Mesoporous WO3-graphene photocatalyst for photocatalytic degradation of Methylene Blue dye under visible light illumination

Advanced oxidation technologies are a friendly environmental approach for the remediation of industrial wastewaters. Here, one pot synthesis of mesoporous WO_3 and WO_3-graphene oxide(GO) nanocomposites has been performed through the sol–gel method. Then, platinum(Pt) nanoparticles were deposited onto the WO_3 and WO_3-GO nanocomposite through photochemical reduction to produce mesoporous Pt/WO_3 and Pt/WO_3-GO nanocomposites. X-ray diffraction(XRD) findings exhibit a formation of monoclinic and triclinic WO_3 phases. Transmission Electron Microscope(TEM) images of Pt/WO_3-GO nanocomposites exhibited that WO_3 nanoparticles are obviously agglomerated and the particle sizes of Pt and WO_3 are ~ 10 nm and 20–50 nm, respectively. The mesoporous Pt/WO_3 and Pt/WO_3-GO nanocomposites were assessed for photocatalytic degradation of Methylene Blue(MB) as a probe molecule under visible light illumination.The findings showed that mesoporous Pt/WO_3, WO_3-GO and Pt/WO_3-GO nanocomposites exhibited much higher photocatalytic efficiencies than the pure WO_3. The photodegradation rates by mesoporous Pt/WO_3-GO nanocomposites are 3, 2 and 1.15 times greater than those by mesoporous WO_3, WO_3-GO, and Pt/WO_3, respectively. The key factors of the enhanced photocatalytic performance of Pt/WO_3-GO nanocomposites could be explained by the highly freedom electron transfer through the synergetic effect between WO_3 and GO sheets, in addition to the Pt nanoparticles that act as active sites for O2 reduction, which suppresses the electron hole pair recombination in the Pt/WO_3-GO nanocomposites.     

Photodegradation of acetochlor in water and UV photoproducts identified by mass spectrometry

The sunlight photodegradation half-lives of 20 mg/L acetochlor were 151, 154 and 169 days in de-ionized water, river water and paddy water, respectively. When exposed to ultraviolet (UV) light, acetochlor in aqueous solution was rapidly degraded. The half-lives were7.1, 10.1, and 11.5 min in de-ionized water, river water and paddy water, respectively. Photopreduets of acetochlor were identified by gas chromatography/mass spectrometry(GC/MS) and found at least twelve photoproducts resulted from dechlorination with subsequent hydrtrxylation and cyclization processes. The chemical structures of ten photoproducts were presumed on the basis of mass spectrum interpretation and literature data. Photoproducts are identified as 2-ethyl-6-methylaniline; N, N-diethylaniline ; 4, 8-dimethyl-2-oxo- 1,2,3,4- tetrahydroquino-line; 2-oxo-N-(2-ethyl-6-methylphenyl)-N-(ethoxymethyl) acetamide; N-(ethoxymethyl)-2‘-ethyl-6‘-methylformanilide; 1-hydroxyaeetyl-2-ethoxyl-7-ethylind ole; 8-ethyl-l-ethoxymethyl-2-oxo-1, 2, 3, 4-tetrahydroquinoline; 4, 8-dimethyl-l-ethoxymethyl-2-oxo-1, 2, 3, 4-tetrahydroquinoline; 2-hydroxy-2‘-ethyl-6‘-methyl-N-(ethoxymethyl) acetanilide and a compound related to acetochlor. The other two photoproducts were detected by GC/MS although their chemical structure was unknown.     

水环境中碳纳米管对沙丁胺醇光降解的影响

选取沙丁胺醇(salbutamol,SAL)为目标污染物,研究了3种碳纳米管(CNTs,单壁碳纳米管SCNT、羟基衍生化多壁碳纳米管MWNT-OH和羧基衍生化多壁碳纳米管MWNT-COOH)对有机污染物在模拟太阳光照下降解的影响;并且研究了CNTs与天然水体中光活性物质三价铁离子(Fe3+)的相互作用.结果表明,3种CNTs能够通过竞争吸收光子,即光屏蔽作用抑制SAL光解;同时又能通过光致激发产生单线态氧(1O2)促进光解反应,两种作用机制同时存在,在绝大多数情况下,抑制作用占主导地位.此外,CNTs还能通过静电吸附作用使水体中的光活性物质Fe3+失活,从而影响有机污染物在天然水体中的光化学行为.     

