微量Ag_3PO_4改性g-C_3N_4的可见光催化活性研究

采用一种简易方法制备了较低Ag3PO4含量的Ag3PO4/g-C3N4复合可见光催化剂,采用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、透射电子显微镜(TEM)、扫描电子显微镜(SEM)、紫外可见漫反射光谱(UV-vis DRS)、荧光光谱(PL)和X射线光电子能谱(XPS)等对Ag3PO4/gC3N4进行了系统分析与表征。通过在Ag3PO4/g-C3N4存在条件下甲基橙的光降解反应,考察该催化剂的可见光催化活性。结果表明,所制备的复合材料中确实存在Ag3PO4,Ag3PO4的引入对gC3N4晶型结构没有明显的影响,但显著提高了其在可见光区的吸收能力和光生电子/空穴对的分离效率,提高了其可见光催化活性。     

含Sr2+和Bi3+有机杂化体的合成及其光降解罗丹明B

采用溶剂热法在N,N-二甲基甲酰胺溶液中合成了不同摩尔比例的SrCl_2和Bi(NO_3)_3(分别为5%,10%,30%,50%,80%)与对苯二甲酸形成的含Sr~(2+)和Bi~(3+)有机杂化体,并在紫外可见光照射下对其进行了罗丹明B降解活性的评价.结果表明:杂化体在紫外可见光下对RhB降解活性良好,其中SrCl_2摩尔比例10%掺杂的催化剂光降解活性最佳,这归结于其在紫外区域对光有很好的吸收及光生电子和空穴能有效地分离.双金属离子能协同调节有机杂化体的光催化活性.     

Visible-light-driven Ag/Ag3PO4-based plasmonic photocatalysts: Enhanced photocatalytic performance by hybridization with graphene oxide

An efficient visible-light-driven plasmonic photocatalyst with regard to graphene oxide(GO) hybridized Ag/Ag3PO4(Ag/Ag3PO4/GO) nanostructures has been facilely synthesized via a deposition-precipitation method.The synthesized nanostructures have been characterized by means of scanning electron microscopy(SEM),energy-dispersive X-ray spectroscopy(EDX),X-ray diffraction(XRD),UV-vis spectra,Fourier transform infrared spectra(FT-IR),X-ray photoelectron spectroscopy(XPS),and Raman spectra.It has been disclosed that compared with the bare Ag/Ag3PO4 nanospecies,the GO hybridized nanostructures display enhanced photocatalytic activity for the photodegradation of methyl orange pollutant under visible-light irradiation.It is suggested that the reinforced charge transfer and the suppressed recombination of electron-hole pairs in Ag/Ag3PO4 /GO,the smaller size of Ag/Ag3PO4 nanospecies in Ag/Ag3PO4/GO,all of which are the consequences of the hybridization of GO,are responsible for the enhanced photocatalytic performance.The investigation might open up new opportunities to obtain highly efficient Ag3PO4-based visible-light-driven plasmonic photocatalyst for the photodegradation of organic pollutants.     

二氧化钛-硫化镉/氧化石墨烯复合材料光催化降解废水中有机物的研究

本论文采用溶剂热法制备出TiO₂-CdS/rGO三元复合光催化材料,并对其降解亚甲基蓝、罗丹明B的光催化活性进行研究,发现TiO₂-CdS/rGO对于亚甲基蓝、罗丹明B的光催化降解活性优于TiO₂-CdS,催化效率明显提高,降解时间大大缩短;在可见光照射下,以TiO₂-CdS/rGO为光催化剂,光反应时间40 min,亚甲基蓝、罗丹明B的降解率可达100%。本文还研究了催化材料的稳定性、催化剂用量对光催化降解效果的影响。     

pH对水热合成红磷晶体及其光催化性能的影响

以商业红磷（C-RP）为原料，NaOH溶液为调节剂，采用水热法处理C-RP获得HRP-pHx（x=5，7，9）光催化剂。选择罗丹明B （RhB）为降解对象考察HRP-pHx的光催化活性，其中HRP-pH7展现出最高的光催化活性，对RhB的降解速率常数为3.1×10^-2，是未调pH水热处理所得HRP的2.8倍。结果表明，调节pH增强RP光催化活性的主要机理是均匀的结构和较小的粒径使得HRP-pH7比HRP具有更多的活性位点。循环光降解实验结果发现HRP-pH7循环降解RhB五次后的降解率仍大于92%，体现了较好的稳定性。捕获剂实验发现光降解中起主要作用的是光生空穴和超氧基自由基。     

