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1.
Ag改性提高TiO2对Cr(VI)的光催化还原活性机理   总被引:14,自引:0,他引:14  
在消除了质子缺乏、光生电子-空穴复合对Cr6+光催化还原负效应影响下,比较了TiO2和Ag/TiO2(Ag质量分数 1.0%)光催化还原活性.结果表明,相同条件下Ag/TiO2表现出比TiO2更高的催化活性. EPR分析表明,对于Ag/TiO2,UV照射后Ag表面有活性物种生成,在TiO2上有活性中心表相Ti3+生成.光生电子通过表相Ti3+向Cr6+传递电子是Cr6+光催化还原的速度控制步骤.较多的表相Ti3+参与还原反应是Ag/TiO2表现出较高催化活性的主要原因,担载Ag上积聚光生电子的较强流动性对反应也起到一定促进作用.  相似文献   

2.
在消除了质子缺乏、光生电子-空穴复合对Cr6 光催化还原负效应影响下,比较了TiO2和Ag/TiO2(Ag质量分数1.0%)光催化还原活性.结果表明,相同条件下Ag/TiO2表现出比TiO2更高的催化活性.EPR分析表明,对于Ag/TiO2,UV照射后Ag表面有活性物种O2生成,在TiO2上有活性中心表相Ti3 生成.光生电子通过表相Ti3 向Cr6 传递电子是cr6 光催化还原的速度控制步骤.较多的表相Ti3 参与还原反应是Ag/TiO2表现出较高催化活性的主要原因,担载Ag上积聚光生电子的较强流动性对反应也起到一定促进作用.  相似文献   

3.
Ag改性提高TiO2对Cr(Ⅵ)的光催化还原活性机理   总被引:3,自引:0,他引:3  
在消除了质子缺乏、光生电子-空穴复合对Cr6+光催化还原负效应影响下,比较了TiO2和Ag/TiO2(Ag质量分数1.0%)光催化还原活性.结果表明,相同条件下Ag/TiO2表现出比TiO2更高的催化活性.EPR分析表明,对于Ag/TiO2,UV照射后Ag表面有活性物种O-2生成,在TiO2上有活性中心表相Ti3+生成.光生电子通过表相Ti3+向Cr6+传递电子是Cr6+光催化还原的速度控制步骤.较多的表相Ti3+参与还原反应是Ag/TiO2表现出较高催化活性的主要原因,担载Ag上积聚光生电子的较强流动性对反应也起到一定促进作用.  相似文献   

4.
Au/TiO2光催化分解臭氧   总被引:7,自引:0,他引:7  
 采用沉积-沉淀法制备了Au/TiO2催化剂,用透射电子显微镜、紫外-可见漫反射光谱和X射线光电子能谱进行了表征,结果表明,样品在空气中于200 ℃处理后,金以金属态Au0的形式沉积在TiO2表面. 与TiO2相比,担载金的TiO2具有明显的光催化分解O3的活性. 黑光灯光照20 h后, 1%Au/TiO2催化剂对O3的分解率仍达98%以上. TiO2上的Au簇作为电子的捕获中心,能够促使电子与空穴的有效分离. 而Au簇和载体TiO2的周界处作为O3新的吸附活性中心,促进了O3的分解.  相似文献   

5.
多价态共存的Ag-TiO2光催化剂的制备及光催化活性   总被引:9,自引:0,他引:9  
辛柏福  井立强  任志宇  王健强  于海涛  付宏刚 《化学学报》2004,62(12):1110-1114,MJ02
在避光条件下采用溶胶凝胶法制备了Ag-TiO2光催化剂,通过XRD, Raman, PL和XPS表征及对光催化降解罗丹明B的性能评价,发现Ag的掺入抑制了TiO2锐钛矿相的晶化,促进了TiO2由锐钛矿相向金红石相的转变.随着掺Ag量的增加,PL光谱强度下降,这说明Ag掺入抑制了光生电子空穴的复合.在较低掺杂浓度区(Ag/Ti atom<3%)以Ag+的迁移、扩散为主,在较高浓度掺杂区(Ag/Ti atom≥3%) Ag+的迁移、扩散和表面还原共存,在浅表层扩散阈值附近(Ag/Ti atom=3%~5%), Ag-TiO2光催化剂既有丰富的浅表层电子捕获阱,又有利于电子向表面还原态Ag的导出,使光生电子和空穴的复合得到有效的抑制,从而使光催化效率显著提高.当掺杂浓度大于阈值时,Ag-TiO2催化剂的催化活性降低.  相似文献   

