碘掺杂TiO2可见光光催化性能研究

在低于100℃温度条件下,采用溶胶-凝胶法以钛酸正丁酯为钛源,碘酸钾为碘源,制备了I掺杂纳米TiO2催化剂(I-TiO2),运用X-射线衍射(XRD)、透射电镜(TEM)及X-射线光电子能谱(XPS)等对催化剂进行表征,结果表明,TiO2及I-TiO2催化剂均为锐钛矿,I吸附并包裹在TiO2表面或以间隙进入的形式存在,并未进入TiO2晶格。通过在可见光照射下(λ>420 nm)以罗丹明B(Rhodamine B,RhB)的光催化降解为探针反应研究了在不同条件下制备催化剂的催化性能,结果表明,掺杂比为nI:nTi=0.05∶1,焙烧温度为400℃,降解介质条件pH=7时,I-TiO2光催化活性明显优于未掺杂的TiO2。光催化降解过程通过红外光谱(IR),总有机碳(TOC)跟踪测定,比较了TiO2掺杂前后降解RhB和对氯苯酚(4-CP)的光催化特性差异;同时采用苯甲酸荧光光度法跟踪测定体系中的氧化物种,表明在可见光下,I-TiO2光催化体系中产生.OH高活性氧化物种从而氧化降解目标化合物。     

降解菌ZQ5与紫茉莉对芘污染土壤的联合修复

在温室盆栽条件下,通过单独种植紫茉莉、单独接种多环芳烃(PAHs)模式化合物芘的专性降解菌ZQ5和两者的联合修复的3种处理,对芘污染土壤的修复效果进行了研究。结果表明,经90 d修复后,植物-微生物联合修复可将人工污染土壤中的芘降解81.1%,将石油污染土壤中的芘降解50.3%,其修复效率明显高于其他2种处理,是紫茉莉修复的1.98倍,是降解菌ZQ5修复的1.39倍。ZQ5的不同接菌量对于修复60 d后的降解率影响不大。外源生物修复条件下,10～20 cm土壤的修复效率要高于5 cm土壤;自然降解条件下,5 cm土层降解率略高于其他土层。     

四环素高效降解酵母菌Trichosporon mycotoxinivoransXPY-10降解特性

Trichosporon mycotoxinivorans XPY-10是一株分离自抗生素制药厂的高效四环素降解酵母菌。为了建立该菌株降解四环素的适宜条件,分别研究了碳源、有机氮源、金属离子等营养物质及初始底物浓度、接种量、pH、温度、装液量、摇床转速等理化因素对菌体生长及四环素降解效率的影响。结果表明,菌株XPY-10生长的最适碳源和氮源分别为蔗糖和蛋白胨。在含有0.05% FeSO₄的培养基中,菌株XPY-10降解四环素的适宜条件为：接种量2%,pH 8,温度34℃,装液量100 mL（250 mL 三角瓶）,摇床转速180 r/min。在此条件下,菌株XPY-10在7 d内对初始浓度为600 mg/L的四环素降解率为83.63%。本菌株对养殖废水及制药废水中四环素的污染治理有一定的应用前景。     

Coffee husk composting: An investigation of the process using molecular and non-molecular tools

Various parameters were measured during a 90-day composting process of coffee husk with cow dung (Pile 1), with fruit/vegetable wastes (Pile 2) and coffee husk alone (Pile 3). Samples were collected on days 0, 32 and 90 for chemical and microbiological analyses. C/N ratios of Piles 1 and 2 decreased significantly over the 90 days. The highest bacterial counts at the start of the process and highest actinobacterial counts at the end of the process (Piles 1 and 2) indicated microbial succession with concomitant production of compost relevant enzymes. Denaturing gradient gel electrophoresis of rDNA and COMPOCHIP microarray analysis indicated distinctive community shifts during the composting process, with day 0 samples clustering separately from the 32 and 90-day samples. This study, using a multi-parameter approach, has revealed differences in quality and species diversity of the three composts.     

土壤中异黄酮植物雌激素降解体系的研究

利用睾丸酮丛毛单胞菌(菌株C.test十act5)具有消化多环芳烃类化合物这一特性,以异黄酮植物雌激素为底物筛选菌株C.test+act5降解雌激素的培养条件,使异黄酮植物雌激素在土壤中的含量相对降低,以期为高效降解环境中激素类物质奠定基础.结果表明:菌株C.test+act5降解异黄酮植物雌激素的最适质量浓度为100～200 μg/mL,最适温度为30℃,最适pH为6.0;在此条件下,降解48 h时的降解率达85％左右,72 h后几乎完全被降解.     

Photocatalytic degradation of bentazone in soil washing wastes containing alkylpolyoxyethylene surfactants

Three alkylpolyoxyethylene surfactants bearing the same hydrophobic chain and a different number of oxyethylene groups were investigated as suitable candidates for the soil washing treatment of contaminated soil samples containing bentazone. Comparable good recoveries of the pesticide were obtained working with these surfactants. The photocatalytic treatment of the collected washing wastes, performed in the presence of suspended TiO₂ particles under irradiation with simulated sunlight, leads to the effective degradation of bentazone residues after a time depending on the nature and concentration of the chosen amphiphile. Brij 35 was found to be the best surfactant candidate, giving the faster abatement of the pesticide in the collected wastes. The overall treatment time depends on the bentazone mineralization kinetics, markedly slow in the presence of surfactants. Useful information about the photocatalytic degradation route was obtained from the HPLC-MS analysis of transient intermediates formed in water.     

