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1.
采用sol-gel法制备了纯的和掺杂不同量Ce的TiO_2纳米粒子,并利用XRD, TEM,BET,XPS和PL光谱对样品进行表征,主要考察焙烧温度和含量对掺杂Ce的 TiO_2纳米粒子性质以及光催化降解苯酚活性的影响,并探讨了Ce的掺杂对TiO_2相 变的作用机制以及PL光谱与光催化活性的关系,结果表明,掺杂的Ce~(4+)没有进 入到TiO_2晶格中,而是以小团簇的CeO_2化学态均匀地弥散在TiO_2纳米粒子中, 这可能导致了Ce的掺杂对TiO_2的相变有很大的抑制作用;Ce的掺杂没有引起新的 光致发光现象,而适量Ce的掺杂能够降低TiO_2纳米粒子PL光谱的强度,这是因为 掺杂的Ce~(4+)易于捕获光生电子而生成Ce~(3+);600℃处理的掺杂Ce的TiO_2纳米 粒子表现出较高的光催化活性,这说明600℃是比较合适的焙烧温度,而掺杂不同 量的Ce的TiO_2样品的光催化活性顺序是:3 mol%>4 mol%>2 mol%>5 mol%>1 mol%>0 mol%,这与它们的PL光谱强度的顺序是相反的,即PL光谱强度越低,其 光催化活性越高,这说明PL光谱与其光催化活性间有着必然的联系,这是因为掺杂 剂Ce~(4+)能够捕获光生电子,在光致发光过程中使PL光谱强度下降,而在光催化 反应过程中使有机污染物加快氧化。  相似文献   

2.
掺杂镧的TiO2纳米粒子的光致发光及其光催化性能   总被引:22,自引:5,他引:17  
采用溶胶-凝胶法制备了纯的和掺杂La的TiO2纳米粒子,并利用XRD,TEM,XPS和荧光光谱(FS)等对样品进行表征,主要考察焙烧温度和La含量对TiO2纳米粒子的性质以及光催化降解苯酚活性的影响,并探讨了La的掺杂对TiO2相变的作用机制以及FS光谱与光催化活性的关系.结果表明,适量La掺杂能够提高TiO2纳米粒子FS光谱强度,这是因为La掺杂能够使表面氧空位和缺陷的浓度增加;600℃热处理的掺杂不同量La的TiO2样品的光催化活性顺序是:1%>1.5%>3%>0.5%>5%>0%,这与它们的FS光谱强度的顺序是一致的,即FS光谱强度越高,其光催化活性越高.这是因为在光致发光过程中,FS信号主要来源于表面氧空位和缺陷,而在光催化反应过程中,表面氧空位和缺陷能够有利于光生电子被捕获.  相似文献   

3.
低量Tm掺杂TiO_2纳米粉体的光致发光特性及光活性   总被引:1,自引:0,他引:1  
利用溶胶-凝胶法制备了不同掺杂量及不同温度焙烧的Tm掺杂TiO2纳米粉体。采用X射线衍射(XRD),紫外-可见漫反射谱(DRS)和光致发光光谱(PL)技术研究了Tm掺杂量和焙烧温度对其相结构、晶粒尺寸、光吸收及光致发光性能的影响;并以亚甲基蓝(MB)溶液的光催化降解评价其光活性。结果表明:低量Tm掺杂强烈抑制TiO2由锐钛矿相向金红石相转变,减小晶粒尺寸;然而,Tm掺杂量增加,抑制相变作用减弱。Tm掺杂导致样品的紫外吸收能力略有降低,光吸收带边蓝移。Tm掺杂导致样品的PL谱强度降低(0.05%0.075%0.025%≈0.1%0%),光活性升高(0.075%0.05%0.1%0.025%0%),但二者顺序并不完全一致。低量Tm掺杂能有效提高纳米TiO2的光活性;当Tm掺杂量为0.075%(质量分数)、焙烧温度为550℃时,制得样品呈双相结构,锐钛矿相占91%,晶粒尺寸为24.48 nm,其光活性最佳。光活性提高的主要根源是Tm掺杂能有效促进纳米TiO2表面光生e-/h+分离,提高量子化效率。  相似文献   

