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1.
以多层电解质作为微型反应器,制备了SiO2/ Polyelectrolyte(PE) / Bi2S3核壳纳米粒子。XRD结果表明Bi2S3颗粒属于正交晶系。由透射电镜和场发射扫描电镜照片可知,在直径为640 nm左右的SiO2表面覆盖了厚度35 nm的Bi2S3壳层。红外光谱分析结果表明硅烷网络在结构上发生了变化(SiO2表面的硅烷醇键沉积在Bi2S3的表面)。SiO2核和SiO2 / PE / Bi2S3的紫外-可见吸收光谱显示在900 nm存在典型吸收边。  相似文献   

2.
采用银修饰介孔磷钨酸/二氧化硅(mesoporous HPW/SiO2)催化剂,并研究了其在模拟柴油和真实柴油氧化脱硫反应中的催化性能。通过银修饰介孔HPW/SiO2,结合银离子对有机硫化物的选择吸附性和HPW对有机硫化物的催化氧化活性,以达到选择氧化脱硫的目的。模拟柴油分别采用石油醚、苯、1-辛烯和二苯并噻吩配制,当银离子与HPW的摩尔比为2时,催化剂具有最高的选择催化氧化活性。采用N2 吸附-脱附、XRD、UV-vis和EDS表征了银修饰的介孔HPW/SiO2催化剂,结果表明,银物种分散均匀且以Ag+形式存在。真实柴油的脱硫研究表明,相比介孔HPW/SiO2催化剂,修饰的催化剂介孔Ag2-HPW/SiO2脱硫率提高了4.6%,初始硫含量为1800×10-6的直馏柴油能被脱除至228×10-6,脱硫率为87.3%。介孔Ag2-HPW/SiO2催化剂具有良好的再生性能,经再生处理后,Ag的损失量极少,其三次脱硫率达到84.8%。  相似文献   

3.
Ag2S‐graphene/TiO2 composites were synthesized by a facile sonochemical method.The products were characterized by X‐ray diffraction,scanning electron microscopy,energy dispersive X‐ray spectroscopy,transmission electron microscopy,and UV‐Vis diffuse reflectance spectrophotometry.During the synthesis reaction,the reduction of graphene oxide and loading of Ag2S and TiO2 particles were achieved.The Ag2S‐graphene/TiO2 composites possessed a large adsorption capacity for dyes,an extended light absorption range,and efficient charge separation properties.Hence,in the photodegradation of rhodamine B,a significant enhancement in the reaction rate was observed with the Ag2S‐graphene/TiO2 composites as compared to pure TiO2.The generation of reactive oxygen species was detected by the oxidation of 1,5‐diphenyl carbazide to 1,5‐diphenyl carbazone.The high activity was attributed to the synergetic effects of high charge mobility and the red shift in the absorption edge of the Ag2S‐graphene/TiO2 composites.  相似文献   

4.
通过沉积法和离子交换法成功地制备了Ag_3PO_4/Ag_2S/g-C_3N_4复合型光催化剂。利用X射线多晶粉末衍射仪(XRD)、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)、N_2吸附-脱附等温线、紫外-可见漫反射光谱、荧光光谱等手段对样品进行了表征。通过降解罗丹明B考察其可见光催化活性及稳定性,研究了硫化钠与磷酸银物质的量的比值(n_(Na_2S)/n_(Ag_3PO_4))、g-C_3N_4添加量对所制备复合光催化材料性能的影响,同时对光催化机理进行了探讨。结果表明,随着n_(Na2S)/n_(Ag3PO4)的增加,所得复合催化材料活性先增加后降低;当n_(Na2S)/n_(Ag_3PO_4)为1.5%、g-C_3N_4与Ag_3PO_4的质量比为3∶7时制备的催化剂ASC1.5的光催化活性最好,在可见光照射下,40 min内可将罗丹明B完全降解,且5次循环使用后仍保持较高的催化活性。和Ag_3PO_4相比,Ag_3PO_4/Ag_2S/g-C_3N_4复合型光催化材料的活性与稳定性都得到明显提高,这主要归因于复合催化剂比表面积和孔结构的增加,载流子分离效率的提高。光催化机理研究表明,空穴(h~+)、超氧阴离子自由基(·O~(2-))和羟基自由基(·OH)都是光催化过程中的主要活性物种。三者作用大小依次为:h~+·O~(2-)·OH。  相似文献   

