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1.
TiO(2) and Fe-titanate (different wt%) supported on zeolite were prepared by sol-gel and solid-state dispersion methods. The photocatalysts prepared were characterized by X-ray diffraction, scanning electron microscopy and ultraviolet (UV)-visible diffuse reflectance spectroscopy techniques. Photocatalytic reduction of nitrate in water and isopropanol/oxalic acid as hole scavengers are investigated in a batch reactor under UV illumination. The yield of urea increased notably when the catalysts were supported on zeolite. The Fe-titanate supported catalyst promotes the charge separation that contributes to an increase in selective formation of urea. The product formation is because of the high adsorption of in situ generated CO(2) and NH(3) over shape-selective property of the zeolite in the composite photocatalyst. The maximum yield of urea is found to be 18 ppm while 1% isopropanol containing solution over 10 wt% Fe-titanate/HZSM-5 photocatalyst was used.  相似文献   

2.
反胶束体系制备负载型TiO2纳米光催化剂   总被引:7,自引:0,他引:7  
在AOT/异辛烷反胶束体系中制备了粒径为2~5nm的单分散球形TiO2纳米粒子,用TEM,DSC和XRD等手段对其进行了分析;用浸渍法以小孔分子筛HZSM-5为载体制备了负载型TiO2纳米粒子,用FTIR,Langmuir及BET等手段进行了表征;用以上2种TiO2粒子作光催化剂进行了简单模拟废水处理研究,用UV-Vis光谱分析其催化效果表明,负载型TiO2纳米粒子比纯TiO2纳米粒子的光催化活性更高.  相似文献   

3.
将改良式溶胶-凝胶法制备的酸性触媒TiO2/SO24-涂布于不锈钢网上,并利用自行设计之批次式光催化反应器,在三组近紫外灯管(波长为365nm,光强度为2.0mW/cm2)照射下,进行CO2光催化还原反应操作参数(还原剂种类、CO2初始浓度和反应温度)之影响研究.结果显示,使用氢气为还原剂可获得最高的光催化还原速率,光还原反应之主要气态产物为CO和甲烷,其次为微量的乙烯与乙烷.同时,光催化还原速率亦随着CO2初始浓度及反应温度的提高而增加.FT-IR光谱分析发现,TiO2/SO42-光触媒表面有甲酸、甲醇、碳酸盐、甲酸盐及甲酸甲酯等产物之存在.TiO2/SO42-光触媒催化还原CO2有两种可能反应路径,其中一种反应路径生成CO,CH4,C2H4及C2H6等气态产物;而另一种反应路径则生成CO23a-ds,CH3OHads,HCOOa-ds,HCOOHads,HCOHads与HCOOCH3ads等吸附在光触媒表面的产物.  相似文献   

4.
B掺杂TiO2/AC光催化剂的制备及活性   总被引:13,自引:1,他引:13  
以硼酸和钛酸丁酯为主要原料,以活性炭(AC)为载体。用溶胶-凝胶法制备了B掺杂TiO2/AC光催化剂.用X射线衍射(XRD)、紫外可见漫反射吸收光谱(UV—VIS)对制得的光催化剂进行了表征.以甲基橙水溶液的光催化脱色反应和氧化乐果水溶液的光催化降解反应。考查了不同B掺杂TiO2/AC光催化剂的活性.结果表明,所有B掺杂TiO2/AC光催化剂均为锐钛矿晶相.B的掺杂未导致TiO2/AC光催化剂的吸收带边发生明显的移动.当B-TiO2质量分数分别为2.0%和2.5%时,TiO2/AC光催化剂的活性有明显的提高.B-TiO2质量分数2.0%时活性最高.但是,当B-TiO2质量分数分别为1.5%和3.0%时。TiO2/AC光催化剂的活性降低.B的缺电子特性可能改变了TiO2能带中的电子密度,使光催化反应中光生电子和空穴的俘获方式发生变化;同时。B的缺电子特性也会使光催化剂表面的Lewis酸强度增强,导致表面吸附OH-数量和目标反应物的吸附方式发生变化.这些可能是B-TiO2/AC光催化剂活性发生变化的主要原因.  相似文献   

