Bi2MoO6-Pt异质结的制备及其光催化性能研究

采用"溶剂热-光还原"法成功制备出Bi_2MoO_6-Pt异质结光催化剂.该催化剂由Bi_2MoO_6三维微球(直径:1~4μm)和Pt纳米颗粒(~2.5nm)组成.本文以罗丹明B(Rh B)和4-氯酚(4-CP)为目标污染物研究了该异质结的可见光光催化性能.Bi_2MoO_6-Pt异质结的光催化活性明显高于纯Bi_2MoO_6,Pt的最佳负载量为0.3 wt%.同时,Bi_2MoO_6-Pt-2异质结(Pt的负载量为0.3 wt%)也可以有效地矿化有机污染物.更重要的是,Bi_2MoO_6-Pt-2异质结具有良好的稳定性,可以被重复使用.     

钛基石墨烯复合材料的制备及其光催化还原Cr（VI）的研究

通过改进的Hummers法制备氧化石墨烯(GO),再将氧化石墨烯和钛酸四丁酯作为初始反应物,利用溶剂热法制备Ti O_2/RGO纳米复合材料.利用SEM、TEM、XPS、XRD等分析手段对Ti O_2/RGO纳米复合材料进行表征,考察其在可见光照射条件下光催化还原水中Cr(Ⅵ)的效能,并对光催化还原机制进行了初步探讨.结果表明,Ti O_2/RGO复合材料的光催化还原能力与单一Ti O_2(P25)相比有了显著提高;复合材料中RGO含量、溶液p H值、催化剂投加量、Cr(Ⅵ)初始浓度均对光催化还原过程有所影响,当复合材料中RGO含量比例为2%、溶液p H值为2,催化剂投加量为40 mg时,光催化还原Cr(Ⅵ)的效率可达98%.光催化还原Cr(Ⅵ)的过程是吸附过程和光催化还原过程的共同作用结果,RGO不但提高了复合材料的吸附能力,还作为复合材料的电子导体,抑制了光生电子-空穴对的复合,增强了复合材料的光催化性能.经过5次循环使用后,复合材料的光催化还原效率仍然保持在90%左右.     

In_2TiO_5纳米带的静电纺丝法制备及光催化性能

以酞酸丁酯(Ti(OC_4H_9)_4)、硝酸铟(In(NO3)3)和聚乙烯吡咯烷酮(PVP-K30)为原料,采用静电纺丝技术制备了In_2TiO_5纳米带.利用X射线衍射(XRD)、扫描电子显微镜(SEM)、紫外-可见漫反射光谱(UV-vis DRS)和氮气吸附-脱附等温线(BET)等技术对样品进行了表征.考察了In_2TiO_5纳米带在光催化降解罗丹明B(RhB)、甲基橙(MO)、亚甲基蓝(MB)和左氧氟沙星(LEV)过程中的应用性能,研究了不同离子型物质、溶液的pH和MB起始浓度对In_2TiO_5纳米带光催化活性的影响.结果表明:In_2TiO_5纳米带具有正交晶系结构,禁带宽度为3.47 eV,比表面积为20.71 m~2·g~(-1),可应用于4种不同离子型物质的光催化降解,发现光催化效果与被降解物质的表面带电性质有关.在紫外光照射下,90 min,对MB的降解率达98.1%,其降解过程服从一级动力学模型.     

Ni2P/Bi2MoO6复合材料的制备及可见光催化活性

分别制备了花状Bi₂MoO₆和片状Ni₂P,采用研磨、水热及超声的方式将两种材料复合,考察了负载方式、负载率和溶液pH值对其可见光下降解亚甲基蓝（MB）的影响;利用XRD、XPS、FTIR、SEM、PL和UV-Vis等测试手段表征了样品的微观结构、形貌和光学性质;研究表明Ni₂P作为助催化剂,可加速电子空穴对分离,显著提高Bi₂MoO₆的光催化活性,其中当Ni₂P负载率为4%时,TOC去除率为64.28%,降解速率为纯Bi₂MoO₆的2倍,且将Ni₂P/Bi₂MoO₆复合催化剂循环利用3次后,同实验条件下降解率为94%,证明复合催化剂稳定性好.     