5.
Ag3PO4/Ag/Ag2Mo2O7 composite photocatalyst was successfully prepared via an in situ precipitation method. The as-prepared Ag3PO4/Ag/Ag2Mo2O7 nanocomposite included Ag3PO4 nanoparticles (NPs) as well as Ag NPs assembling on the surface of Ag2Mo2O7 nanowires. Under visible light irradiation (λ > 420 nm), the Ag3PO4/Ag/Ag2Mo2O7 composite degraded rhodamine B (Rh B) efficiently and showed much higher photocatalytic efficiency than pure Ag3PO4, Ag2Mo2O7, or Ag3PO4/Ag2Mo2O7. It was elucidated that the excellent photocatalytic performance of Ag3PO4/Ag/Ag2Mo2O7 for the degradation of Rh B under visible light could be ascribed to the high specific surface area, the extended absorption in the visible light region resulting from the Ag3PO4/Ag loading, and the efficient separation of photogenerated electrons and holes through the ternary heterostrucure composed of Ag3PO4, Ag and Ag2Mo2O7.  相似文献   

6.
The activity of 0.25–5% Ag/Al2O3 catalysts in the selective catalytic reduction of nitrogen oxides with n-hexane under the conditions of promotion with a small amount of H2 was studied. It was found that, upon the introduction of ∼1000 ppm of H2 into the reaction mixture, the Ag/Al2O3 samples containing 1–2% Ag exhibited optimum activity and selectivity. It was established that, in the presence of 1000 ppm of H2, the rate of the selective catalytic reduction of NO x was higher by a factor of 10–13, and the onset temperature of the reaction was lower by approximately 100°C. It was found by X-ray photoelectron spectroscopy, temperature-programmed reduction, and UV spectroscopy that the high activity of 1–2% Ag/Al2O3 catalysts was due to the presence of small Ag n δ+ and Ag m 0 clusters on their surface. A decrease in the concentration of Ag below the optimum value resulted in the predominance of an inactive ionic form on the catalyst surfaces. As the concentration of Ag was increased (>2%), large particles of Ag2O and Ag0, which facilitate the oxidation of n-C6H14, were formed to lead to a decrease in selectivity and in the degree of reduction of nitrogen oxides.  相似文献   

7.
采用电化学方法制备Ag2S/Ag3PO4/Ni复合薄膜,以扫描电子显微镜(SEM)、X射线衍射(XRD)、紫外-可见漫反射光谱(UV-Vis DRS)对薄膜的表面形貌、晶相结构、光谱特性及能带结构进行了表征,以罗丹明B为模拟污染物对薄膜的光催化活性和稳定性进行了测定,采用向溶液中加入活性物种捕获剂的方法对薄膜的光催化机理进行了探索。结果表明:最佳工艺制备的Ag2S/Ag3PO4/Ni是由均匀的球形纳米颗粒构成的薄膜,其光催化活性明显优于纯Ag3PO4/Ni薄膜和纯Ag2S/Ni薄膜,且在保持薄膜光催化活性基本不变的前提下可循环使用6次。提出了可见光下Ag2S/Ag3PO4/Ni复合薄膜光催化降解罗丹明B的反应机理。  相似文献   