4.
掺杂Cu的TiO2纳米粒子的制备、表征及其光催化活性   总被引:12,自引:0,他引:12  
采用Sol-gel法制备了纯的和掺杂不同量Cu的TiO2纳米粒子,并用TG-DTA,XRD,XPS,UV-Vis和荧光光谱对样品进行了表征,考察焙烧温度和Cu含量对TiO2纳米粒子的性质及光催化活性的影响,初步探讨了Cu的掺杂对TiO2相变的作用机制及样品荧光光谱与光催化活性的关系.结果表明,Cu2+的掺杂对TiO2的相变有很大的促进作用,并使其光谱响应范围向可见光区拓展.Cu的掺杂未引起新的荧光现象,但适量Cu的掺杂能够降低TiO2纳米粒子的荧光强度.此外,在光催化降解苯酚的实验中,于500℃处理的掺杂Cu的TiO2纳米粒子的光催化活性较高,与表征结果一致.而掺杂不同量Cu的TiO2的光催化活性顺序与样品荧光光谱强度的顺序相反,即荧光光谱强度越低,其光催化活性越高.  相似文献   

5.
随着工业化的快速发展,化石燃料等不可再生能源的快速消耗,人类将面临不可预测的能源危机.寻找有效的方法来解决能源短缺问题已成为当今的重要研究课题.氢能是一种可以替代化石燃料的清洁可再生能源.利用半导体光催化分解水制氢技术可以将太阳能转化为氢能.目前,在已开发的半导体光催化材料中, TiO_2因具有无毒、稳定、廉价等优点而备受光催化领域关注.但是,在实际应用方面, TiO_2的光催化效率受限于其低的光子利用率和较高的光生电子-空穴复合率.许多研究表明, TiO_2不同晶面的协同作用有利于光生载流子的迁移分离,并且适量的掺杂能够捕获光生电子,从而抑制其复合.而镧系元素因其特殊4f电子结构受到广泛的关注.采用物理或化学方法将镧系离子引入TiO_2晶格中,可以影响光生电子和空穴的动力学过程,延长光生载流子的分离状态,从而提高光催化活性.本文通过简单溶剂热法成功合成了镧系离子掺杂{001}/{101}面共暴露的TiO_2纳米片.X-射线粉末衍射(XRD)、X-射线光电子能谱(XPS)和高分辨透射电子显微镜(HRTEM)的表征结果证明了镧系离子选择性掺杂在TiO_2纳米片{101}面上.结合紫外可见吸收光谱、稳态荧光、瞬态荧光衰减曲线、光电流及莫特-肖特基曲线等手段对镧系离子掺杂TiO_2光催化剂进行了表征,结果表明,镧系离子掺杂TiO_2纳米片增强了对光的吸收,同时延长光生载流子的分离状态,阻碍光生电子和空穴的复合.考察其光催化分解水制氢的性能.研究表明,在相同掺杂量(0.5 mol%RE~(3+)=Ho~(3+), Er~(3+), Tm~(3+), Yb~(3+), Lu~(3+))的TiO_2纳米片中, Yb~(3+)-TiO_2纳米片光催化剂具有优异的产氢活性,在模拟太阳光照射1 h后产氢量是纯TiO_2的4.25倍.同时讨论了不同浓度助催化剂Pt作用下的Yb~(3+)-TiO_2纳米片产氢效果,当Pt含量量为0.3wt%时,光解水产氢活性最佳, Pt/Yb~(3+)-TiO_2纳米片的产氢量是Yb~(3+)-TiO_2的2倍,纯TiO_2的8.5倍.光催化分解水产氢活性的显著提高可以归因于光生电子-空穴对在TiO_2纳米片{001}/{101}面的快速分离,以及镧系离子4f电子轨道对电子的捕获和杂质能级的产生减小了禁带宽度,这不仅延长了光生载流子的分离状态,增加了H~+还原成H_2的机会,而且还可以拓展可见光的吸收范围.可见,利用镧系离子掺杂TiO_2和共暴露{001}/{101}面协同作用是一种实现TiO_2基光催化活性提高的有效方法之一.镧系离子掺杂的策略对提高半导体纳米材料的光催化活性有显著的影响,可能在光催化、光电化学和太阳能电池领域有更广泛的应用.  相似文献   