6.
纳米Au/TiO2光催化剂的XPS和SPS研究   总被引:4,自引:0,他引:4  
 以溶胶-凝胶法制备的TiO2纳米粒子为载体,通过浸渍法制备了Au/TiO2样品,并利用XPS和SPS等技术对样品进行表征,考察了热处理温度和Au含量对TiO2纳米粒子光催化氧化苯酚活性的影响. 结果表明,Au是以金属纳米微晶的形式均匀地分散在TiO2纳米粒子表面. 用适量Au进行表面修饰不仅拓宽了TiO2对光的响应范围,而且改善了TiO2光生电子和空穴的分离效率,提高了样品对氧物种的吸附,并促进了光生电子向吸附氧的传输. 在光催化氧化苯酚反应中,500 ℃处理的Au/TiO2纳米粒子具有较高的光催化活性,这与XPS和SPS表征结果是一致的. 从电子能级匹配的角度揭示了Au对TiO2样品表面光电性质和光催化性能的影响机制.  相似文献   

7.
方奕文  余林  叶飞  孙明 《分子催化》2011,25(6):569-573
用溶胶-凝胶法制备Ag改性的TiO2催化剂,并用XRD、SEM、BET、O2-TPD和UV-Vis DRS等测试手段对其进行表征.结果表明,与TiO2相比,所制备催化剂颗粒直径明显减小,比表面积明显增大,对可见光的吸收明显增强,同时出现了表面吸附氧和Ag电子捕获中心.甲苯气相光催化降解结果显示,当Ag与Ti的摩尔比(n...  相似文献   

8.
传统的Ti O2半导体光催化剂存在光谱响应范围窄、量子效率低及不易回收等不足,使其在实际应用中受到限制.通过离子掺杂、贵金属沉积和半导体复合等方法对Ti O2进行改性可以拓展其光响应范围,其中半导体复合方法最为常用.复合半导体的特殊能带结构能够有效促进光生载流子的界面迁移,实现光生电荷的有效分离,提高光催化性能,且通过固定化或负载可改善Ti O2的可回收利用性能.鉴于此,本文针对半导体Ti O2的复合和负载制备及其光催化降解有机污染物的性能和反应机理进行了研究.采用条件温和、稳定的溶胶-凝胶法于低温制备出Ti O2/海泡石复合物,通过浸渍和焙烧将Ag2O负载于其上,修饰和拓展了Ti O2的可见光响应范围,最终获得了可见光响应、高效、稳定的Ag2O-Ti O2/海泡石复合光催化剂.利用X射线衍射(XRD)、X射线光电子能谱(XPS)、扫描电镜(SEM)、透射电镜(TEM)、N2吸附-脱附和紫外-可见光光谱(UV-vis)等手段对其物理化学特性进行了表征.XRD结果表明,复合样品中Ti O2呈锐钛矿相和金红石相的混合晶相.TEM结果表明,复合样品中存在Ag2O和Ti O2两种组分,晶格条纹相互交叠形成了异质结结构.UV-vis谱表明,与Ti O2/海泡石相比,Ag2O-Ti O2/海泡石复合光催化剂的吸收带边明显红移,展现了较强的可见光吸收能力.N2吸附-脱附结果表明,Ag2O-Ti O2/海泡石复合光催化剂具有较大的比表面积和介孔结构,这有助于增强催化剂对污染物的吸附能力并提供更多的复合位点.以酸性红G为模拟污染废水,研究了焙烧温度和Ag2O负载量等制备条件对所制催化剂可见光催化性能的影响.结果表明,在可见光照射下,焙烧温度为200°C,Ag2O负载量为10%条件下制备的复合光催化剂对酸性红G的降解率为98%,与Ag2O-Ti O2、Ag2O/海泡石和Ti O2/海泡石等复合物相比,Ag2O-Ti O2/海泡石复合光催化剂展现了优异的可见光催化性能.此外,Ag2O-Ti O2/海泡石复合光催化剂同样能够在可见光条件下有效降解常见室内空气污染物甲醛,进一步证实了催化剂优异的光催化性能.化学荧光法和活性物种捕获实验表明,复合光催化剂降解有机污染物的活性基团主要是光生空穴和超氧自由基.催化剂能带结构分析表明,Ag2O和Ti O2具有相匹配的能带结构,两者复合有利于光生载流子分离和迁移,增强催化剂光催化活性.海泡石作为光催化剂载体能够有效固载光催化成分,增加光催化剂有效表面积和活性位,有利于提高复合光催化剂的吸附性能和回收利用率.  相似文献   