8.
赵娣  张博  段召娟  李爱昌 《无机化学学报》2016,32(12):2158-2164
采用电化学方法制备Ag_2S/Ag_3PO_4/Ni复合薄膜,以扫描电子显微镜(SEM)、X射线衍射(XRD)、紫外-可见漫反射光谱(UVVis DRS)对薄膜的表面形貌、晶相结构、光谱特性及能带结构进行了表征,以罗丹明B为模拟污染物对薄膜的光催化活性和稳定性进行了测定,采用向溶液中加入活性物种捕获剂的方法对薄膜的光催化机理进行了探索。结果表明:最佳工艺制备的Ag_2S/Ag_3PO_4/Ni是由均匀的球形纳米颗粒构成的薄膜,其光催化活性明显优于纯Ag_3PO_4/Ni薄膜和纯Ag_2S/Ni薄膜,且在保持薄膜光催化活性基本不变的前提下可循环使用6次。提出了可见光下Ag_2S/Ag_3PO_4/Ni复合薄膜光催化降解罗丹明B的反应机理。  相似文献   

9.
陈熙  李莉  张文治  宋强  李奕萱 《无机化学学报》2015,31(10):1971-1980
在不同的制备条件下,通过微波水热两步法获得了一系列Ag2S/ZnO光催化剂,采用X射线粉末衍射(XRD)、X射线光电子能谱(XPS)、紫外-可见漫反射吸收光谱(UV-Vis/DRS)、扫描电子显微镜(SEM)和N2吸附-脱附等测试手段对产物结构和形貌进行了表征。结果表明,产物以六方纤锌矿ZnO为主,其晶型结构并未随着反应温度和Ag2S物质的量的增加而改变。Ag2S的引入显著增强了光催化剂在可见光区的吸收,使吸收边带发生红移,同时抑制了ZnO(001)晶面的生长。另外,所得产物的形貌随着Ag2S物质的量的增加从爆米花状转变为少量的柱体颗粒,且BET比表面积经过复合后明显减小。以罗丹明B为目标降解物,研究并比较了一系列Ag2S/ZnO光催化剂对罗丹明B的光降解性能。结果表明,nAg2S/nZnO=1:10时,光催化剂在紫外光、可见光和模拟日光的照射下具有最好的光催化效果,优于目前应用最广泛的市售P25。另外,所制备的光催化材料Ag2S/ZnO经4次循环使用后,其降解效率没有明显下降,表明该催化材料具有一定的光催化稳定性。经捕获实验研究发现,在Ag2S/ZnO的光催化反应中空穴起主要作用,并根据绝对电负性估算了复合材料Ag2S/ZnO的能带位置,据此提出了可能的光催化反应机理。  相似文献   

10.
在不同的制备条件下,通过微波水热两步法获得了一系列Ag2S/ZnO光催化剂,采用X射线粉末衍射(XRD)、X射线光电子能谱(XPS)、紫外-可见漫反射吸收光谱(UV-Vis/DRS)、扫描电子显微镜(SEM)和N2吸附-脱附等测试手段对产物结构和形貌进行了表征。结果表明,产物以六方纤锌矿ZnO为主,其晶型结构并未随着反应温度和Ag2S物质的量的增加而改变。Ag2S的引入显著增强了光催化剂在可见光区的吸收,使吸收边带发生红移,同时抑制了ZnO(001)晶面的生长。另外,所得产物的形貌随着Ag2S物质的量的增加从爆米花状转变为少量的柱体颗粒,且BET比表面积经过复合后明显减小。以罗丹明B为目标降解物,研究并比较了一系列Ag2S/ZnO光催化剂对罗丹明B的光降解性能。结果表明,nAg2S/nZnO为1:10时,光催化剂在紫外光、可见光和模拟日光的照射下具有最好的光催化效果,优于目前应用最广泛的市售P25。另外,所制备的光催化材料Ag2S/ZnO经4次循环使用后,其降解效率没有明显下降,表明该催化材料具有一定的光催化稳定性。经捕获实验研究发现,在Ag2S/ZnO的光催化反应中空穴起主要作用,并根据绝对电负性估算了复合材料Ag2S/ZnO的能带位置,据此提出了可能的光催化反应机理。  相似文献   