Ag-AgI/CN/MA复合物的制备及其可见光催化性能

采用沉淀法和热聚合法分别将AgI、氮化碳(CN)负载在介孔γ-Al_2O_3(MA)上,并通过光还原银离子成功制备了等离子体诱导可见光催化剂Ag-AgI/CN/MA.利用X射线衍射(XRD)、X射线光电子能谱(XPS)、场发射扫描电子显微镜(FESEM)、紫外可见漫反射光谱(UV-vis DRS)和透射电子显微镜(TEM)对Ag-AgI/CN/MA复合材料进行表征,并对其在可见光照射下(λ420 nm)的光催化性能进行了研究,考察了初始溶液pH值及催化剂投加量等条件对光催化反应的影响.结果表明,表面银以Ag+和Ag0形式共存,并且Ag和AgI均匀地分散在CN的表面.与CN和Ag-AgI/MA相比,Ag-AgI/CN/MA复合物对甲基橙(MO)具有更高的可见光催化降解效率,且反应过程中Ag+的释放量显著减少,显示出良好的稳定性.当溶液pH值为7、催化剂投加量为1 g·L~(-1)时,Ag-AgI/CN/MA-2显示出最优的催化性能.同时,其对罗丹明B(Rh B)、甲基红(MR)和刚果红(CR)等不同电性的染料均体现出良好的催化性能.     

水体中甲基汞光化学降解特征研究

为探究水体中甲基汞（MMHg）的光化学行为,采用室内模拟实验,以不同波长紫外灯及室内可见光为光源,探讨紫外光波长、光强度等因素对MMHg光降解的影响,并根据生成物Hg0的量变化分析MMHg光降解反应历程.研究表明,MMHg光降解最终产物中含有Hg0,且光照条件对MMHg光降解速率、Hg0的产量有影响.在反应器暴露于紫外光条件下时,MMHg光降解速率随紫外光波长的变短而增加,随紫外光强度的提高而增加,且MMHg光降解呈一级动力学反应,速率常数分别为KUVA 0.403～0.562 h-1、KUVB 0.961 h-1、KUVC 1.221 h-1和KVL＋UVA＋UVB 1.346 h-1;Hg0释放通量为0.166～0.392 ng·min-1.当反应器暴露于可见光条件下时,反应器内MMHg浓度下降速率较慢,KVL0.061 h-1;Hg0释放通量为0.008 ng·min-1.而在黑暗条件下没有发现反应器内MMHg浓度下降,无Hg0生成.可见紫外光是导致MMHg降解的主要原因,光波波长与强度对MMHg的环境地球化学行为有重要影响.     

阿替洛尔在硝酸根溶液中的光降解研究

以氙灯为模拟太阳光光源,研究了β阻滞剂阿替洛尔(ATL)在硝酸根溶液中的光解,探讨了硝酸根离子浓度、溶液pH值、碳酸氢根离子浓度和腐殖质浓度对ATL光解的影响.结果表明,ATL在不同浓度硝酸根溶液中的光解反应符合准一级动力学规律,增大硝酸根离子浓度促进了ATL的光降解率,当硝酸根离子浓度由0增至5 mmol.L-1时其速率常数由0.002 26min-1增至0.009 4 min-1;酸性或碱性溶液有利于ATL在硝酸根溶液中的光解,碳酸氢根离子浓度对光解无明显影响,而加入Suwannee富里酸(SRFA)对光解产生抑制作用.采用异丙醇作为羟基自由基分子探针检测到.OH存在于ATL光解过程中.采用SPE-LC-MS方法鉴定了ATL在硝酸根溶液中的主要光解产物,并提出了可能的光解途径.     

