纳米复合材料H_6P_2W_(18)O_(62)/TiO_2(P123)微波增强光催化降解染料

采用非离子表面活性剂(C3H6O·C2H4O)x(P123)作为模板剂,通过溶胶-凝胶与程序升温溶剂热一步法在较低温度下制备了具有锐钛矿晶型结构的有序复合孔材料-H6P2W18O62/TiO2(P123)。通过FT-IR、X-射线衍射、电感耦合等离子体原子发射光谱、透射电子显微镜、N2吸附-脱附测定以及扫描电子显微镜配合X-射线能量色散谱仪等测试手段对其组成、结构、表面形貌进行了表征。结果表明,复合材料中多酸的Dawson结构未发生明显变化,与母体多酸和TiO2相比,复合材料H6P2W18O62/TiO2(P123)的BET比表面积显著增大,高达414.6m2/g,且孔径有序性大幅度提高。光催化反应实验结果显示,H6P2W18O62/TiO2(P123)在微波场作用下,催化活性显著增强,可有效降解多种染料。     

有序复合光催化剂H6P2W18O62/TiO2的低温制备及其可见光光催化降解一氯苯

近年来,随着人们环保意识的增加,越来越多的人开始关注河流污染问题,各种处理有机污染物的方法逐渐被人们所研究.常见的方法主要有物化法、化学法、生物法和光催化氧化法等.其中,利用光催化氧化技术来处理各种有机污染物,如一氯苯的研究成为人们关注的热点[1-4].在大量的研究中,人们发现常见的光催化材料如TiO2,ZrO2和杂多酸的带隙较宽,光谱反应范围较窄,吸收主要集中在紫外区,光生载流子的复合效率较高,量子效率较低,因而,他们的实际应用受到了限制.为此将两种光催化剂通过掺杂改性来提高催化活性成为一种趋势.本文采用非离子表面活性剂C18H37(OCH2CH2)10OH(Brij-76)作为模板剂,利用Dawson结构的杂多酸H6P2W18O62对TiO2进行掺杂改性来提高复合催化剂的性能,并选择具有生物蓄积性的一氯苯[5,6]为探针分子,考察了该复合催化剂在可见光条件下的光催化活性,实验结果显示,H6P2W18O62/TiO2对有机污染物一氯苯的光催化降解效果良好.     

单斜BiVO4可见光催化降解甲基橙的形貌效应

以硝酸铋和偏钒酸铵为无机源,NaOH为pH值调节剂,三嵌段共聚物P123为表面活性剂,采用醇-水热法制备了多种形貌的单斜BiVO4.利用X射线衍射、N2吸脱附、扫描电子显微镜、X射线光电子能谱和紫外可见光漫反射等技术表征了其物化性质,并考察了这些BiVO4样品在可见光照射下降解甲基橙的催化活性.结果表明,表面活性剂和溶...     

银促进的TiO2光催化降解甲基橙

 采用溶胶-凝胶和水热协同法制备了不同Ag含量的负载型Ag-TiO2样品,这些样品具有较大的比表面积和较小的粒径. 适量负载金属银后的TiO2在紫外及可见光下的光催化活性均得到提高. 银在TiO2上的最佳负载量为0.15%, 过高的负载量反而会降低TiO2光催化降解甲基橙的活性. 由于反应机理的不同,银负载对TiO2可见光下催化活性的提高要明显高于对其紫外光下催化活性的提高. 在可见光照射下,从激发态染料注入到TiO2导带的电子迅速转移到了Ag原子簇, Ag原子簇通过促进电荷分离抑制了电子和染料正离子自由基的复合,从而促进了光催化过程. 研究结果表明,有效地促进电荷分离以及激发态电子和氧气分子的反应是提高染料敏化光催化活性的关键.     

有序介孔材料H6P2W18O62/TiO2(Brij-76)的制备与微波增强光催化降解一氯苯

采用非离子表面活性剂C18H37(OCH2CH2)10OH(Brij-76)作为模板剂,在以杂多酸H6P2W18O62对TiO2掺杂改性基础上,通过模板-溶胶-凝胶-程序升温溶剂热一步法在较低温度下制备了有序复合介孔材料H6P2W18O62/TiO2(Brij-76).通过傅立叶变换红外(FT-IR)光谱,X射线衍射(XRD),扫描电子显微镜(SEM),能量色散X射线(EDX),N2吸附-脱附测定和NH3程序升温脱附(NH3-TPD)等手段对其进行了表征.结果表明,以非离子表而活性剂Brij-76为模板剂制得的复合材料H6P2w18O62/TiO2(Brij-76)平均孔径约为3.31 nm,BET比表面积为99.78 m2·g-1.与TiO2相比,其孔径有序性大幅度提高,粒子的聚集度降低,表面酸性显著增加.微波增强光催化性能研究结果显示,H6P2W18O62/TiO2(Brij-76)在微波作用下催化活性更高,可有效地降解一氯苯溶液.     