11.
The nanosized titania and TiO2/SiO2 particles were prepared by the microwave-hydrothermal method. The effect of physical properties TTIP/TEOS ratio and calcination temperature has been investigated. The major phase of the pure TiO2 particle is of the anatase structure, and a rutile peak was observed above 800°C. In TiO2/SiO2 particles, however, no significant rutile phase was observed, although the calcination temperature was 900°C. No peaks for the silica crystal phase were observed at either silica/titania ratio. The crystallite size of TiO2/SiO2 particles decreases as compared to pure TiO2 at high calcination temperatures. The TiO2/SiO2 particles show higher activity on the photocatalytic decomposition of orange II as compared to pure TiO2 particles.  相似文献   

12.
Subsolidus phase relations in the Ag2MoO4-CuO-MoO3 oxide-salt ternary system were determined. T-x diagram was plotted for the Ag2MoO4-CuMoO4 quasi-binary join. Double molybdate Ag2Cu2(MoO4)3 was found to exist on this join. This compound is a superstructure derived from orthorhombic Li3Fe(MoO4)3. Its structure was solved in terms of a subcell (a = 5.0749(3), b = 11.300(2), c = 18.127(3) ?, space group Pnma, Z = 4, R = 0.0678). In the true unit cell, the parameter a is tripled; suggested space group is P212121. A characteristic feature of the Ag2Cu2(MoO4)3 structure is infinite columns (extended along axis a) of face-sharing oxygen octahedra, in which disordered silver atoms are located (Ag(21), Ag(22), and Ag(23)) with various degrees of irregularity of their octahedral coordination and a strong anisotropy of thermal vibrations. Distorted CuO6 octahedra form zigzag ribbons extended in the same direction. MoO4 tetrahedra, which are arranged according to the pseudo-hexagonal law, link the aforementioned major structural elements into a three-dimensional framework. Trigonal-prismatic voids of the framework are occupied by silver atoms Ag (1). Presumably, the disorder of the silver ions in octahedral columns can be responsible for the increased ion conductivity of silver copper molybdate. A partial order of the same ions is the most likely reason for the appearance of superstructure with the tripled unit cell volume. Original Russian Text ? G.D. Tsyrenova, S.F. Solodovnikov, E.T. Pavlova, E.G. Khaikina, Z.A. Solodovnikova, 2009, published in Zhurnal Neorganicheskoi Khimii, 2009, Vol. 54, No. 5, pp. 802–809.  相似文献   

13.
Oxidative stress and hydroxyl radicals (·OH) play important roles in adverse health effects caused by inhalable ambient air particles (PM10). The ultra-fine fraction of PM10 has been hypothesized as one of the critical contributors to ·OH generation. Both in vivo and in vitro studies have shown that ultra-fine particles (UFPs) or nano-particles generate more ·OH than larger particles with identical mass and composition. Both the surface area and surface-adsorbed redox-active metals have been suggested as factors to determine the oxidative capacity of UFPs. In this study, the ·OH-generating capability of different sizes of SiO2 particles was investigated in order to determine which factor influences particle-induced ·OH generation. The amount of ·OH generated in both acellular and cellular systems was quantified using a capillary electrophoresis method following exposure to SiO2 particles with diameters of 14, 100, and 500 nm. The amount of ·OH was strongly dependent on particle size, and a significant enhancement was observed only with 14 nm particles. Further studies indicated a close association between ·OH and iron ion concentration (R 2 = 0.812, p<0.01). Washed particles, with their surface iron being removed, did not generate ·OH. The iron-containing leachate from these washings was able to enhance ·OH production as untreated particles did. Therefore, the presence of adsorbed iron on the surface of the SiO2 particles is presented as a possible mechanism of UPFs-induced ·OH generation. The SiO2 acted as an inert substrate, and the surface of ultra-fine SiO2 particles acted as a carrier for iron. Supported by the National Basic Research Priorities Program (Grant No. 2002CB410802) and the National Natural Science Foundation of China (Grant No. 20637020)  相似文献   