6.
以电纺TiO_2纳米纤维为基质,利用水热法制备了异质结型Eu~(3+)掺杂NaBi(MoO_4)_2/TiO_2复合纤维。利用X射线衍射(XRD)、扫描电子显微镜(SEM)、 X射线光电子能谱(XPS)、高分辨透射电镜(TEM)、紫外-可见漫反射(UV-Vis DRS)光谱以及荧光(PL)光谱等分析测试手段对样品的物相、形貌和光学性能等进行表征。以三乙醇胺为电子给体,研究了Eu~(3+)掺杂NaBi(MoO_4)_2/TiO_2复合纤维光催化裂解水制氢的反应过程。结果表明:NaBi(MoO_4)_2与TiO_2复合形成异质结,使光生电子-空穴对得到较好分离,而Eu~(3+)掺杂进入NaBi(MoO_4)_2晶格,部分取代Bi~(3+)离子,导致晶胞膨胀,在拓宽光谱响应范围的同时,形成光生载流子的浅势捕获阱,进一步促进了光生电荷的产生、转移,有效提高材料的光催化制氢活性。最佳产氢速率达到7.86 mmol·h~(-1)·g~(-1)。  相似文献   

7.
铈掺杂WO3的表征及其光解水催化性能的研究   总被引:3,自引:0,他引:3  
采用固相烧结法制备了掺杂不同量铈的WO3催化材料,并用XRD,XPS,DRS和PL光谱对样品进行了表征,主要考察了铈含量和焙烧温度对WO3的性质及光催化分解水制氧活性的影响,初步探讨了样品的PL光谱与其光催化分解水制氧活性的关系。结果表明,铈的掺杂可以使WO3的光谱响应范围向可见光区拓展。铈的掺杂没有引发新的荧光现象,适量铈的掺杂能够增强催化剂样品的荧光强度。在可见光辐射下进行光催化分解水制氧,于600 ℃处理的掺杂铈为0.05%(wt)的WO3催化剂的催化活性最高,此时催化剂的析氧速率比未掺杂WO3提高了1.5~1.7倍。研究表明,样品的光催化活性与其PL信号强度顺序一致,即PL信号越强,光催化活性越高。  相似文献   

8.
以Ba(NO_3)_2、NaBH_4、Er_2O_3和CeO_2为原料,在十六烷基三甲基溴化铵(CTAB)表面活性剂辅助下,采用水热法制备了β-BaB_2O_4(β-BBO)纳米棒,稀土离子Er~(3+)单掺杂的β-BBO(β-BBO:Er~(3+))及Er~(3+)和Ce~(3+)/Ce~(4+)共掺杂的β-BBO(β-BBO:Er(3+)/Ce~(3+)/Ce~(4+))纳米棒.通过X射线粉末衍射(XRD)、傅里叶变换红外(FTIR)光谱、拉曼光谱、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)和光致发光(PL)光谱分别对样品的物相、结构、形貌、成分及光致发光性质进行了表征.研究结果表明:微量稀土离子掺杂并不改变β-BBO的结构,制得的纳米棒尺寸均匀,长度在200-500 nm之间,直径在10-20 nm之间;β-BBO:Er~(3+)和β-BBO:Er~(3+)/Ce~(3+)Ce~(4+)纳米棒在400nm光激发下,在可见光范围内都观察到中心波长为515和542 nm的绿光.对发光机理的初步研究表明:发光分别对应于Er~(3+)的~2H_(11/2)→~4I_(15/2),~4S_(3/2)→~4I_(15/2)跃迁,铈离子以Ce~(3+)和Ce~(4+)两种形式存在于体系中,Ce~(3+)对Er~(3+)起敏化作用,可以显著增强β-BBO:Er~(3+)/Ce~(3+)/Ce~(4+)纳米棒的发光强度,存在Ce~(3+)→Er~(3+)的能量传递过程.  相似文献   

