrode in 1972,many efforts have been made to improve the photocatalytic performance of TiO_2.Because of its high photostability,nontoxicity,low cost,and availability,TiO_2 has been widely utilized for photocatalytic decomposition of harmful organic compounds in water and air.However,it can not utilize the solar light efficiently due to its large band gap(3.2eV).In order to enhance the quantum efficiency of TiO_2, many investigations have been made to improve the intrinsic efficiency of TiO_2.These include doping by transition metal elements,nonmetal elements,sensitization,coupling with other semiconductors,and addition of noble metals.
In this thesis,a series of Ti_(1-x)Zr_xO_2 solid solutions photocatalysts(x=0.000,0.045, 0.090,0.135,and 0.180)were directly obtained by an ultrasonic spray pyrolysis method (USP).The resulting samples were characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,nitrogen adsorption,and UV-Vis diffuse reflectance spectroscopy.The characterizations revealed core-shell spherical structures of the resulting solid solutions.We evaluated photocatalytic activities of the solid solutions on degradation of rhodamine B in aqueous solution under simulated solar light.
On the basis of our previous work,visible-light active carbon-doped Ti_(0.91)Zr_(0.09)O_2 solid solution photocatalysts were also directly obtained by USP method.The characterization results revealed that the carbon doping successfully extended the absorption edges of the solid solution to visible light region.These experiments confirmed that the USP method is suitable to synthesize high-efficiency solid solution photocatalysts in a large scale.
引文
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