α-H_6P_2W_(18)O_(62)·37H_2O的热稳定性

通过溶解性实验、变温红外、紫外光谱、X射线粉末衍射(XRD)和热重-差热分析(TG DTA)等手段,对Dawson结构钨磷酸的热稳定性进行了较系统的研究,结果表明,阴离子骨架在360℃左右开始分解,并提出了化合物热分解的可能机理.     

Hydrothermal Synthesis of CdIn2S4 and Photocatalytic Degradation of Methyl Orange under Visible-light Irradiation

CdIn2S4 microspheres were synthesized by a facile hydrothermal method with the temperature ranging from 120 to 200 ℃. X-ray diffraction, UV-vis diffuse reflectance spectroscopy, nitrogen sorption analysis, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy were used to characterize the products. It was found that the crystallographic structure and optical property of the products synthesized at different temperature were almost the same. The SBET of CdIn2S4 products decreased when the synthesized temperature increased, and the largest SBET was 33.16m2g-1 (120 ℃ sample). The degradation of methyl orange (MO) under the visible-light irradiation had been used as a probe reaction to investigate the photocatalytic activity of the as-prepared CdIn2S4, which showed that the CdIn2S4 sample synthesized at 120 ℃ presented the best photocatalytic activity for MO degradation.     

纳米复合材料Ag/TiO_2-ZrO_2的制备及其微波增强光催化降解甲基橙

采用EO20PO70EO20(P123)作模板剂,通过溶胶-凝胶-程序升温溶剂热一步法,并经萃取处理制备了具有光催化活性的纳米复合材料Ag/TiO2-ZrO2.用X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)、N2吸附-脱附测定和扫描电子显微镜配合X射线能量色谱仪(SEM-EDS)等测试手段对其组成、结构及形貌等进行了表征.结果表明,复合材料Ag/TiO2-ZrO2中Ag以单质形式存在,材料具有双孔结构,颗粒分布较均匀,结构也较规整,平均孔径约为3.6和9.0nm.通过微波增强光催化降解染料甲基橙的实验,对复合材料Ag/TiO2-ZrO2的光催化活性进行了探究.实验结果表明,微波辅助光催化效果优于紫外辐射,并且萃取后的合成产物Ag/TiO2-ZrO2在90min内对甲基橙的降解率可达81.5%,其活性高于市售P25以及TiO2-ZrO2.     

UV/TiO2 Photocatalytic Degradation of Xanthene Dyes

UV/titanium dioxide (TiO₂) degradation of two xanthene dyes, erythrosine B (Ery) and eosin Y (Eos), was studied in a photocatalytic reactor. Photocatalysis was able to degrade 98% of Ery and 73% of Eos and led to 65% of chemical oxygen demand removal. Experiments in buffered solutions at different initial pH values reveal the pH dependence of the process, with better results obtained under acidic conditions due to the electrostatic attraction caused by the opposite charges of TiO₂ (positive) and of anionic dyes (negative). Batch activity tests under methanogenic conditions showed the high toxicity exerted by the dyes even at low concentrations (~85% with initial concentration of 0.3 mmol L^?1), but the end products of photocatalytic treatment were much less toxic toward methanogenic bacteria, as detoxification of 85 ± 5% for Eos and 64 ± 7% for Ery were obtained. In contrast, the dyes had no inhibitory effect on the biogenic‐carbon biodegradation activity of aerobic biomass, obtained by respirometry. The results demonstrate that photocatalysis combining UV/TiO₂ as a pretreatment followed by an anaerobic biological process may be promising for the treatment of wastewaters produced by many industries.     