La掺杂对SrTiO_3纳米颗粒光催化性能的影响

采用高温固相反应法,向SrTiO_3中掺杂不同含量La制备光催化剂,通过XRD、SEM、UV-Vis等手段对其结构和形貌进行表征,并以罗丹明B(RhB)为模拟污染物,研究掺杂不同含量La所制催化剂对RhB的光催化降解能力的影响,从而评价所制催化剂的光催化性能。结果表明,随着掺La含量的增加,所制催化剂的晶体结构从SrTiO_3的立方晶系逐步向La_2Ti_2O_3的单斜晶系转变;La掺杂使得所制催化剂的禁带宽度减小、对紫外光的吸收阈值增大,使其光催化性能得到显著提升;掺La含量越高,所制催化剂的光催化性能越好。     

可见光响应WO_3光催化材料的研究进展

光催化材料在治理环境污染问题特别是大气污染和水污染方面表现出良好的应用前景。综述了可见光响应的WO_3光催化材料近些年的研究进展,指出通过调整和优化制备方法可以获得不同形貌特征的WO_3粉体光催化材料,而制备的具有大比表面积和高结晶性的WO_3粉体往往表现出高的光催化活性;跟WO_3粉体相比,WO_3薄膜实现了其在衬底表面的负载,不存在分离回收及失活等缺点,具有可观的实际应用价值,但其光催化活性有待进一步提高;通过构建异质结或形成复合材料可以提高WO_3薄膜光催化活性,也可通过贵金属单质沉积调控WO_3薄膜能带结构进而增强光催化活性;贵金属合金团簇亦可大大提高WO_3光催化活性,这一新方法为改善WO_3光催化活性的研究提供了一个新思路,具有重要应用前景。     

SiC/BiVO_4复合材料光催化降解亚甲基蓝

采用化学沉淀法制备了不同配比的SiC/BiVO_4复合材料,研究了在白炽灯照射下复合材料对亚甲基蓝的光催化降解性能.结果表明:2∶1型SiC/BiVO_4复合材料的光催化降解能力最强,光照60min时亚甲基蓝的降解率达90%;光降解反应速率常数为0.023 1/min,是纯SiC的22倍.采用X-射线衍射(XRD)、扫描电子显微镜(SEM)和紫外可见-漫反射光谱(UV-Vis DRS)表征了SiC/BiVO_4复合材料的结构和形貌特征,初步分析了亚甲基蓝的光催化降解机理.     

Nb_2O_5/CdS纳米粒子的制备及其光催化性能研究

通过简单的沉淀法合成了Nb2O5/Cd S纳米粒子,利用XRD、TEM、XPS对其进行了表征,采用制备的Nb2O5/Cd S纳米粒子在可见光照射下对罗丹明B进行了降解实验.结果表明:负载在Nb2O5表面上的Cd S粒径大小较均一,约为35 nm,在可见光照射下,Cd S质量比为20%的Nb2O5/Cd S纳米粒子光催化活性最佳,可见光照射下3 h对罗丹明B降解率为98%,经过3次循环利用,发现其具有良好的光催化稳定性.     

Low temperature hydrothermal synthesis and electrochemical performances of LiFePO4 microspheres as a cathode material for lithium-ion batteries

Mesoporous LiFePO4 microspheres were simply synthesized by a low temperature(130℃),template-free hydrothermal route using low cost LiOH,Fe(NO3)3 and NH4H2PO4 as starting raw materials.These microspheres are composed of densely aggregated LiFePO4 nanoparticles and filled with interconnected mesochannels,which demonstrates not only a high tap density(≥1.4 g cm-3),a high capacity of 150 mAh g-1(～90% of its theoretical capacity) at 0.5 C rate,but also a ≥ 80% utilization of its theoretical capacity at a high rate of 1 C.In addition,the hydrothermal synthesis developed in this work is simple and cost-effective,it may provide a new route for production of the LiFePO4 material in battery applications.     

Synthesis of ZnWO4−x nanorods with oxygen vacancy for efficient photocatalytic degradation of tetracycline

Persistent organic pollutants (POPs) especially tetracycline pose a great threat to human health, and the photocatalytic degradation of tetracycline by ZnWO4 nanomaterials has drawn much attention. To improve the photo-response range and photoactivity, we prepared ZnWO4?x sample with oxygen vacancies by solvothermally treating Zn(NO3)3 and Na2WO4 in water/ethanol/PEG-400 mixture where ethanol could act as a reducing agent to selectively remove some oxygen atoms from ZnWO4. ZnWO4?x sample is composed of nanorods with length of ~50 nm and diameter of ~20 nm. Furthermore, ZnWO4?x nanorods are brown and exhibit the obviously broadened photoabsorption from ultraviolet (UV) to near infrared (NIR) region, compared with the tradition white ZnWO4 nanorod without oxygen vacancies and with UV absorption edge of 365 nm. Under the irradiation of UV or ultraviolet-visible-near infrared (UV–Vis–NIR) light, ZnWO4?x nanorods can photocatalytically degrade 91% or 78% tetracycline, higher than those (67% or 71%) by ZnWO4 nanorods. The enhanced photocatalytic efficiency can be attributed to the introduction of oxygen vacancies which have been found to reduce photogenerated electron-hole pair recombination and narrow band gap.     