5.
Mesostructured TiO(2) nanocrystals have been prepared using Pluronic F127 as the structure-directing agent. Platinum nanoparticles at different contents (0.1-1.0 wt%) have been photochemically deposited onto the mesoporous TiO(2). TEM investigation of 0.2 wt% Pt/TiO(2) calcined at 450 °C reveals that the TiO(2) particles are quite uniform in size and shape with the particle sizes of TiO(2) and Pt being 10 and 3 nm, respectively. The photocatalytic activities of the Pt loaded TiO(2) have been assessed and compared with those of nonporous commercial Pt/TiO(2)-P25 by determining the rates and the photonic efficiencies of molecular hydrogen production from aqueous methanol solutions. The results show that the amount of hydrogen evolved on Pt/TiO(2)-450 at low Pt loading (0.2 wt%) is three times higher than that evolved on Pt/TiO(2)-P25 and twelve times higher than that evolved on Pt/TiO(2)-350. Despite the BET surface area of the TiO(2)-450 photocatalyst being 3.5 times higher than that of TiO(2)-P25, a 60% smaller amount of the Pt co-catalyst is required to obtain the optimum photocatalytic hydrogen production activity. The reduced Pt loading on the mesoporous TiO(2) will be important both from a commercial and an ecological point of view.  相似文献   

6.
TiO2膜电极光电催化降解苯甲酸的机理研究   总被引:1,自引:0,他引:1  
利用自制纳米TiO2薄膜作电极, 对苯甲酸光电催化降解过程进行了系统研究. 同时利用扫描电镜(SEM)、X射线衍射图谱(XRD)和光电流-电压响应谱分析光催化剂的微观性质和光电性能. 选取较高的pH 10.5, 以利于苯甲酸降解中间产物的检测(GC/MS). 通过对比光电催化与单一的TiO2光催化体系中苯甲酸的降解动力学、总有机碳(TOC)的去除率、降解产物的生成(GC/MS)及活性自由基物种的产生(ESR), 提出光电催化降解苯甲酸的具体反应路径和氧化机理. 羟基化的苯甲酸在羟基自由基与活性氧自由基的共同作用下, 经由含六个碳原子的二酸(顺式己二烯二酸), 被进一步氧化成小分子酸和CO2.  相似文献   

7.
高活性Ti基纳米TiO_2膜催化电极的制备   总被引:16,自引:0,他引:16  
采用“牺牲阳极法”恒槽压电解含有 0 .0 0 5mol·L- 1四乙基溴化铵的乙醇溶液 ,加入微量乙酰丙酮作稳定剂 ,电合成TiO2 前驱体钛酸乙酯Ti(EtO) 4 ,经水解、涂膜、煅烧制备Ti基纳米TiO2 膜电极 (Ti/nano_TiO2 ) .TEM、SEM、XRD测试表明 :TiO2 颗粒尺寸在 10~ 35nm ,膜厚达 0 .5μm ,主要为锐钛矿晶型 ,膜为多孔三维网状结构 .循环伏安法研究了纳米TiO2 膜电极对草酸还原为乙醛酸、硝基苯还原为对氨基苯酚反应的电催化活性 ,结果发现纳米膜中的Ti(Ⅳ ) /Ti(Ⅲ )氧化还原电对起一种中介作用 ,可使有机物如草酸和硝基苯间接电还原 ,且电极催化活性高 ,性能稳定  相似文献   

8.
采用溶胶 凝胶法制备复合纳米微粒Rh3+/TiO2/SnO2作系列光催化剂,运用BET、XRD等技术对样品进行了表征.讨论了影响污染物4 (2 吡啶偶氮)间苯二酚(PAR)光催化降解率的主要因素,实验结果表明:以Rh3+/TiO2/SnO2为复合光催化剂,当m(TiO2)∶m(SnO2)=56:44,ω(Rh3+)=2.0%,催化剂用量为1.0 g,通入空气的流量为10.0 L/min,试液的质量分数为2.0×10-6,pH=7.0时,光照2h,PAR的降解率达到96.2%.  相似文献   