CoCuMnOx光催化氧化多组分VOCs特性及其动力学

实验采用共沉淀法制备太阳能吸收涂料Co Cu Mn O_x,探究可见光下甲苯、乙酸乙酯和丙酮混合3组分VOCs的光催化氧化性能,并从动力学角度分析各自的反应速率变化.结果表明,单组分VOCs初始浓度400 mg·m~(-3)、光照距离120 mm,350cm~2镜面载体负载1 g Co Cu Mn O_x下用100 W卤钨灯照射6 h后,甲苯转化率为57%、乙酸乙酯为62%、丙酮为58%;由于3组分VOCs之间相互竞争,甲苯、乙酸乙酯和丙酮的转化率较单组分下降了5%~26%.单组分与3组分VOCs的光催化均符合假一级反应动力学,单组分甲苯、乙酸乙酯和丙酮的反应速率分别为0.002、0.002 8和0.002 33 min~(-1);混合3组分中其反应速率为单组分的0.49~0.88倍.     

MoS2/BiOI复合光催化剂制备及其光催化氧化还原性能

通过两步法合成花状MoS_2/BiOI复合光催化剂,采用X射线衍射(XRD)、扫描电镜(SEM)、紫外可见漫反射(UVVis)、光电子能谱(XPS)等方法对合成的样品进行了表征,对其可能的形成机制进行探究,通过电化学表征计算出BiOI与MoS_2的价带与导带位置,显示复合材料形成了1型异质结.同时以罗丹明B(RhB)与含Cr6+溶液作为目标污染物测试光催化剂的氧化还原性能,相比于BiOI和MoS_2单体,MoS_2/BiOI复合光催化剂表现出更强的光催化氧化与还原能力,其中以质量分数为2%的MoS_2与BiOI复合光催化剂效果最佳,可见光照20 min后RhB降解率达到98.92%,80 min后Cr6+溶液光催化还原率可达到97.87%,较纯BiOI分别提高了1.79倍与3.85倍,且经过4次重复利用后仍具有较高的光催化活性.光催化降解Rh B过程中空穴(h+)与超氧自由基(·O-2)作为主要活性物种,其中空穴影响更为显著.     

混晶纳米TiO_2的制备及其光催化降解有毒有机污染物

以无定形TiO2沉淀为前驱体,在水热条件下得到了含板钛矿(121)相混晶纳米TiO2,考察了水热反应的温度和时间等因素对含板钛矿型TiO2光催化活性的影响.采用XRD、TEM对制备的TiO2进行初步表征,并结合光催化(λ≤387 nm)降解有机染料的光活性探针反应.结果表明,水热温度为150℃,时间为24 h时,可制得具有较高光催化活性的纳米TiO2,其纳米尺寸为14.20 nm,板钛矿相含量63.6%,锐钛矿含量为36.4%.光催化实验中跟踪研究了其对染料酸性桃红(sulforhodmineB,SRB)的褪色及2,4-DCP的降解情况,并对降解中间产物H2 O2、.OH进行跟踪测定,实验结果表明板钛矿相混晶TiO2的光催化主要涉及.OH氧化历程,光照射9 h对SRB和2,4-DCP的矿化氧化分别达到89%和78%,循环5次光催化降解SRB实验,催化剂表现出较好的稳定性,催化性能无明显变化.     

TiO_2对In-Ag-O/γ-Al_2O_3催化剂上CO选择性还原NO的改性研究

以Ti O2、γ-Al2O3及Ti O2-γ-Al2O3复合氧化物为载体,以In-Ag-O基为活性组分,采用等体积浸渍法制备了一系列In/Ag催化剂,通过XRD、BET、SEM、H2-TPR等技术手段对催化剂表面形态进行分析,并考察了催化剂对CO选择性还原NO的反应活性和载体中Ti O2含量对催化性能的影响.结果表明,Ti O2的添加促进了活性组分铟和银物种的分散,当Ti O2的含量为载体的15%时制备的催化剂活性最高,合适的Ti O2与γ-Al2O3配比使活性组分与载体之间发生了强烈的相互作用,由此提高了CO选择性还原NO的活性.     