Synthesis of magnetically recoverable visible-light-induced photocatalysts by combination of Fe_3O_4/ZnO with BiOI and polyaniline

Magnetically recyclable photocatalysts with efficient performances under visible light were synthesized by combining Fe_3O_4/ZnO with BiOI and polyaniline(PANI). The FT-IR, XRD, HRTEM, SEM, EDX, XPS, UV–vis DRS,VSM, BET, and PL instruments were utilized for characterization of the as-prepared products. The activity tests exhibited that the superior rate constant in photocatalytic performance was achieved over the Fe_3O_4/ZnO/BiOI/PANI(20%) nanocomposite, which enhanced for more than 59.9, 10.0, and 6.57 times, as compared to those of the Fe_3O_4/ZnO, Fe_3O_4/ZnO/PANI, and Fe_3O_4/ZnO/BiOI photocatalysts in degradation of RhB, respectively.Successful photocatalytic degradations of MO/MB and photo reduction of Cr(VI) were also investigated to confirm the potential application of the photocatalyst in removal of various pollutants. The considerably enhanced activity pointed to a promoting effect of p-n-p heterojunctions formed between PANI, ZnO, and BiOI, and improved textural characteristics, which are benefit for improvement of the photocatalytic performances.     

Catalysis of organic pollutant photodegradation by metal phthalocyanines immobilized on TiO<Subscript>2</Subscript>@SiO<Subscript>2</Subscript>

A TiO2@SiO2 hybrid support was prepared by the sol-precipitation method using n-octylamine as a template.The photocatalyst manganese phthalocyanine tetrasulfonic acid (MnPcS) was immobilized on the support to form MnPcS-TiO2@SiO2.X-ray diffraction (XRD) and UV-Visible diffuse reflectance spectra (UV-Vis DRS) were employed to characterize the catalyst.The photocatalytic degradation of rhodamine B (RhB) and the catalytic oxidation of o-phenylenediamine (OPDA) under visible light irradiation were used as probe reactions.The mineralization efficiency and the degradation mechanism were evaluated using chemical oxygen demand (COD Cr) assays and electron spin resonance (ESR),respectively.RhB was efficiently degraded by immobilized MnPcS-TiO2@SiO2 under visible light irradiation.Complete decolorization of RhB occurred after 240 min of irradiation and 64.02% COD Cr removal occurred after 24 h of irradiation.ESR results indicated that the oxidation process was dominated by the hydroxyl radical (·OH) and superoxide radical (O-·2) generated in the system.     

WO3纳米片的制备表征及其可见光下降解罗丹明B的研究

通过水热合成法制备氧化钨（WO₃）纳米片,采用扫描电子显微镜（SEM）、固体紫外漫反射（UV-vis）和X 射线光电子能谱（SEM-EDX）对WO₃纳米片进行表征,并通过实验研究了可见光下WO₃对溶液中罗丹明B（RhB）染料废水的光催化降解性能。实验结果表明：WO₃投加量为0.10g时,在150W氙灯模拟可见光照射4h条件下,对质量浓度为10mg/L,体积为100mL罗丹明B染料废水的光催化降解率达到88.3%。此结果说明制备的WO₃催化剂对罗丹明B染料废水具有良好的光催化活性。     

Ag_2O/FACs复合材料的制备及其光催化性能

以经过酸化刻蚀改性的粉煤灰漂珠(FACs)为催化剂载体制备Ag_2O/FACs复合材料。借助SEM、XRD、FTIR、BET等对相关样品的物相结构及微观形貌进行表征,并通过亚甲基蓝(MB)溶液的光降解实验评价了所制复合材料的光催化性能。结果表明,尽管FACs改性前后的结构及化学组成差别不大,但酸化刻蚀处理能有效提高FACs的吸附性能;Ag_2O/FACs复合材料在近红外光条件下对亚甲基蓝溶液的降解率可达97.5%,并具有较高的催化稳定性;Ag_2O光生空穴在降解反应中起到重要作用。     