9.
H4SiW12O40/TiO2/SiO2复合光催化剂的制备及性能研究   总被引:3,自引:2,他引:3  
溶胶-凝胶法制备了TiO2/S iO2光催化剂,利用所得TiO2/S iO2光催化剂为基体,浸渍烧结法制备了H4S iW12O40/TiO2/S iO2表面负载修饰型复合光催化剂。TG-DSC、XRD、SEM、BET对催化剂的物化结构进行了表征,分析了TiO2和H4S iW12O40催化活性组分在S iO2载体表面上的键联机理。光催化性能测试是以低浓度酸性品红染料的水溶液为降解目标物,试验结果表明H4S iW12O40的负载修饰可以改进TiO2/S iO2光催化剂的催化活性,酸性品红的降解效率最高可以增加45%。  相似文献   

10.
Photolysis studies on formic acid (HCOOH) and formate ion (HCOO−) in presence of TiO2, a photocatalyst, as suspension in water were carried out separately using 350 nm ultraviolet light. The products, such as H2, CO, CO2 and CH4, generated during the experiments were monitored with varying the ambient, light exposure time, and the concentration of HCOOH/HCOO−. The yields of CO in all these systems increased with light exposure time. In aerated systems, CO yields were higher in contrast to the deoxygenated (Ar-purged) systems under identical conditions. It is proposed apparently that the formation of CO is taking place during the chemical reduction of in-situ generated CO2, a photo-mineralized product of HCOOH/HCOO−, but not through the direct photodecomposition or photodehydration (CO+H2O) of solute molecules. The rates of CO formation during 1.3 M HCOOH photolysis in presence of TiO2 photocatalyst were evaluated to be 0.21 and 0.13 μl/min in aerated and Ar-purged systems, respectively. As compared with HCOOH systems, the CO yields are lower when 0.2 M HCOONa was exposed to light under identical conditions. The CO growth rates were evaluated to be 0.07 and 0.046 μl·min−1 for aerated and deoxygenated HCOONa systems, respectively; moreover, the trend is quite similar to that of the HCOOH system. Under these conditions, the emission of H2 was also observed, and its yield was significantly higher in Ar-purged system as compared with the CO yields. However, in aerated system, the yields of these products were just opposite. The formation of low yield of methane was observed during photolysis of HCOOH/HCOO− ions. In CO2 ambient, the yields of CO and H2 varied drastically with time.  相似文献   

11.
以草酸为电子给体在Pt-TiO2上光催化生成氢   总被引:8,自引:0,他引:8  
 以草酸为电子给体,研究了在Pt-TiO2上光催化生成氢的反应.草酸的存在明显促进了生成氢的反应;二氧化钛负载Pt也明显提高了反应速率,Pt的最佳负载量为w(Pt)=0.5%.草酸浓度对氢生成反应的影响符合Lang-muir关系式.最佳pH值为2~4.  相似文献   

12.
甲醇在纳米TiO2作用下进行光催化氧化反应的机理研究   总被引:1,自引:0,他引:1  
以纳米TiO2为催化剂,以主波长为364 nm的汞灯为光源,用气相色谱法分别考察了0.1 mol/L的甲醇、甲醛和甲酸水溶液进行光催化氧化反应的动力学规律.Langmuir-Hinshelwood方程进行核算结果证明,该组反应均为零级反应.用TEM、 XRD、 SSA和XPS对催化剂进行表征.根据XPS的检测结果提出了甲醇光催化氧化的反应机理.TiO2光激发活化时间约为30~60 min,生成物及剩余反应物浓度随时间变化的曲线表明,该反应速率为HCH2OH相似文献   