CuxCe1-xO2/γ-Al2O3催化剂催化燃烧甲苯性能的研究

以γ-Al₂O₃ 为载体,以复合氧化物Cu_xCe_1-xO₂为活性组分,其中,x=0.1,0.2,0.4,0.6,0.8,通过浸渍法制备了一系列Cu_xCe_1-xO₂/γ-Al₂O₃催化剂.在固定床反应器中评价了催化剂对甲苯的催化活性,通过XRD、SEM对催化剂进行表征,并运用ICP-MS分析并计算Cu、Ce的摩尔比以及活性组分的负载量.结果表明,在Cu_xCe_1-xO₂/γ-Al₂O₃催化剂中Cu、Ce摩尔比的实际值与理论值相近,活性组分的负载量在19%以上,而且对甲苯都有较好的低温催化活性,其中当x=0.2时,即Cu_0.2Ce_0.8O₂/γ-Al₂O₃催化剂对甲苯的催化活性最高,其中T₁₀=160 ℃,T₉₀=265 ℃;当甲苯的进口浓度在700~3000 mg·m^-3时,进口浓度对Cu_0.2Ce_0.8O₂/γ-Al₂O₃催化剂的催化活性影响较小,且经过连续80 h的稳定性操作后转化率仍然保持在90%以上.     

硼掺杂CeO2/TiO2光催化剂的制备及其活性研究

在三氯化钛和钛酸丁酯水解过程中引入硼酸、硝酸铈,制备了具有可见光活性的硼(B)掺杂CeO₂/TiO₂复合氧化物光催化剂,采用XRD、DRS、XPS等手段进行表征,以偶氮染料酸性红B为模型污染物评估了催化活性.结果表明,硝酸铈加入量影响催化剂的吸收带边,随用量增加,吸收带边红移至481nm(Ce/Ti=1.0,摩尔比),继续增加用量,吸收带边轻微蓝移.催化剂晶相组成与焙烧温度有关,500℃时焙烧样品主要由立方晶型CeO₂和锐钛矿TiO₂组成,焙烧温度高于700℃时,TiO₂转化为金红石型,CeO₂则无显著变化.随焙烧温度升高,催化剂吸收带边明显蓝移,综合考虑催化剂稳定性和太阳能利用,认为500℃焙烧较为合适.B1s XPS显示仅有少量B原子进入复合氧化物晶格取代了氧原子,主要以B₂O₃形式存在.酸性红B降解试验显示B掺杂CeO₂/TiO₂可以提高TiO₂的催化活性,紫外光辐射10min最高可使96.0%的酸性红B分解,且反应彻底,表现出较强的氧化能力,但Ce/Ti>0.5(摩尔比)时催化活性显著下降.     

Photocatalytic defluorination of perfluorooctanoic acid by surface defective BiOCl: Fast microwave solvothermal synthesis and photocatalytic mechanisms

There is an urgent need for developing cost-effective methods for the treatment of perfluorooctanoic acid(PFOA)due to its global emergence and potential risks.In this study,taking surface-defective BiOCl as an example,a strategy of surface oxygen vacancy modulation was used to promote the photocatalytic defluorination efficiency of PFOA under simulated sunlight irradiation.The defective BiOCl was fabricated by a fast microwave solvothermal method,which was found to induce more surface oxygen vacancies than conventional solvothermal and precipitation methods.As a result,the asprepared BiOCl showed significantly enhanced defluorination efficiency,which was 2.7 and33.8 times higher than that of BiOCl fabricated by conventional solvothermal and precipitation methods,respectively.Mechanistic studies indicated that the defluorination of PFOA follows a direct hole(h~+)oxidation pathway with the aid of·OH,while the oxygen vacancies not only promote charge separation but also facilitate the intimate contact between the photocatalyst surface and PFOA by coordinating with its terminal carboxylate group in a bidentate or bridging mode.This work will provide a general strategy of oxygen vacancy modulation by microwave-assisted methods for efficient photocatalytic defluorination of PFOA in the environment using sunlight as the energy source.     

气相合成二氧化钛超细粒子的形态及其光催化性

高温 管式气溶胶反应器中，利用ＴｉＣｌ４氧化反应制备ＴｉＯ２超细粒子，研究反应温度、停贸时间对ＴｉＯ２形态的影响。结果表明反应温度升高，ＴｉＯ２粒度增大、金红石含量为１３００℃时出现最大值；停留时间延长，粒粒度增大、金红石含量也增加。     

Photocatalytic reduction of organic pollutant under visible light by green route synthesized gold nanoparticles