9.
为了改善染料敏化太阳电池内电子的传输复合过程,研究者尝试不同方法制备或改性TiO2薄膜.不同烧结气氛可以改变TiO2薄膜的表面特性,是一种有效的方法并被广泛研究.采用两步烧结法制备氧气氛烧结TiO2电极并应用于染料敏化太阳电池:第一步将电极在空气或氧气氛中510℃保温30 min以清除TiO2薄膜中有机物;第二步将电极进一步在氮气氛中510℃保温10 min以移除电极表面吸附的多余氧原子.通过与空气烧结电池宏观性能及微观性能的对比,细致研究了氧气氛烧结电极表面特性对染料敏化太阳电池传输复合微观动力学过程的影响机制.TiO2薄膜表面特性及带边移动、电子传输复合过程的表征分别借助XPS能谱仪和强度调制光电流谱(IMPS)/强度调制光电压谱(IMVS)等探测技术完成.结果表明,氧气烧结电极Ti3+复合中心减少,使电池内部电子复合得到有效抑制.同时,氧气烧结电极染料吸附量增加且导带边正移,使得光生电子浓度升高,膜内电子传输过程加快.最终,氧气烧结电极有效改善了电池光吸收效率、电子收集效率以及注入效率,使电池效率由6.90%提升至7.53%.  相似文献   

10.
微波载银对纳米二氧化钛相变及光催化性能的增效作用   总被引:4,自引:1,他引:3  
用微波法制备系列载Ag纳米TiO2,发现微波载Ag对纳米TiO2的相变和光催化活性具有增效作用。采用X-射线粉末衍射(XRD),透射电镜(TEM),X-射线光电子能谱仪(XPS),激光Raman光谱及漫反射光谱(DRS)方法对比研究纳米TiO2与载Ag纳米TiO2的性质。结果表明,所制得载Ag纳米TiO2是以锐钛矿为主相的混晶,平均粒径约为10 nm,负载Ag促进纳米TiO2中锐钛矿相转化金红石相相变,减小纳米晶尺寸,并使纳米TiO2光响应范围向可见光区移动 6 nm。在低浓度范围,微波法能均匀地将Ag负载于纳米TiO2表面,并以Ag0/Ag+的形式存在,抑制光生电子与光生空穴复合,大大地提高了纳米TiO2光催化活性。在近紫外-可见光照射下,载Ag量为0.05 mol %的纳米TiO2对罗丹明B的光催化降解效果最好。  相似文献   