14.
SiO2/TiO2 composite microspheres with microporous SiO2 core/mesoporous TiO2 shell structures were prepared by hydrolysis of titanium tetrabutylorthotitanate (TTBT) in the presence of microporous silica microspheres using hydroxypropyl cellulose (HPC) as a surface esterification agent and porous template, and then dried and calcined at different temperatures. The as-prepared products were characterized with differential thermal analysis and thermogravimetric (DTA/TG), scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption. The results showed that composite particles were about 1.8 μm in diameter, and had a spherical morphology and a narrow size distribution. Uniform mesoporous titania coatings on the surfaces of microporous silica microspheres could be obtained by adjusting the HPC concentration to an optimal concentration of about 3.2 mmol L−1. The anatase and rutile phase in the SiO2/TiO2 composite microspheres began to form at 700 and 900 °C, respectively. At 700 °C, the specific surface area and pore volume of the SiO2/TiO2 composite microspheres were 552 and 0.652 mL g−1, respectively. However, at 900 °C, the specific surface area and pore volume significantly decreased due to the phase transformation from anatase to rutile.  相似文献   

15.
采用水热、化学沉积和原位光还原的方法成功制备了新型Ag/Ag2MoO4/Bi2MoO6三元复合光催化剂。通过X射线粉末衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)和紫外可见漫反射光谱(UV-Vis DRS)等技术对材料的组成、形貌、光吸收特性和光电化学性能等进行系统分析。以四环素为目标污染物,研究Ag/Ag2MoO4/Bi2MoO6在可见光下的光催化性能。研究结果表明,相比于纯Ag2MoO4和Bi2MoO6,Ag的表面等离子体共振(SPR)效应显著拓宽了催化体系对可见光的吸收能力及响应范围。当Ag2MoO4理论负载量(质量分数)为24.6%时,Ag/Ag2MoO4/Bi2MoO6复合材料在20 min内可将四环素完全降解,且5次循环使用后仍保持较高的催化活性,表现出良好的循环稳定性。  相似文献   

16.
以钼酸铵、硝酸铋和硝酸银为原料, 以十六烷基三甲基溴化铵(CTAB)为辅助活性剂, 采用水热法合成了Ag2O-Bi2MoO6光催化剂。用X射线粉末衍射、扫描电镜及紫外-可见吸收光谱等进行表征, 并对水中天然有机物富里酸进行了光催化氧化研究。结果表明:未掺杂钼酸铋表面平滑, Ag2O-Bi2MoO6表面有明显的小块颗粒存在, 分布集中, 且其XRD图出现Ag2O的衍射峰。与未掺杂样品相比, 掺杂Ag2O后Bi2MoO6的可见光催化活性提高, 当掺银量为1.5%时活性最高。实验最佳催化剂浓度为0.6 g·L-1, 在溶液pH值减小、富里酸初始浓度减小时有助于富里酸的去除。富里酸降解过程符合一级反应动力学方程, 拟合方程为y=-0.019 5x。对富里酸降解产物进行发光菌生物毒性测试, 发现光催化2 h后降解产物比处理前毒性降低约90%。  相似文献   

17.
以钼酸铵、硝酸铋和硝酸银为原料,以十六烷基三甲基溴化铵(CTAB)为辅助活性剂,采用水热法合成了Ag2O-Bi2MoO6光催化剂。用X射线粉末衍射、扫描电镜及紫外-可见吸收光谱等进行表征,并对水中天然有机物富里酸进行了光催化氧化研究。结果表明:未掺杂钼酸铋表面平滑,Ag2O-Bi2MoO6表面有明显的小块颗粒存在,分布集中,且其XRD图出现Ag2O的衍射峰。与未掺杂样品相比,掺杂Ag2O后Bi2MoO6的可见光催化活性提高,当掺银量为1.5%时活性最高。实验最佳催化剂浓度为0.6g·L-1,在溶液pH值减小、富里酸初始浓度减小时有助于富里酸的去除。富里酸降解过程符合一级反应动力学方程,拟合方程为y=-0.0195x。对富里酸降解产物进行发光菌生物毒性测试,发现光催化2h后降解产物比处理前毒性降低约90%。  相似文献   