9.
采用沉淀法制备了ZnO纳米粒子, 并利用XPS, SPS, ESR和PL等测试技术对样品进行了表征, 同时评估了样品在光催化氧化气相n-C7H16中的活性. 重点考察了ZnO纳米粒子的表面组成和结构与其光致发光和光催化性能的关系. 结果表明: ZnO纳米粒子的粒子尺寸越小, 表面氧空位的量越大, 光致发光信号越强, 光催化活性越高. 说明它们之间必然存在一定的关系, 这是因为光致发光信号主要归属于表面氧空位引发的自由和束缚激子发光, 而表面氧空位由于易于捕获光生电子, 且与吸附氧间存在强烈的相互作用, 以至于有利于氧化反应的进行. 此外, 也说明了ZnO纳米粒子的表面态是非常丰富的, 主要是由氧空位和氧物种等引起的.  相似文献   

10.
Fe~(3+)掺杂的TiO_2纳米复合粒子的合成及表征   总被引:24,自引:2,他引:24  
苏碧桃  张彰  郑坚  苏致兴 《化学学报》2002,60(11):1936-1940
利用酸催化的溶胶-凝胶法合成了一系列不同Fe~(3+)掺杂量的TiO_2纳米复合 料子。用XRD,TEM,UV-vis等技术进行了表征。结果表明:在所研究的掺杂量范围 内(x_B = 0.0005 ~0.1000),未发现有铁氧化物的晶相生成;Fe~(3+)的掺杂可以 实现TiO_2由锐钛矿(anatase)结构向金红石(rutile)结构的低温转化,随着Fe~ (3+)掺杂量的增大,对光的吸收发生红移,吸收强度增大。掺杂适量的Fe~(3+)可 以使TiO_2纳米微粒的光催化活性得以提高。  相似文献   

11.
In this paper, pure and La doped TiO2 nanoparticles with different La content were prepared by a sol-gel process using Ti (OC4H9)4 as raw material, and also were characterized by XRD, TG-DTA, TEM, XPS, DRS and Photoluminescence (PL) spectra. We mainly investigated the effects of calcining temperature and La content on the properties and the photocatalytic activity for degrading phenol of as-prepared TiO2 samples, and also discussed the relationships between PL spectra and photocatalytic activity as well as the mechanisms of La doping on TiO2 phase transformation. The results showed that La3+ did not enter into the crystal lattices of TiO2 and was uniformly dispersed onto TiO2 as the form of La2O3 particles with small size, which possibly made La dopant have a great inhibition on TiO2 phase transformation; La dopant did not give rise to a new PL signal, but it could improve the intensity of PL spectra with a appropriate La content, which was possibly attributed to the increase in the content of surface oxygen vacancies and defects after doping La; La doped TiO2 nanoparticles calcined at 600°C exhibited higher photocatalytic activity, indicating that 600°C was an appropriate calcination temperature. The order of photocatalytic activity of La doped TiO2 samples with different La content was as following: 1>1.5>3>0.5>5>0 mol%, which was the same as the order of their PL intensity, namely, the stronger the PL intensity, the higher the photocatalytic activity, demonstrating that there were certain relationships between PL spectra and photocatalytic activity. This could be explained by the points that PL spectra mainly resulted from surface oxygen vacancies and defects during the process of PL, while surface oxygen vacancies and defects could be favorable in capturing the photoinduced electrons during the process of photocatalytic reactions.  相似文献   

12.
掺Sn的纳米TiO2表面光致电荷分离及光催化活性   总被引:7,自引:0,他引:7  
采用溶胶-凝胶法制备了不同掺Sn量的TiO2纳米粒子, 主要利用表面光电压谱(SPS)和光致发光光谱(PL)对样品进行了表征, 并通过光催化降解苯酚实验来评估样品活性. 重点考察了热处理温度和掺Sn量对样品表面光生载流子的分离及光催化活性的影响, 并探讨了Sn使TiO2纳米粒子改性的机制. 结果表明, 在适当温度处理下, 适量Sn的掺入能够有效促进TiO2纳米粒子表面光生载流子的分离, 以至于使其光催化活性得到显著提高.  相似文献   