11.
金属离子的光催化去除研究进展   总被引:12,自引:0,他引:12  
刘守新  孙承林 《化学通报》2004,67(12):898-903
利用光催化剂表面的光生电子或空穴等活性物种,通过还原或氧化反应去除水相中的金属离子,是与环境保护、贵金属回收或金属担载催化剂制备相关的重要过程。笔者结合半导体的结构特征,综述了利用光催化还原反应或氧化反应,对铬、汞、铜、镍、银及铂、钯等贵金属和锰、铀等的光催化去除效果,介绍了该技术在处理金属离子混合体系实现金属分离过程的应用。结合有关实验数据,对一些可能反应机制进行了探讨。对与环境保护及其它相关工艺过程的应用进行了介绍。  相似文献   

12.
Ag/TiO2对含酚废水的光电催化降解   总被引:5,自引:0,他引:5  
Ag/TiO2对含酚废水的光电催化降解;Ag/TiO2; 光电催化; 苯酚;电解质  相似文献   

13.
The effects of a room temperature ionic liquid, 1-butyl-3-methylimidazolium terafluoroborate ([Bmim]BF4), on the photocatalytic performance of Degussa P25 TiO2 were investigated. Also, the photocatalysis mechanism was systematically analyzed by conducting different reactive radical trapping experiments. The results showed that photogenerated electrons were the main reactive species involved in the photocatalytic degradation of methyl orange (MO), while ?OH radicals and photogenerated holes played an important role in the photocatalytic decomposition of rhodamine B (RhB). The addition of ionic liquid (IL) could slightly enhance the photocatalytic degradation rate of MO because adsorption of [Bmim]+ ions on the TiO2 surface not only enhanced traping and transfer of photogenerated electrons, but also facilitated adsorption of negatively charged MO. On the contrary, IL suppressed the degradation rate of RhB because [Bmim]+ on the TiO2 surface not only hindered the access of positively charged RhB to TiO2, but also restricted the diffusion of positively charged holes to the TiO2/solution interface.  相似文献   

14.
采用化学沉淀法合成了一系列Mg-ZnO光催化剂. 研究了在Mg 2+和MgO绝缘介质共同作用下Mg-ZnO光催化剂的活性. 结果表明, 紫外光照射5 min后, 10%Mg-ZnO复合物对10 mg/L RhB的降解率达到81.3%, 光降解速率常数为0.3271 min -1, 是纯ZnO的3.42倍. 瞬态光电压(TPV)、 接触电势差、 表面光电流(SPC)和Cr(Ⅵ)还原等实验结果表明, MgO绝缘颗粒的形成抑制了ZnO中光生电子的“逆向”传输, 使电子和空穴的复合时间延长, 从而间接提高了光生空穴的利用率.  相似文献   

15.
The recent discovery of Ag@AgX (X=Cl, Br, I) plasmonic photocatalysts motivates us to elucidate the origin of the higher photocatalytic performance compared to commonly used TiO2‐based materials. Herein, the electronic structure and effective masses of electrons at the conduction band minimum (CBM) and holes at the valence band maximum (VBM) are studied along different directions in the silver halide for the first time by means of first‐principles calculations. It is revealed that the smaller effective mass of electrons at the CBM in silver halides contributes to the higher photocatalytic performance. The remarkable dependence of the effective mass of holes on the direction and the anion of the silver halide explains well the experimental observed morphology and anion dependence of photocatalytic activities of Ag@AgX. The crystal field splitting of the Ag 4d bands in the valance band of silver halides is found to be a main factor leading to the large effective mass of the photogenerated holes and consequently to a weaker transfer ability. A new crystal design and exerting strain along the coordinate axis are proposed as solutions to decrease the effective mass of holes. The present work may be helpful in exploring this novel class of silver halide‐based photocatalysts.  相似文献   

16.
采用瞬态光电导谱研究了TiO2的光电导衰减曲线,通过计算机拟合得到光生载流子的寿命,并考察了Pt的负载量对TiO2光生载流子有效寿命的影响。结果表明,增大Pt的负载量,可延缓光电导的衰减趋势,从而延长TiO2光生载流子的有效寿命,有效地降低了光生载流子的复合率。  相似文献   