We report a rapid method of green chemistry approach for synthesis of gold nanoparticles(AuNPs)using Lagerstroemia speciosa leaf extract(LSE). L. speciosa plant extract is known for its effective treatment of diabetes and kidney related problems. The green synthesis of Au NPs was complete within 30 min at 25°C. The same could also be achieved within 2 min at a higher reaction temperature(80°C). Both UV–visible spectroscopy and transmission electron microscopy results suggest that the morphology and size distribution of Au NPs are dependent on the pH of gold solution,gold concentration,volume of LSE,and reaction time and temperature. Comparison between Fourier transform infrared spectroscopy(FT-IR)spectra of LSE and the synthesized Au NPs indicate an active role of polyphenolic functional groups(from gallotannins,lagerstroemin,and corosolic acid)in the green synthesis and capping of Au NPs. The green route synthesized Au NPs show strong photocatalytic activity in the reduction of dyes viz.,methylene blue,methyl orange,bromophenol blue and bromocresol green,and 4-nitrophenol under visible light in the presence of Na BH_4. The non-toxic and cost effective LSE mediated Au NPs synthesis proposed in this study is extremely rapid compared to the other reported methods that require hours to days for complete synthesis of Au NPs using various plant extracts. Strong and stable photocatalytic behavior makes Au NPs attractive in environmental applications,particularly in the reduction of organic pollutants in wastewater.     

光催化薄膜的亲水性及其应用

玻璃表面的雾化及建筑物表面的污染严重影响人们日常生活及工业。传统方法通常借助外力解决表面雾化及污染问题,如人工清洗,不仅维护成本高,而且施工难度大。光催化亲水薄膜作为一种具有特殊润湿性的表面,可高效持久地实现基底表面的防雾和自清洁功能。近年来,光催化薄膜防雾和自清洁性能的研究不断涌现,但相关的针对性综述却很少。本文详细阐述了光催化薄膜的亲水原理及亲水性评价方法,重点介绍了亲水性的改善方法,并对缺乏研究的亲水性与光催化分解有机污染物活性关系进行了简要概述,总结了国内外光催化薄膜亲水性的应用现状,分析了其存在问题及发展方向,旨在为光催化薄膜亲水性的研究及其应用起到一定的指导作用。     

Ti-MCM-41的微波水热法合成、表征及其催化氧化性质研究

本研究利用微波水热法合成Ti-MCM-41,并采用XRD、FTIR、BET、XPS及TEM等技术对材料进行表征.同时,使用甲基橙溶液作为光催化氧化的对象,对光催化剂的氧化性能进行考察.实验结果表明:利用微波水热法合成Ti-MCM-41,可将合成时间缩短至3 h,能够大大缩减反应时间并节省能源.通过在MCM-41多孔结构中掺杂钛,可明显提高其光催化活性.在酸性溶液中,Ti-MCM-41的催化氧化效率较高.XRD、FTIR、BET、XPS及TEM等表征结果表明,钛成功地掺入到了MCM-41中,并未破坏其多孔有序的结构,Ti-MCM-41同时兼具介孔材料的高比表面积和二氧化钛的光催化性能,有利于在环境污染修复上的应用.     

Graphitic carbon nitride/biochar composite synthesized by a facile ball-milling method for the adsorption and photocatalytic degradation of enrofloxacin

In order to enhance the removal performance of graphitic carbon nitride (g-C₃N₄) on organic pollutant, a simultaneous process of adsorption and photocatalysis was achieved via the compounding of biochar and g-C₃N₄. In this study, g-C₃N₄ was obtained by a condensation reaction of melamine at 550°C. Then the g-C₃N₄/biochar composites were synthesized by ball milling biochar and g-C₃N₄ together, which was considered as a simple, economical, and green strategy. The characterization of resulting g-C₃N₄/biochar suggested that biochar and g-C₃N₄ achieved effective linkage. The adsorption and photocatalytic performance of the composites were evaluated with enrofloxacin (EFA) as a model pollutant. The result showed that all the g-C₃N₄/biochar composites displayed higher adsorption and photocatalytic performance to EFA than that of pure g-C₃N₄. The 50% g-C₃N₄/biochar performed best and removed 45.2% and 81.1% of EFA (10 mg/L) under darkness and light with a dosage of 1 mg/mL, while g-C₃N₄ were 19.0% and 27.3%, respectively. Besides, 50% g-C₃N₄/biochar showed the highest total organic carbon (TOC) removal efficiency (65.9%). Radical trapping experiments suggested that superoxide radical (?O₂^?) and hole (h⁺) were the main active species in the photocatalytic process. After 4 cycles, the composite still exhibited activity for catalytic removal of EFA.     

