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3DOM-TiO2的可控合成、表面修饰及光催化性能研究
论文作者:童鞋论文网  论文来源:www.txlunwenw.com  发布时间:2019/10/26 13:32:41  

摘要:二氧化钛(TiO2)作为一种重要的半导体材料,具有长期稳定,耐腐蚀和无毒等优点,但是存在可见光下的响应较弱、电子与空穴易符合等缺陷。在材料科学领域,围绕TiO2的研究工作一直是材料及催化研究人员关注的热点。3DOM-TiO2其本身为反蛋白石结构(即三维互通的规则孔道),因此具有非常高的表面积、高的衰减率以及低的导热性能,从而展现出优于其他形貌TiO2的特殊性能。

本课题基于3DOM-TiO2载体材料,从结构以及表界面调控的角度出发,分别采用无机碳材料和金属氧化物材料对其进行可控地改性研究,借助光催化性能表征,建立材料结构与性能之间的构效关系,并提出了合理的解释。具体研究内容如下:

(1)通过调节自组装过程的驱动力,首次合成了窗口尺寸可调控的三维有序大孔TiO2。并通过XRD,SEM,TEM,BET等表征手段确定了催化材料的晶型,结构和比表面积。通过光催化实验确定3DOM-TiO2材料在光催化活性和连接窗口尺寸之间表现出明显的线性关系,这为连接窗口尺寸效应提供了新的视角。基于实验结果,提出了具有窗口尺寸依赖效应的3DOM-TiO2的可能机理,研究结果对于3DOM大类光催化材料的设计与合成具有一定的指导意义。

(2)基于(1)部分的窗口优化结果,采用甲阶段酚醛树脂作为碳前躯体,通过调控甲阶段酚醛树脂的不同质量分数,首次实现了对于3DOM-TiO2表面碳层厚度的精细调控。通过XRD,SEM,TEM,BET等手段对其基本物理化学性质进行了表征。光催化研究结果表明,碳层厚度对其吸附及降解过程均有较大影响。过小(6.3 wt%)或过大(62 wt%)的碳负载量均会限制3DOM-TiO2的催化性能。碳负载量为12 wt%的样品具有最优的吸附降解效果。

(3)基于(1)部分的窗口优化结果,采用聚多巴胺作为碳氮(NC)的前驱体,通过简单的后处理来合成NC修饰的3DOM-TiO2材料。借助XRD,SEM,TEM,BET等表征手段确定了催化材料的基本物理化学性质。相比于纯碳材料修饰的3DOM-TiO2,3DOM-TiO2@NC复合材料在紫外光辐照下的催化性能更加优异,即使在可见光下也表现出不错的光催化降解性能。

(4)通过甲醛气相还原法,探索了Cu2O在3DOM-TiO2表面及体相两种方式的负载。首次制备了表面(Cu2O/3DOM-TiO2)及体相(3DOM-Cu2O-TiO2)负载的3DOM-TiO2材料。通过XRD,SEM,TEM,BET等表征手段确定了催化材料的晶型、表界面状态等物理化学性质。结果表明,掺杂Cu2O有效地提高了光电子激发与电荷载体分离的效率,最终在可见光下实现了非贵金属纳米粒子负载TiO2的光解水产氢。

As an important semiconductor material,titanium dioxide (TiO2) has the advantages of long-term stability, corrosionresistance and non-toxicity, but it has weak defects in visible light and easyto conform to electrons and holes. In the field of materials science, researchwork around TiO2 has been a hot spot for materials and catalysis researchers.3DOM-TiO2 itself is an inverse opal structure (for example, a regular channelof three-dimensional intercommunication), and therefore has a very high surfacearea, high attenuation rate and low thermal conductivity, thereby exhibitingspecial properties superior to other morphologies of TiO2.

Based on the 3DOM-TiO2 carrier material,the subject is controlled by the inorganic carbon material and the metal oxidematerial from the perspective of structure and surface interface control. Thestructure and properties of the material are established by photocatalytic performancecharacterization. The structure-activity relationship between them and areasonable explanation. The specific research contents are as follows:

(1) By adjusting the driving force of theself-assembly process, the three-dimensional ordered macroporous TiO2 withwindow size controllable was synthesized for the first time. The crystal form,structure and specific surface area of the catalytic material were determinedby XRD, SEM, TEM, BET and other characterization methods. The photocatalyticexperiment determined that the 3DOM-TiO2 material showed a clear linearrelationship between photocatalytic activity and the size of the connectionwindow, which provided a new perspective for the connection window size effect.Based on the experimental results, the possible mechanism of 3DOM-TiO2 withwindow size dependence is proposed. The research results have certain guidingsignificance for the design and synthesis of 3DOM photocatalytic materials.

(2) Based on the window optimizationresults of part (1), using the stage phenolic resin as the carbon precursor,the fine control of the thickness of the surface carbon layer of 3DOM-TiO2 wasachieved for the first time by regulating the different mass fractions of thephenolic resin. The basic physical and chemical properties were characterizedby XRD, SEM, TEM and BET. The results of photocatalysis show that the thicknessof carbon layer has a great influence on its adsorption and degradationprocesses. Too small (6.3 wt%) or too large (62 wt%) carbon loading will limitthe catalytic performance of 3DOM-TiO2. Samples with a carbon loading of 12 wt%have the best adsorption degradation.

(3) Based on the window optimizationresults of part (1), polydopamine was used as a precursor of carbon nitrogen(NC), and NC modified 3DOM-TiO2 material was synthesized by simple posttreatment. The basic physical and chemical properties of the catalyticmaterials were determined by XRD, SEM, TEM, BET and other characterizationmethods. Compared with the pure carbon material modified 3DOM-TiO2, the3DOM-TiO2@NC composite has better catalytic performance under ultraviolet lightirradiation, and exhibits good photocatalytic degradation performance evenunder visible light.

(4) The loading of Cu2O on the surface andbulk of 3DOM-TiO2 was investigated by formaldehyde vapor phase reductionmethod. The surface (Cu2O/3DOM-TiO2) and bulk (3DOM-Cu2O-TiO2) supported3DOM-TiO2 materials were prepared for the first time. The physicochemicalproperties such as crystal form and surface state of the catalytic materialwere determined by XRD, SEM, TEM, BET and other characterization methods. Theresults show that the doping of Cu2O effectively improves the efficiency ofphotoelectron excitation and charge carrier separation, and finally realizesthe photolysis of hydrogen produced by non-precious metal nanoparticles loadedwith TiO2 under visible light.

关键词:3DOM-TiO2;可控合成;表面修饰;光催化

3DOM-TiO2; Controllable synthesis; Surfacemodification; Photocatalysi

上一篇:双子磷酸酯改性硼酸锌晶须及其在聚 乙烯中的阻燃增强研究     下一篇:聚偏氟乙烯/凹凸棒石复合超滤膜结构调控及其性能
 
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