17.
Porous ZnO nanorods that displayed excellent photocatalytic degradation of organic pollutants (RhB and phenol) were prepared via a solvent thermal method followed by surface modification with carbon dots (C-dots) using a deposition method. The photocatalysts were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and ultraviolet-visible (UV-Vis) spectroscopy. The degradation of the organic pollutants using the nanorods was tested under Xe-light illumination and was enhanced following C-dot modification. Nanorods that were modified by the C-dots at a mass fraction of 1.2% (CZn1.2) exhibited the highest photocatalytic activity for the degradation of RhB, which was 2.5 times of the pure porous ZnO nanorods. Additionally, the modified nanorods with strangely oxidation ability could catalyze the degradation of phenol by open-rings reaction under Xe-light illumination. The improved photocatalytic activity was attributed to the effective separation of the photogenerated electrons and holes, in which the C-dots served as the receptor of the photogenerated electrons.  相似文献   

18.
Fluorescent carbon nanoparticles (FCNPs) have broad application prospects in the fields of bioimaging, ion detection, and photocatalysis. In this paper, coal-based FCNPs were prepared by using mixed acid oxidation, hydrogen peroxide etching, and organic solvent extraction methods (marked as FCNPs-AO, FCNPs-HE, and FCNPs-OS, respectively), and the structures and properties of the as-prepared products were compared. It was found that the coal-based FCNPs obtained by three kinds of methods are all aromatic structural nanomaterials linked with oxygen-containing groups. Among them, FCNPs-AO is a kind of hollow annular spherical particles and FCNPs-HE and FCNPs-OS are solid spherical particles. These FCNPs not only have similar fluorescence properties as traditional quantum dots, but also can be photoexcited to generate photogenerated electrons and holes, and it can also suppress the recombination of photogenerated electrons and holes by using its own surface defects. In particular, the electron transport capability of the FCNPs-AO is stronger than that of FCNPs-HE and FCNPs-OS because of its lower charge transfer impedance, so it can be excited to generate more photogenerated electrons and has the best photogenerated carrier separation efficiency.  相似文献   

19.
Recently, it has been proven that directional flow of photogenerated charge carriers occurs on specific facets of TiO2 nanocrystals. Herein, we demonstrate that the photocatalytic activity of anatase TiO2 nanocrystals in both photoreduction and photooxidation processes can be enhanced by selectively depositing Pt nanoparticles on the {101} facets, which strengthens spontaneously surface‐induced separation between photogenerated electrons and holes in the photocatalysis process. An optimal ratio of the oxidative {001} facets to the reductive {101} facets exists with regard to the photocatalysis of the faceted TiO2 nanocrystals, and this is crucial for balancing the recombination and redox reaction rates of photogenerated electrons and holes. The present work might help us gain deeper insight into the relation between the specific surface of semiconductor photocatalysts and their photocatalytic activities and provides us with a new route to design photocatalysts with high photocatalytic activity.  相似文献   

20.
Pyrroloquinoline quinone (PQQ) forms a tridentate complex with coordinatively unsaturated titanium atoms on the surface of approximately 4.5 nm TiO2 particles; an association constant of K = 550 M-1 per Ti(IV)surf has been determined. Low-temperature electron paramagnetic resonance was employed in identification of localized charges and consequently produced radicals and in determination of charge-transfer processes. The photoexcitation of the PQQ-TiO2 complex results in the transfer of conduction band electrons from TiO2 to bound PQQ and the formation of the semiquinone radical. Attaching dopamine (DA) as an electron donor and PQQ as an electron acceptor on the surface of TiO2 results in spatial separation of photogenerated charges; the holes localize on dopamine and electrons on PQQ, with higher yields than for each component separately. In this triad-type assembly (PQQ-TiO2/DA) the PQQ that is bound to the particles acts as a sink for electrons allowing their almost complete scavenging even at temperature as low as 4 K.  相似文献   

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