水热法制备BiVO4及其可见光催化降解糖蜜酒精废水

以Bi(NO3)3•5H2O为铋源,NH4VO3为钒源,采用简单的水热法制备了BiVO4 光催化剂,并用X-射线衍射(XRD)、扫描电子显微镜(SEM)、红外光谱(IR)和紫外-可见光漫反射光谱(UV-vis)对产品进行了结构表征。同时,在BiVO4光催化降解糖蜜酒精废水反应中考察了催化剂用量、通氧量、溶液pH值、双氧水用量及光照强度对糖蜜酒精废水脱色率的影响。实验结果表明,水热产品属于单斜晶系BiVO4,其带隙能为2.398 eV,并具有良好的可见光催化活性。当降解经30倍稀释的糖蜜酒精废水,BiVO4添加量为3.0 g•L−1 ,通氧量为120 L•h-1,助氧化剂H2O2添加量为9 %,不改变废水pH值,在400W镝灯离液面11cm照射反应180 min的条件下,糖蜜酒精废水的脱色率为88.60 %,COD去除率为25.84%,而添加5g•L−1的FeSO4•7H2O后其脱色率和COD去除率分别提高到90.90 %和91.26%。单斜晶型BiVO4晶体的可见光催化糖蜜酒精废水过程符合一级动力学反应。     

Effects of Cu（Ⅱ） and humic acid on atrazine photodegradation

This work was designed to explore the characteristics of photodegradation of herbicides in the copper-polluted water body. The results showed that Cu(II) alone could induce a photo Fenton-like reaction to enhance the degradation of atrazine, in which hydroxyl radical ( OH) was a main active species. Humic acids restrained atrazine degradation, nevertheless, when introducing Cu(II), the photodegradation was accelerated, in which singlet oxygen (1O2) replaced OH acting as the prevailing species. A feasible mechanism for the photochemical process was also proposed, which is helpful for better understanding the environmental photochemistry of atrazine in the copper-polluted water.     

Potential particulate pollution derived from UV-induced degradation of odorous dimethyl sulfide

UV-induced degradation of odorous dimethyl sulfide (DMS) was carried out in a static White cell chamber with UV irradiation. The combination of in situ Fourier transform infrared (FT-IR) spectrometer, gas chromatograph-mass spectrometer (GC-MS), wide-range particle spectrometer (WPS) technique, filter sampling and ion chromatographic (IC) analysis was used to monitor the gaseous and potential particulate products. During 240 min of UV irradiation, the degradation e ciency of DMS attained 20.9%, and partially oxidized sulfur-containing gaseous products, such as sulfur dioxide (SO2), carbonyl sulfide (OCS), dimethyl sulfoxide (DMSO), dimethyl sulfone (DMSO2) and dimethyl disulfide (DMDS) were identified by in situ FT-IR and GC-MS analysis, respectively. Accompanying with the oxidation of DMS, suspended particles were directly detected to be formed by WPS techniques. These particles were measured mainly in the size range of accumulation mode, and increased their count median diameter throughout the whole removal process. IC analysis of the filter samples revealed that methanesulfonic acid (MSA), sulfuric acid (H2SO4) and other unidentified chemicals accounted for the major non-refractory compositions of these particles. Based on products analysis and possible intermediates formed, the degradation pathways of DMS were proposed as the combination of the O(1D)- and the OH- initiated oxidation mechanisms. A plausible formation mechanism of the suspended particles was also analyzed. It is concluded that UV-induced degradation of odorous DMS is potentially a source of particulate pollutants in the atmosphere.     

水体中锰离子对酚类有机物的光化学降解的影响

通过对不同锰离子浓度下三种酚在三种不同介质中的光降解情况的研究,来确定水体中的锰离子对酚类有机物的光化学降解的影响。实验结果表明,在不同条件下,不同浓度的锰离子对实验中所选的三种酚的影响有所不同。对邻硝基苯酚的光降解几乎不产生影响,对对甲基苯酚的光降解起到抑制作用,而对2,4-二硝基苯酚的光降解则起到促进作用。