13.
TiO2 has attracted considerable attention due to its stability, non-toxicity, low cost, and great potential for use as a photocatalyst in environmental applications. Since strong metal-support interaction (SMSI) of titania-supported noble metals was first reported in 1978, titania supported catalyst has been intensively studied in heterogeneous catalysis. However, the effective catalytic activity was restricted due to the low surface area of TiO2. Recently, TiO2-based nanotubes were extensively investigated because of their potentials in many areas such as highly efficient photocatalysis and hydrogen sensor.In the present study, formation of titanium oxide (TiO2) nanotubes was carried out by hydrothermal method, with TiO2 nanoparticle-powders immersed in concentrated NaOH solution in an autoclave at 110 ℃. Preparation of nano-size Pt on TiO2-nanoparticles or TiO2-nanotubes was performed by photochemical deposition method with UV irradiation on an aqueous solution containing TiO2 and hexachloroplatinic acid or tetrachloroauric acid. The TEM micrographs show that TiO2-nanotubes exhibit ~300 nm in length with an inner diameter of ~ 6 nm and the wall thickness of ~ 2 nm, and homogeneous nanosize Pt particles (~ 2 nm) were well-dispersed on both nanoparticle- and nanotube- titania supports. It also shows the nanotube morphology was retained up2o n Pt-immobilization. Nitrogen adsorption isotherm at 77K resulted a high surface area (~ 200m/g) of TiO2-nanotubes, which is about 40 times greater than that of "mother" TiO2 nanoparticles (~5 m/g). All the spectroscopic results exhibited that the nanotube structure was not significantly affected by the immobilized Pt particles. Ti K-edge XANES spectra of TiO2 nanotube and Pt/TiO2-nanotube represent that most titanium are in a tetrahedral coordination with few retained in the octahedral structure.In the in-situ FT-IR experiments, an IR cell was evacuated to a pressure of 10-5 torr at room temperature as soon as the catalyst-pellet, Pt/TiO2 or Pt/TiO2-nanotube, was placed inside the cell.Then, 60 torr of hydrogen was introduced into the cell and subsequently the temperature was programmed to increase from room temperature to 300℃ at a constant heating rate of 5℃/min.For Pt/TiO2, an IR peak at 2083 em-1 started to appear at 200℃ with a maximum intensity at 250℃ and then decreasing as temperature increased. The 2083 em-1 IR peak corresponds to the linearly adsorption of CO on the well-dispersed Pt sites. Simultaneously, the IR bands of gaseous methane at 3016 em-1 started to appear at 225℃ and the peak intensity increased with temperature. The results reveal that Pt/TiO2 can adsorb gaseous CO2 and further catalyzes the reduction of CO2 by H2 through the intermediate CO, which further produces gaseous methane. While for the Pt/TiO2-nanotube catalyst, methane was produced at relatively low temperature, 100℃, and it catalyzed the direct conversion of CO2 to CH4. The absence of intermediate CO-adsorption signals durinng the temperature programmed process indicates that the prepared TiO2 nanotube-supported nanosize Pt possesses a potent capability for CO2 adsorption and highly catalytic activity in the hydrogenation of CO2, and was superior to the conventional Pt/TiO2 catalyst. The catalytic activity of Pt/TiO2-nanotube was indeed significantly enhanced by the high surface area of TiO2-nanotubes.Details will be discussed.  相似文献   

14.
本文提出用氧扩散膜作TiO2光催化膜的载体,介绍了氧扩散膜的制备及TiO2在氧扩散膜表面的固定方法,TiO2光催化膜的表面形态与微结构,不同条件下光催化分解草酸的速度.研究结果表明,以氧扩散膜作载体的TiO2光催化薄膜表现出了较高的光催化活性.文中详细分析了氧扩散膜的作用.  相似文献   

15.
The degradation of aniline has been investigated using aqueous TiO2 suspensions containing carbonate ions as photocatalyst. The addition of carbonate to Degussa P-25 increased the number of active adsorption sites at its surface. For the TiO2 suspensions containing carbonate ions the intensity of adsorption of aniline increased to 6.9 x 10(2) from 5.5 x 10(2) mol(-1) dm(3) in case of bare TiO2 suspensions. This in turn results in the increased interfacial interaction of the photogenerated charge carriers with the adsorbed aniline and thus enhancing the rate of its photodecomposition to 6.5 x 10(-6) mol dm(-3) s(-1) compared to 2.7 x 10(-6) mol dm(-3) s(-1) in the absence of Na(2)CO(3). The maximum efficiency of this photocatalyst has been obtained upon addition of 0.11 mol dm(-3) of Na(2)CO(3) at pH 10.8. The photocatalytic action is understood by the simultaneous interaction of intermediates, *OH and CO*-(3), and their reactivity with aniline. Azobenzene, p-benzoquinone, nitrobenzene, and NH(3) have been identified as the major products of the photooxidation of aniline. Both the reactant and products have been followed kinetically. The photodegradation follows Langmuir-Hinshelwood Model. The mechanism of the occurring reactions has been analyzed and discussed. In the presence of Na(2)CO(3), 3 x 10(-3) mol dm(-3) of aniline could be photodegraded completely in about 6 h while all organic intermediates decomposed completely within about 10 h.  相似文献   