13.
In recent years, nanosized TiO2 materials have been widely studied in photocatalytic and photoelectric conversion fields because of their intrinsic characteris- tics, such as stable chemical property, strong oxidizing capability and nontoxicity[1,2]. And the preparation, characterization and modification of nanosized TiO2 are always crucial contents in semiconductor photo- electric chemistry and photocatalytic researches[3,4]. To further improve TiO2 performance, doping metal ion is consider…  相似文献   

14.
ZnO和TiO2纳米粒子的光致发光性能及其与光催化活性的关系   总被引:17,自引:2,他引:15  
采用沉淀法和溶胶-凝胶法制备了ZnO和TiO2及掺Zn2+的TiO2纳米粒子,用XRD和荧光光谱(FS)等手段对样品进行了表征,重点探讨了样品光致发光机制及与光催化活性的关系.结果表明,ZnO和TiO2样品在大于带隙能的光激发下均表现出明显的FS信号,热处理温度升高,FS信号强度下降,并且二者的FS信号类似,这可能与二者具有类似的电子能带结构有关,同时也说明FS信号主要源于表面氧空位以及吸附氧物种等引起的激子或表面态能级.掺杂Zn2+使TiO2纳米粒子FS信号增强,这主要与表面氧空位和缺陷等量增加有关;此外,在光催化氧化苯酚实验中,样品光催化活性与其FS信号强度顺序一致,即FS信号越强,活性越高.这是由于在光致发光过程中,FS信号主要源于表面氧空位,而在光催化反应中,表面氧空位有利于氧化反应进行.  相似文献   

15.
In this paper, TiO(2) nanoparticles doped with different amounts of Zn were prepared by a sol-gel method and were mainly characterized by means of X-ray photoelectron spectroscopy (XPS), photoluminescence (PL), and surface photovoltage spectrum (SPS). The effects of surface oxygen vacancies (SOVs) of Zn-doped TiO(2) nanoparticles on photophysical and photocatalytic processes were investigated along with their inherent relationships. The results show that the SOVs easily bind photoinduced electrons to further give rise to PL signals. The SOVs can result in an interesting sub-band SPS response near the band edge in the TiO(2) sample consisting of much anatase and little rutile, except for an obvious band-to-band SPS response. Moreover, the intensities of PL and SPS signals of TiO(2), as well as the photocatalytic activity for degrading phenol solution, can be enhanced by doping an appropriate amount of Zn. These improvements are mainly attributed to the increase in the SOV amount. It can be suggested that the SOVs should play an important role during the processes of PL, surface photovoltage, and photocatalytic reactions, and, for the as-prepared TiO(2) samples doped with different amounts of Zn by thermal treatment at 550 degrees C, the larger the SOV amount, the stronger the PL and SPS signal, and the higher the photocatalytic activity.  相似文献   

16.
In this study, TiO(2)- and Mg-doped TiO(2) nanoparticles with different dopant contents were prepared by sol-gel method. The prepared photocatalysts were characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Brunauer-Emmett-Teller (BET) and diffuse reflectance spectroscopy (DRS) techniques. The results of BET analysis indicated a pore diameter of 8 nm and surface area of 48.5 m(2) g(-1). XRD patterns of pure and doped TiO(2) nanoparticles at 450 °C revealed that all phases are anatase. The particle size obtained from TEM was less than 20 nm. The band gap energy of Mg-doped TiO(2) nanoparticles was lower than that of TiO(2) . The photocatalytic activity of the pure and doped nanoparticles has been compared in the removal of C.I. Acid Red 27 (AR27). The photocatalytic activity of Mg-doped (0.2 mol%) TiO(2) for the degradation of AR27 was higher than that of bare TiO(2) nanoparticles. Results of total organic carbon analysis and changes in the AR27 UV-Vis peaks indicated 99% mineralization and extinguishing of all peaks in UV and visible regions is possible with Mg-doped TiO(2) nanoparticles. Removal efficiency of AR27 was sensitive to the parameters such as catalyst dose, pollutant concentration and light intensity.  相似文献   