纳米复合GeO2/TiO2的制备及光催化性能研究

采用改进的Sol-gel方法,制备了一种新型的单分散椭球形微孔结构的纳米GeO2/TiO2复合光催化剂,并用TG-DTA、XRD、XPS、UV-vis、FT-IR、TEM、BET等手段进行了表征.以难生化降解的染料罗丹明B为目标降解物,采用HPLC测定不同光照时间下催化剂对染料降解的情况,考察了催化剂的光催化活性结果表明,改进的Sol-gel法制得的复合光催化剂具有明显的孔结构,而且比表面积大、粒径小、粒径分布窄、分散性好;与适量GeO2复合后能够有效提高TiO2纳米粒子的光催化活性;复合光催化剂的最佳制备条件为GeO2摩尔含量为0.1%,煅烧温度为400℃,所制得的GeO2/TiO2光催化活性比纯TiO2有显著提高.     

Preparation, characterization, and photocatalytic activities of boron- and cerium-codoped TiO2

Boron- and cerium-codoped TiO2 photocatalysts were synthesized using modified sol-gel reaction process and characterized by X- ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS）, particle size distribution （PSD）, diffuse reflectance spectra （DRS）, and Brunauer-Emmett-Teller （BET）. The photocatalytic activities were evaluated by monitoring the degradation of dye Acid Red B （ARB）. The results showed that the prepared photocatalysts were mixed oxides mainly consisting of titania, ceria, and boron oxide. The structure of TiO2 could be transformed from amorphous to anatase and then to rutile by increasing calcination temperature; the transformation being accompanied by the growth of particle size without any obvious change in phase structure of CeO2. The XPS of B1.6Ce1.0-TiO2 prepared at 500℃ showed that a few boron atoms were incorporated into titania and ceria lattice, whereas others existed as B2O3. Cerium ions existed in two states, Ce^3＋ and Ce^4＋, and the atomic ratio of Ce^3＋/Ce^4＋ was 1.86. When boron and cerium were doped, the UV-Vis adsorption band wavelength showed an obvious shift toward the visible range （〈526 nm）. As the atomic ratio of Ce/Ti increased to 1.0, the absorbance edge wavelength increased to 481 nm. The absorbance edge wavelength decreased for higher cerium doping levels （Ce/Ti=2.0）. The particles size ranged from 122 to 255 nm with a domain at 168 nm （39.4%）. The degradation of ARB dye indicated that the photocatalytic activities of boron- and cerium-codoped TiO2 were much higher than those of P25 （a standard TiO2 powder）. The activities increased as the boron doping increased, whereas decreased when the Ce/Ti atomic ratio was greater than 0.5. The optimum atomic ratio of B/Ti and Ce/Ti was 1.6 and 0.5, respectively.     

微波合成有机膨润土及其吸附水中有机物的性能

采用微波辅助合成法制备有机膨润土.试验表明,其最佳条件是表面活性剂(CPC)的用量为膨润土阳离子交换容量(CEC)的 80%～100%,微波能量为420J/mL.在微波的作用下,有机膨润土合成反应速度有较大提高,反应活化能从常规合成的44.83kJ/mol降低到5.23kJ/mol.与常规湿法合成的有机膨润土相比,微波法合成的 CPC 有机膨润土的层间距增加 12.8%,有机碳含量提高 32.5%,比表面积降低 33.9%,在废水处理过程中不易脱附,对酸性大红的吸附处理效率提高 50.89%.     

纳米TiO2的凝胶网格沉淀法制备及其光催化性能

以明胶为反应介质,采用凝胶网格沉淀法制备纳米TiO2光催化剂,利用TG-DTA、XRD、TEM、FT-IR、UV-Vis、FL等分析测试手段对制备过程、样品的结构和性能进行了研究.结果表明,利用凝胶网格沉淀法不仅能够控制纳米微粒的晶相和大小,而且可防止沉淀物相互聚集和团聚,获得的纳米微粒粒径更小,分散性更好.以染料罗丹明B溶液为目标降解物,1h的降解率为98%.最佳光催化剂的合成条件为8%明胶浓度、650℃煅烧2h.