Photocatalytic property of TiO2 sensitized by different crystal phase CdS

TiO2 samples sensitized by different crystal phase CdS(CT) are synthesized by hydrothermal process at different reaction temperature. The samples are characterized by X-ray diffraction(XRD), transmission electron microscopy(TEM), and UV-Vis diffuse reflectance(UV-Vis). The XRD result reveals that the crystal phase of CdS is transformed from cubic phase to hexagonal phase with the increase of hydrothermal reaction temperature(120-160 ℃). The absorption edge of CT is extended from 498 nm to 546 nm. The photocatalytic degradation of rhodamin B(RhB) in aqueous solution is used to evaluate the photocatalytic activity of CT. With the increase of the preparation temperature, the photocatalytic activity of CT becomes stronger. The degradation rate of RhB by CdS/TiO2 at 160 ℃(CT-160 ℃)reaches 78%.     

光降解用WO_3-TiO_2复合光催化剂

用溶胶 凝胶法制备了纳米WO3 TiO2复合薄膜型光催化剂·利用该薄膜对罗丹明B溶液的光催化降解作用,考察了钨酸盐种类及其掺杂量、涂膜层数、溶解氧、焙烧温度、焙烧时间、基体材料等因素对光催化活性的影响·结果表明,钨酸铵加入量x(W)=1 5%、多孔钛片为基质,涂覆9层、500℃下焙烧1h得到的WO3 TiO2薄膜型复合光催化剂活性最高,其光催化活性较纯TiO2光催化剂提高1 5倍·该温度下多孔钛片负载的TiO2为锐钛矿型·     

A ternary TiO2/WO3/graphene nanocomposite adsorbent: facile preparation and efficient removal of Rhodamine B

Ternary TiO₂/WO₃/graphene (TWG) nanocomposites were prepared by a facile salt-ultrasonic assisted hydrothermal method. The products were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption-desorption. Both anatase TiO₂ and orthorhombic WO₃ formed in the nanocomposites, along with a highly disordered overlay of individual graphene nanosheets. Polyhedral and spherical TiO₂ and WO₃ nanoparticles of uniform size 10–30 nm were densely anchored to the graphene sheets. The maximum specific surface area of the products was 144.59 m²·g^?1. The products showed clear abilities for the removal of Rhodamine B in the absence of illumination. Furthermore, the adsorption activity of the products exhibited only a slight decrease after three successive cycles. The results demonstrate that the ternary nanocomposites could be used as a high-efficiency adsorbent for the removal of environmental contaminants.     

球磨法制备Bi12GeO20/WO3复合材料及可见光催化去除NO性能研究

采用简易球磨法制备了一系列Bi₁₂GeO₂₀/WO₃二元半导体复合材料,并对其物相、光学和电化学性质进行了分析。可见光光催化去除NO试验表明：随着WO₃负载量的逐渐增大,材料去除活性先增大后减小,这主要归结于合适的相组成以及异质结提高了界面载流子的分离效率。另外,WO₃的加入可有效抑制有毒中间产物NO₂的生成,从而促进硝酸根与亚硝酸根的生成。通过活性物种捕捉试验发现,超氧自由基和空穴在光催化反应中均起到了主要作用,羟基自由基起到了辅助作用。能带结构分析表明,复合材料的光催化机制遵从Ⅰ型过程。循环试验证明,材料具有较好的重复利用性和结构稳定性。     

Preparation and photocatalytic properties of ilmenite NiTiO<Subscript>3</Subscript> powders for degradation of humic acid in water

The powders of ilmenite structure NiTiO₃ were prepared by a modified Pechini process using tetrabutyl titanate and nickel acetate as raw materials, and using citric acid and ethanol as a chelating agent and a solvent respectively. The powder samples were characterized by thermogravimetric and differential thermal analysis (TG-DTA) and X-ray diffraction (XRD). The photocatalytic activity of NiTiO₃ under the irradiation of ultraviolet rays (UV) light was evaluated by degrading humic acid (HA) in water as a probe reaction. The possible photodegradation mechanism was studied by the examination of active species ·OH, ·O₂⁻, and holes (h⁺) through adding scavengers. The TG-DTA and XRD results indicated that the good crystal structure of ilmenite phase NiTiO₃ could be obtained when the Ni-Ti citrate complex was calcined at 600°C. The photocatalytic activity experiments indicated that NiTiO₃ had favourable photocatalytic activity under the irradiation of UV light, and the photocatalytic degradation rate of HA reached 95.3% after a 2.5 h reaction with the photocatalyst calcined at 600°C and a photocatalyst dosage of 0.4 g/L. The possible photocatalytic mechanism was deduced that holes (h⁺) and ·OH radicals are the major reactive active species in the photocatalytic reaction, and dissolved oxygen plays a weak role in the degradation of HA.