18.
史楠  高保娇  杨青 《物理化学学报》2015,30(11):2168-2176
以微米级硅胶微粒为基质, 通过接枝聚合和大分子反应, 制备了具有刷状结构的阳离子性接枝微粒, 深入研究了其对牛血清白蛋白(BSA)的强吸附能力、吸附机理和吸附热力学. 首先使含叔胺基团的单体甲基丙烯酸二甲基氨基乙酯(DMAEMA)在硅胶微粒表面发生接枝聚合, 制得接枝微粒PDMAEMA/SiO2, 然后以氯乙胺为试剂, 使接枝大分子PDMAEMA链中的叔胺基团发生季铵化反应, 获得了具有刷状结构的阳离子聚电解质的功能接枝微粒QPDMAEMA/SiO2. 测定了微粒QPDMAEMA/SiO2的zeta 电位, 实施了对BSA的等温吸附实验, 考察了介质pH值、离子强度及温度对吸附作用的影响, 研究了吸附热力学. 研究结果表明, 功能接枝微粒QPDMAEMA/SiO2 比接枝微粒PDMAEMA/SiO2 具有更高的zeta 电位, 在静电相互作用驱动下, 微粒QPDMAEMA/SiO2对BSA具有很强的吸附能力. 吸附容量随介质pH值的增大呈现先增大后减小的变化趋势,当pH值等于BSA的等电点(pI=4.7)时, 具有最高的吸附容量(高达112 mg·g-1). 以等电点为界, 离子强度对吸附容量会产生完全相反的影响作用: 当介质pH值小于BSA的等电点时, 电解质浓度增大, 吸附容量增高; 当介质pH值等于BSA的等电点时, 吸附容量几乎不随电解质的浓度发生变化. 吸附过程熵值减小而且放出热量,是一个焓驱动的吸附过程.  相似文献   

19.
Fumed oxides, such as silica, alumina, titania, and mixed X/silicas (X=Al2O3 (AS), TiO2 (TS), CVD-TiO2, Al2O3/TiO2 (AST)), pristine or covered by carbon deposits formed due to pyrolysis of cyclohexene, were studied using nitrogen adsorption–desorption, photon correlation spectroscopy particle sizing, and electrophoresis. A significant influence of the nature of surface-active sites and structural features of oxides (individual silica, mixed fumed, or prepared using chemical vapor deposition (CVD)) on the pyrolysis of cyclohexene is observed with respect to the pore size distributions due to differences between primary particles in aggregates and on their outer surfaces in the filling of channels by pyrocarbon, resulting also in a decrease in fractal dimension. Structural characteristics and dependences of the particle size distribution and electrokinetic potential of X/SiO2 and C/X/SiO2 on the pH of aqueous suspensions suggest that the carbon deposit covers mainly acidic sites at the X/SiO2 interfaces and X phase patches possessing catalytic activity in pyrolysis, as the negative charge of particles is reduced by pyrocarbon grafting.  相似文献   

20.
比较了3种具有羟基表面SiO2层的差异:紫外光照SAMs形成的羟基表面,紫外光照射前、照射后的羟基表面;用光照前后表面的差异,结合化学浴沉积技术在单晶硅基底上制得了TiO2微图案薄膜。系统考察了光源、硅片表面性质的变化、溶液等方面对图案生成的影响。实验表明TiO2沉积在未照区,电子和空穴动力学上的差异造成光照区表面正电荷增多,抑制了TiO2的沉积。该方法不需要光刻胶和自组装膜作为辅助模板,具有简单廉价的特点。  相似文献   

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