17.
以Ba(NO3)2、NaBH4、Er2O3和CeO2为原料, 在十六烷基三甲基溴化铵(CTAB)表面活性剂辅助下, 采用水热法制备了β-BaB2O4 (β-BBO)纳米棒, 稀土离子Er3+单掺杂的β-BBO(β-BBO:Er3+)及Er3+和Ce3+/Ce4+共掺杂的β-BBO(β-BBO:Er3+/Ce3+/Ce4+)纳米棒. 通过X射线粉末衍射(XRD)、傅里叶变换红外(FTIR)光谱、拉曼光谱、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)和光致发光(PL)光谱分别对样品的物相、结构、形貌、成分及光致发光性质进行了表征. 研究结果表明: 微量稀土离子掺杂并不改变β-BBO的结构, 制得的纳米棒尺寸均匀, 长度在200-500 nm 之间, 直径在10-20 nm 之间; β-BBO:Er3+和β-BBO:Er3+/Ce3+/Ce4+纳米棒在400nm光激发下, 在可见光范围内都观察到中心波长为515和542 nm的绿光. 对发光机理的初步研究表明: 发光分别对应于Er3+的2H11/2→4I15/2, 4S3/2→4I15/2跃迁, 铈离子以Ce3+和Ce4+两种形式存在于体系中, Ce3+对Er3+起敏化作用, 可以显著增强β-BBO:Er3+/Ce3+/Ce4+纳米棒的发光强度, 存在Ce3+→Er3+的能量传递过程.  相似文献   

18.
The pure, 1 mol% only La or only Cu doped TiO2 and La and Cu codoped TiO2 were prepared by a sol-gel process. The effects of doping on photoinduced charge properties of nanosized TiO2 were mainly investigated by means of Surface Photovoltage Spectrum (SPS) and Photoluminescence Spectrum (PL), together with their relationships with photocatalytic activity. The results show that La dopant can inhibit the phase transformation of TiO2, meanwhile improve the separation rate of photoinduced charge carriers, and enrich the binding surface states. However, Cu dopant has a reverse effect compared to La dopant. This is responsible for the results that doping La is favorable for the increase in the photocatalytic activity for degrading the RhB solution, while doping Cu is bad to photocatalyitc reaction. In addition, codoping La and Cu cannot exhibit an obvious combination effect.  相似文献   

19.
Lanthanum trivalent ions (La(3+)) doped titanium dioxide (TiO(2)) nanopowders in the range of 20-60 nm were prepared successfully by plasma spray in the self-developed plasma spray equipment. The photocatalytic activity of samples at different doping concentrations in photocatalytic degradation of methyl orange was discussed. The nanopowders prepared were characterized by transmission electron microscopy, X-ray diffraction, ultraviolet-visible spectra, photoluminescence (PL) and X-ray photoelectron spectroscopy. The results show that La(3+) doping increased the photocatalytic activity of TiO(2) greatly, the optimal doping concentration was 0.5 at%. The La(3+) doping decreases the particle size and the distribution of particle sizes becomes more uniform. The doped powders were the mixture of anatase and rutile phase. The contents of anatase phase decreased firstly and then increased with an increase in the contents of La(3+). The intrinsic absorption band of La(3+) doped TiO(2) nanopowders appears red shift from that of pure TiO(2) nanopowders. The intensity of PL spectra increases and then decreases with increasing the content of La(3+). The PL spectral intensity reaches its peak when the ratio of La(3+)/TiO(2) is 0.2 at%. There are O, Ti, C and La elements in the prepared La(3+) doped TiO(2) nanopowders, La element still exists in trivalent and Ti element always exists in tetravalent.  相似文献   

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