16.
光催化还原CO2生成烃类燃料是一种可同时解决全球变暖和能源危机问题的最有效途径之一。尽管这方面的研究已经取得了一定的进展,但是整体的光催化转换效率还非常低。因此,需要发展更加高效的催化剂。由于半导体材料禁带宽度与太阳光谱相匹配,人们已经对其进行了广泛研究。其中TiO2因具有无毒、强氧化性以及良好的光学和电学性质等而成为最主要的研究对象。但是对于光催化还原CO2反应来说, TiO2仍存在很多不足,如只能吸收太阳光谱中的紫外光,光生载流子会快速结合,以及光生空穴的强氧化能力等,这些都限制了其光催化还原CO2的效率。采用窄禁带宽度半导体修饰TiO2是解决上述不足的有效途径之一。本文采用简单的电化学方法成功制备了一种由窄禁带半导体Cu2O修饰的TiO2纳米管(TNTs)的复合物,并运用扫描电子显微镜(SEM)、X射线衍射(XRD)以及X射线光电子能谱(XPS)表征了所制备复合物的形貌、化学组成和结晶度。表征结果显示,所制备的TiO2为整齐排列的纳米管阵列结构;复合物中的纳米颗粒为Cu2O;当电化学沉积Cu2O的时间为5 min时,得到的Cu2O纳米颗粒初步呈类八面体结构。随着沉积时间的增加, Cu2O颗粒尺寸增加,具有八面体结构。 XRD和XPS结果表明, TiO2纳米管为锐钛矿,八面体Cu2O纳米颗粒的主要暴露晶面为(111)面。我们还进一步研究了不同量Cu2O纳米颗粒修饰的TiO2纳米管复合物在可见光以及模拟太阳光下光催化还原CO2的能力。在可见光下,由于自身的禁带宽度,纯净的TiO2纳米管没有任何光催化还原CO2的能力;经过Cu2O纳米颗粒的修饰,复合物显现出明显的光催化还原CO2的能力,其中经过30 min Cu2O沉积的TNTs具有最高的光催化效率。在模拟太阳光下,经过15 min Cu2O沉积的TNTs具有最高的光催化效率。在所有光催化还原CO2过程中,主要碳氢产物为甲烷。为了深入地理解该复合体系在还原CO2中的高催化效率,我们对催化剂进行了进一步的表征。紫外-可见漫反射光谱表明, Cu2O八面体纳米颗粒的沉积将TNTs的吸收光谱拓展到了可见光区域,提高了复合物对太阳光的吸收能力。此外,我们还通过测试所制样品的光电流反应、荧光发射光谱以及电化学阻抗谱,研究了催化剂中光生电子和空穴的分离和迁移能力。结果表明,适量的Cu2O沉积提高了复合物对光的吸收能力,增加了光生载流子的数量,从而使更多的光生载流子参与光催化反应。综上,本文首次报道了八面体Cu2O纳米颗粒修饰TNTs复合物的光催化还原CO2的能力。在一定量的Cu2O纳米颗粒修饰下,该复合物在光催化还原CO2生成烃类反应中表现出高效性。经过一系列详细的表征和讨论,我们认为其高效性主要源于三个方面:(1) TNTs的管状结构为反应物的吸附提供了大量的活性位点,同时一维的管状结构更有利于光生载流子的运载,从而提高了电子和空穴的分离;(2) Cu2O纳米颗粒的修饰提高了催化剂对光的吸收,促进催化剂最大程度地利用太阳光;(3) TiO2和Cu2O之间导带以及价带位置的匹配,在减少光生载流子复合的同时也降低了TiO2价带上空穴的氧化能力,从而抑制了CO2还原产物的再氧化过程。  相似文献   