K_8P_2V_2W_(16)O_(62)/TiO_2复合催化剂的制备及光催化降解罗丹明B

采用溶胶-凝胶-程序升温一步法合成了复合材料K_8P_2V_2W_(16)O_(62)/TiO_2,经X-射线衍射(XRD)、扫描电子显微镜(SEM)对复合材料的结构和形貌进行了表征。结果表明,复合材料K_8P_2V_2W_(16)O_(62)/TiO_2中呈锐钛矿晶型结构的TiO_2附着在多酸K_8P_2V_2W_(16)O_(62)表面。以罗丹明B为模型分子,分别考察了K_8P_2V_2W_(16)O_(62)、TiO_2及复合材料K_8P_2V_2W_(16)O_(62)/TiO_2在紫外光下的降解性能,发现在120 min内,K_8P_2V_2W_(16)O_(62)/TiO_2的光催化活性优于K_8P_2V_2W_(16)O_(62)和TiO_2。     

H2O2/TiO2超声协同光降解活性艳橙的研究

以活性艳橙溶液为模拟废水,通过H₂O₂/TiO₂超声(US)协同作用光降解活性艳橙溶液,探讨了TiO₂催化剂用量、H₂O₂用量、活性艳橙溶液的初始浓度、pH值、TiO₂催化剂锻烧温度等对活性艳橙溶液降解率的影响,并比较了几种不同作用方式对活性艳橙溶液的降解效果.结果表明:UV/H₂O₂/TiO₂/US协同作用降解活性艳橙溶液的效果最好;当活性艳橙溶液的初始浓度为20 mg·L^-1,pH＝5,TiO₂用量为0.4 g·L^-1,H₂O₂用量为0.4 ml·L^-1时,降解率可达92.06%.     

板式纳米碳纤维负载二氧化钛光催化复合材料的制备及降解甲基橙的研究

以板式纳米碳纤维为载体,采用酸性氧化法对载体进行预处理之后,使用钛酸异丙酯为钛源,高温水热法制备了二氧化钛/纳米碳纤维复合光催化剂,并考察了其对甲基橙的光催化去除能力及循环反应性能.复合材料中二氧化钛含量通过改变前驱体组成进行调节.材料的结构性能通过氮气吸附、X射线衍射(XRD)、能谱分析仪(EDS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、热重分析仪(TG-DSC)等测试技术进行了表征.结果表明,锐钛矿型的二氧化钛以纳米颗粒形式均匀分散在纳米碳纤维表面,从而形成了高度分散的二氧化钛/碳纤维纳米复合材料.另外,复合系统中中孔吸附作用的存在,与纳米二氧化钛的光催化产生协同作用,增强了复合材料在紫外光照射下对于水溶液中甲基橙的去除能力.在光照射下反应120 min时,不同担载量样品对甲基橙的去除率最高可达80.1%,不同煅烧温度样品最高可达79.2%.此外,光催化剂有着良好重复利用性能,3次循环反应后对甲基橙去除率仍可保持80.0%.     

K_6[P_2W_(18)O_(62)]·14H_2O制备及性质表征实验教学研究

Dawson结构多酸化合物K_6[P_2W_(18)O_(62)]·14H_2O的制备及性质表征实验,通过水溶液回流方法制备,利用红外光谱、热重分析和电化学方法表征其性质。该实验中采用了经典的多酸化合物制备方法,不但产物具有良好的电致变色性质,而且将多酸化学研究的方法和思路,化合物制备、测试、数据分析等训练融入到"多酸化学"实验课的教学中,加深了学生对多酸化学相关知识点的理解,探索提升无机化学研究生科研素质的实验教学。     

Nanocomposite of CeVO4/BiVO4 Loaded on Reduced Graphene Oxide for the Photocatalytic Degradation of Methyl Orange

A facile procedure, involving one-pot synthesis of CeVO₄/BiVO₄ and in-situ reduction of graphene oxide (GO), has been used to prepare CeVO₄/BiVO₄/rGO nanocomposites. Different ratios of the CeVO₄–BiVO₄ were prepared to afford composites represented as CBVG3, CBVG5, and CBVG7. The ternary nanocomposite materials were characterized by using powder X-ray diffractometer (XRD), scanning electron microscopy (SEM), transmission electron microscope (TEM), photoluminescence and UV–vis spectroscopic techniques. Photocatalytic efficiency of the as-prepared ternary nanocomposites was investigated through the photo degradation of methyl orange under a visible light irradiation at 470 nm. The photocatalytic performance was enhanced by loading the CeVO₄/BiVO₄ nanoparticles on reduced graphene oxide (rGO), given MO degradation rate of 57, 65, 80, and 90% for BVG, CBVG3, CBVG5, and CBVG7, respectively after exposure to visible light for 120 min. Effects of experimental process parameters including initial dye concentration, catalysts loading and effect of different modification regimes were studied using CBVG7, which exhibited the highest efficiency. The improvement in the photocatalytic efficiency may be attributed to increased surface area of the nanocomposites, enhanced light absorption capacity and improved charge separation. The study showed a one-pot synthesis route to prepare promising CeVO₄/BiVO₄/GO nanocomposites for the photo-enhanced degradation of dye contaminants.