Aerobic degradation of tetrabromobisphenol-A by microbes in river sediment

This study investigated the aerobic degradation of tetrabromobisphenol-A (TBBPA) and changes in the microbial community in river sediment from southern Taiwan. Aerobic degradation rate constants (k₁) and half-lives (t_1/2) for TBBPA (50 μg g⁻¹) ranged from 0.053 to 0.077 d⁻¹ and 9.0 to 13.1 d, respectively. The degradation of TBBPA (50 μg g⁻¹) was enhanced by adding yeast extract (5 mg L⁻¹), sodium chloride (10 ppt), cellulose (0.96 mg L⁻¹), humic acid (0.5 g L⁻¹), brij 30 (55 μM), brij 35 (91 μM), rhamnolipid (130 mg L⁻¹), or surfactin (43 mg L⁻¹), with rhamnolipid yielding a higher TBBPA degradation than the other additives. For different toxic chemicals in the sediment, the results showed the high-to-low order of degradation rates were bisphenol-A (BPA) (50 μg g⁻¹) > nonylphenol (NP) (50 μg g⁻¹) > 4,4′-dibrominated diphenyl ether (BDE-15) (50 μg g⁻¹) > TBBPA (50 μg g⁻¹) > 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209) (50 μg g⁻¹). The addition of various treatments changed the microbial community in river sediments. The results also showed that Bacillus pumilus and Rhodococcus ruber were the dominant bacteria in the process of TBBPA degradation in the river sediments.     

Effects of excited-state structures and properties on photochemical degradation of polybrominated diphenyl ethers: a TDDFT study

This study presents new insight into the photochemical degradation of polybrominated diphenyl ethers (PBDEs), and it provides details about the structures and properties of 27 PBDE congeners in the electronically excited state using the time-dependent density functional theory method. Each PBDE congener exhibited remarkably different geometries in the ground state and the excited state. The significant lengthening of C-Br bond in each PBDE congener was observed in the excited state for the first time by theoretical calculation, which is directly involved in the photochemistry reductive debromination of n-BDE to (n−1)-BDE. Generally, the lengthening of C-Br bonds cannot occur at the para position. Furthermore, the calculated results demonstrated that the photoreactivity of PBDEs increased with an increase of bromination degree. It was also found that the pattern of Br substituents had an effect upon the photoreactivity of PBDEs. These findings suggest that the information obtained in the excited state is crucial to the mechanism explanation of the photochemical degradation of PBDEs.     

Conductive-diamond electrochemical oxidation of chlorpyrifos in wastewater and identification of its main degradation products by LC-TOFMS

The electrochemical transformation of the organophosphorous insecticide chlorpyrifos (CPF) was investigated in wastewater. The oxidation of CPF was carried out in a single-compartment electrochemical flow cell working under batch operation mode, using diamond-based material as anode and stainless steel as cathode. In order to evaluate its persistence and degradation pathway, two different concentration levels (1.0 mg L⁻¹ and 0.1 mg L⁻¹) were studied. Liquid chromatography/mass spectrometry was used for evaluation of the initial and electrolyzed solutions. The identification of CPF transformation products was performed by liquid chromatography-time of flight-mass spectrometry (LC-TOFMS). Results showed that CPF is completely removed at the end of treatment time. Analysis by LC-TOFMS allowed the identification of six degradation products (with Mw 154, 170, 197, 305 321 and 333). Three of the identified intermediates (Mw 170, 305 and 321) were completely removed at the end of electrolysis time. Interestingly, the formation of diethyl 3,5,6-trichloropyridin-2yl phosphate (chlorpyrifos oxon) and 3,5,6-trichloropyridin-2-ol was also found in previous reported degradation pathways using different degradation technologies.     

SO_4~（2-）/TiO_2光催化降解苯酚

以工业硫酸氧钛为原料水解制得SO42-/TiO2光催化剂,并以苯酚为目标降解物,考察了SO24-/TiO2的光催化性能。结果表明：随着SO42-/TiO2制备过程中焙烧温度的升高,其光催化活性逐渐增加,650℃焙烧获得的SO24-/TiO2的光催化活性最好,此后再升高温度会因催化剂中硫的挥发而下降;在确定苯酚原液初始浓度为50 mg/L条件下,SO42-/TiO2的光催化降解苯酚的最佳工艺条件为反应时间2 h、苯酚pH为7、催化剂用量1 g/L。XRD、SEM和FTIR的分析结果显示实验温度下制得的SO42-/TiO2均为锐钛型TiO2;其间掺杂的SO24-在TiO2表面分散性较好,没有聚集成大的颗粒;红外分析的结果初步判定低温（〈550℃）焙烧制得的催化剂SO42-在TiO2表面是螯合双配位吸附,高温焙烧时（〉550℃）SO42-在TiO2表面是桥式配位吸附。