17.
CeO2-TiO2复合氧化物的制备、表征及其对CO氧化的催化性能   总被引:1,自引:0,他引:1  
采用溶胶-凝胶法制备了一系列不同n(Ce)/n(Ti)的CeO2-TiO2复合氧化物,对复合氧化物的物相结构、形貌特征、比表面积和氧化还原性质进行了表征,并考察了复合氧化物对CO氧化反应的催化性能.结果表明,n(Ce)/n(Ti)>0.10时,复合氧化物为无定形结构;n(Ce)/n(Ti)=0.10~0.30时,复合氧化物失去CeO2和TiO2各自的特征,形成CeO2-TiO2固溶体,具有较大的比表面积.CeO2-TiO2复合氧化物本身对CO氧化反应的催化活性不如TiO2或CeO2的高,但Pd/CeO2-TiO2比Pd/TiO2或Pd/CeO2具有更高的催化活性.  相似文献   

18.
The production of H(2) by photocatalytic water splitting has attracted a lot attention as a clean and renewable solar H(2) generation system. Despite tremendous efforts, the present great challenge in materials science is to develop highly active photocatalysts for splitting of water at low cost. Here we report a new composite material consisting of TiO(2) nanocrystals grown in the presence of a layered MoS(2)/graphene hybrid as a high-performance photocatalyst for H(2) evolution. This composite material was prepared by a two-step simple hydrothermal process using sodium molybdate, thiourea, and graphene oxide as precursors of the MoS(2)/graphene hybrid and tetrabutylorthotitanate as the titanium precursor. Even without a noble-metal cocatalyst, the TiO(2)/MoS(2)/graphene composite reaches a high H(2) production rate of 165.3 μmol h(-1) when the content of the MoS(2)/graphene cocatalyst is 0.5 wt % and the content of graphene in this cocatalyst is 5.0 wt %, and the apparent quantum efficiency reaches 9.7% at 365 nm. This unusual photocatalytic activity arises from the positive synergetic effect between the MoS(2) and graphene components in this hybrid cocatalyst, which serve as an electron collector and a source of active adsorption sites, respectively. This study presents an inexpensive photocatalyst for energy conversion to achieve highly efficient H(2) evolution without noble metals.  相似文献   

19.
TiO2 was prepared by sol-gel method using tetrabutyl titanate as precursor. TiO2 was loaded on Bi12TiO20. The photocatalyst with different TiO2 loading was calcined at 723 K. The photocatalytic activity of decomposition gaseous benzene was investigated in a batch reactor. The prepared photocatalyst was characterized by UV-vis diffuse reflectance. The result showed that TiO2/Bi12TiO20 absorbed much more ultraviolet light than Ti02 in the ultraviolet light region and showed red shift. The results indicated that the prepared photocatalyst can greatly promote the photocatalytic activity. The 2.0% TiO2/Bi12TiO20 system exhibited the highest photocatalytic activity.  相似文献   

20.
A simple method of synthesizing a large quantity of TiO(2) nanorods was developed. A nonhydrolytic sol-gel reaction between titanium(IV) isopropoxide and oleic acid at 270 degrees C generated 3.4 nm (diameter) x 38 nm (length) sized TiO(2) nanocrystals. The transmission electron microscopic image showed that the particles have a uniform diameter distribution. X-ray diffraction and selected-area electron diffraction patterns combined with high-resolution transmission electron microscopic image showed that the TiO(2) nanorods are highly crystalline anatase crystal structure grown along the [001] direction. The diameters of the TiO(2) nanorods were controlled by adding 1-hexadecylamine to the reaction mixture as a cosurfactant. TiO(2) nanorods with average sizes of 2.7 nm x 28 nm, 2.2 nm x 32 nm, and 2.0 nm x 39 nm were obtained using 1, 5, and 10 mmol of 1-hexadecylamine, respectively. The optical absorption spectrum of the TiO(2) nanorods exhibited that the band gap of the nanorods was 3.33 eV at room temperature, which is 130 meV larger than that of bulk anatase (3.2 eV), demonstrating the quantum confinement effect. Oleic acid coordinated on the nanorod surface was removed by the reduction of the carboxyl group of oleic acid, and the Brunauer-Emmett-Teller surface area of the resulting naked TiO(2) nanorods was 198 m(2)/g. The naked TiO(2) nanorods exhibited higher photocatalytic activity than the P-25 photocatalyst for the photocatalytic inactivation of E. coli.  相似文献   

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