     

MoS_2/TiO_2复合催化剂的制备及其在紫外光下的光催化制氢活性

为了研究复合光催化剂在光催化中的制氢效率,采用水热法制备了Mo S2纳米片,然后通过水热法在Mo S2纳米片上负载了TiO_2纳米颗粒,形成了Mo S2/TiO_2异质结复合催化剂。采用冷场发射扫描电子显微镜(FE-SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、紫外-可见吸收光谱(UV-Vis)、拉曼光谱(Raman),X射线光电子能谱(XPS)对材料的结构和光学性能表征并进行分析。通过光催化制氢测试对光催化剂进行评价,实验结果表明,在波长为365 nm的紫外光照射下,最高光催化制氢速率为1004μmol·h-1·g-1,对应的催化剂的Mo S2含量为30%,其催化速率远大于单一的Mo S2和TiO_2,表明Mo S2/TiO_2复合催化剂在紫外光照下能显著提高光催化产氢性能。基于Mo S2/TiO_2复合光催化剂优越的光催化产氢性能,本文对复合光催化剂的产氢机理做了研究和分析。     

Hydrothermal Synthesis of H3PW12O40/TiO2 Nanometer Photocatalyst and Its Catalytic Performance for Methyl Orange

H3PW12O40/TiO2 nanometer photocatalyst was prepared by one step hydrothermal synthesis from H3PW12O40′nH2O and Ti(OBu)4,simultaneously realizing the load and modification of H3PW12O40.The catalyst was ...     

H6P2W18O62·14H2O as an efficient catalyst for the green synthesis of α-aminophosphonates from α-amino acids

Abstract

A simple, efficient and eco-friendly protocol has been described for the synthesis of α-aminophosphonates via Kabachnik-Fields reaction, catalyzed by H₆P₂W₁₈O₆₂·14H₂O as a reusable catalyst. The reaction was realized by condensation of amino acids, various aromatic aldehydes and triethylphosphite under solvent-free conditions, the corresponding α-aminophosphonates were formed in good yields. All the new products were characterized by IR, ¹H, ¹³C and ³¹P-NMR analyses. This method offers advantages such as simplicity workup with the green aspects, good yields and short reaction times.     

Dawson型磷钨杂多阴离子P2W18O6-62的电化学性质和对O2还原的电催化作用

用循环伏安、交流伏安和交流阻抗法对Dawson型磷钨杂多阴离子P2W18O66-2的电化学性质进行了详细研究,循环伏安结果显示,P2W18O66-2在pH2.52的0.1mo·lL-1Na2SO4+NaHSO4溶液中有两对可逆的单电子还原-氧化波和两对可逆的双电子还原-氧化波.单电子波的峰电位和电流与溶液的pH无关,双电子波的峰电位则随溶液pH的增加而负移,峰电流降低,表明双电子电极过程完全受扩散控制,实验测定其扩散系数(DO)为2.5×10-6cm2-1.循环伏安结果表明P2W18O6-62的第III对波对O2还原为H2O2具有显著的电催化作用,催化效率约达300%.将P2W18O6-62应用于PW11O39Fe(III)(H2O)4-构成的类电-芬顿过程,使该过程对硝基苯的降解效率显著提高.     

BiOI/Bi_2WO_6对甲基橙和苯酚的光催化降解及光催化机理(英文)

采用简单的沉积方法制备了不同碘化氧铋含量的BiOI/Bi2WO6光催化剂,通过X射线衍射(XRD)、扫描电子显微镜(SEM)、高分辨透射电子显微镜(HR-TEM)、紫外-可见漫反射光谱(UV-Vis DRS)和BET比表面积测量对其进行了表征。在紫外和可见光的照射下,使用甲基橙和苯酚的光催化降解评价了BiOI/Bi2WO6催化剂的光催化性能。结果表明:与商业P25和纯Bi2WO6相比,13.2%BiOI/Bi2WO6光催化剂具有更高的紫外和可见光催化性能。这明显增加的光催化活性主要归功于光生电子和空穴在Bi2WO6和BiOI界面上的有效转移,降低了电子-空穴对的复合。基于BiOI和Bi2WO6的能带结构,提出了光生载流子的一种转移过程。自由基清除剂的实验表明,·OH,h+,·O2-和H2O2,特别是h+,共同支配了甲基橙和苯酚的光催化降解过程。