钛酸四丁酯水解制备TiO_2半导体光催化剂研究

研究了钛酸四丁酯水解制备TiO2 粉末的两大影响因素R值 (R是水和钛酸四丁酯的摩尔比 )和烧结温度 .通过光催化氧化五氯苯酚钠实验 ,结合对催化剂晶型结构、比表面积的表征分析 ,综合评价所制备的催化剂 .实验结果表明 ,当R =10 0、烧结温度为 6 5 0℃、烧结时间为 1h ,钛酸四丁酯水解所制备的TiO2 半导体光催化剂催化活性和使用寿命均比较理想 .从晶型结构分析 ,当催化剂中锐钛矿和金红石按一定比例共存时 ,其催化活性较单一金红石或锐钛矿高 .实验认为锐钛矿与金红石的最佳比约为 2∶1     

钛酸四丁酯水解制备TiO2光催化氧化五氯苯酚钠

为制备高效、实用的TiO2半导体光催化剂,通过光催化氧化五氯苯酚钠实验,结合对催化剂晶型结构、比表面积的表征分析,研究了钛酸四丁酯水解制备TiO2粉末的两大影响因素R值(R是水和钛酸四丁酯的摩尔比)和烧结温度.实验结果表明,当R=100、温度为650℃烧结1h,钛酸四丁酯水解所制备的TiO2粉末光催化活性和使用寿命均比较理想.用R100-650型催化剂做光催化实验,当反应液初始五氯苯酚钠(PCP-Na)浓度为100 mg/L、pH值为6.5,TiO2投加量为2 g/L,光照强度为30W/m2时,五氯苯酚钠2 h光催化氧化率达95.5%.     

高效负载型光催化剂制备及其加铂修饰技术

通过光催化氧化五氯苯酚钠实验,结合对催化剂晶型结构、比表面积的表征分析,优化钛酸四丁酯水解制备TiO₂负载型催化剂并加铂修饰的制备条件:R值、烧结温度、粘合剂添加量、空心玻璃珠粒径大小及催化剂中铂含量,从而制备出高效、实用的负载加铂修饰型半导体光催化剂.实验结果表明,当R=10,温度为650℃烧结1h,TiO₂∶硅酸钠∶空心玻璃珠=10∶2.5∶20(W),铂在催化剂中的重量百分比为1.4%～1.6%,空心玻璃珠的粒径为0.5mm时,所制备的加铂修饰负载型催化剂催化活性、使用寿命和牢固度均比较理想.用该催化剂做光催化实验,当反应液初始五氯苯酚钠浓度为100mg/L、pH值为6.5,催化剂投加量为2g/L,通氧气量为1.6mL/s,光照强度为30kW/m²时,五氯苯酚钠2 h光催化氧化率达92.0%.     

稀土掺杂TiO2膨润土光催化降解中性红的研究

文章主要以膨润土为载体,钛酸正四丁酯和硫酸高铈为原料,采用溶胶-凝胶法制备稀土掺杂TiO2膨润土复合光催化剂,用XRD和SEM对稀土掺杂TiO2膨润土的结构和形貌进行表征,表征结果表明其具有很高的比表面积,并且存在明显的锐钛矿型TiO2晶型特征峰.研究催化剂的用量、染料的初始浓度、光照时间、pH值等因素对中性红染料脱色...     

制备条件对低温NH_3-SCR脱硝催化剂Mn-Ce/TiO_2结构与性能的影响

采用溶胶凝胶法制备了Mn-Ce/TiO2催化剂,以NH3为还原剂,通过程序升温反应考察其选择性催化还原NO的催化性能.同时,着重探讨了焙烧温度、焙烧时间、活性物质负载量及Mn、Ce负载比例对催化剂结构和性能的影响,并用BET、XRD等对催化剂进行了表征.结果表明,活性组分负载量由0增至20%时,NO转化率随着负载量的增加而提高,当(Mn+Ce)质量分数为20%,催化剂活性最高,此后随着活性组分负载量的增加,NO转化率明显下降;Mn与Ce的负载比例为0.85∶0.15时,催化剂比表面积最大,为112.31m2·g-1;焙烧温度500℃时催化剂晶相均为TiO2锐钛矿型结构,焙烧温度升高至600℃,催化剂晶相为TiO2锐钛矿型和金红石型混合结构,且催化剂比表面积急剧减小;焙烧时间对催化剂晶相结构影响不大,焙烧时间为5h时,Mn-Ce/TiO2的脱硝性能最好.     

纳米TiO2/硅藻土光催化降解蒽醌染料废水的研究

为提高光催化剂的稳定性,选取硅藻土为载体,以钛酸四异丙酯为前驱物,采用溶胶-凝胶法制备了TiO2/硅藻土光催化剂,并利用XRD、SEM、FT-IR等技术对其进行表征.以蒽醌染料弱酸性艳蓝RAW为目标降解物,考察了TiO2/硅藻土的光催化活性、最佳pH值范围及催化剂重复使用对光催化活性的影响.结果表明,所制备的TiO2为锐钛矿和金红石混晶型,平均粒径11nm,通过控制硅藻土加入量可以得到负载均匀的光催化剂.所制备的TiO2/硅藻土具有较强的光催化活性,对弱酸性艳蓝RAW的降解效果好于商品Degussa P25型TiO2,最佳pH值为4.0.该催化剂性质稳定,重复使用15次后,催化活性仅降低12.4%.     

不同煅烧温度制备TiO_2及光解2-氯苯甲酸

为了考察煅烧温度对TiO2结构和光催化活性的影响,以酞酸丁酯作为前驱体,利用溶胶-凝胶法在不同煅烧温度下制备TiO2,并用亚甲基蓝测试其光催化活性。TG热重分析表明,450~700℃时TiO2有晶型变化,XRD表征说明,TiO2晶型受煅烧温度影响显著,其中450~600℃煅烧制备的TiO2为锐钛矿型,650℃煅烧时TiO2出现金红石晶型;亚甲基蓝光解实验结果表明,煅烧温度显著影响TiO2的光催化活性,其中,450~600℃煅烧TiO2对亚甲基蓝光解效果较好,光降解2.5h后降解率高达95%~97%;550℃煅烧制备的锐钛矿型TiO2对2-氯苯甲酸有一定光解催化效果,紫外光解4h后降解率高达80%左右,光解过程符合零级动力学模式。     

负载型活性炭/TiO2光催化降解苯酚的研究

在温和条件下(75℃和常压),通过在酸性水溶液中水解钛酸四丁酯并回流提高其结晶度,制备了锐钛矿型的TiO2.将此TiO2负载于粉末活性炭上,并用之来降解模拟废水苯酚.实验结果表明,该负载型催化剂的光催化效果要优于纯TiO2以及P25 TiO2加活性炭的混合体系.0.58g负载型催化剂降解0.4L浓度为100mg·L-1的苯酚溶液,经18W紫外灯光照6h后溶液中的苯酚去除率达到98%.同时,载体活性炭上吸附的苯酚量也随着光照时间逐渐减少,6h后残留的量仅为初始值的3.5%.     

邻-氯酚在TiO_2膜上光催化降解及反应动力学特征

以钛酸四丁酯为原料采用Sol Gel法制备了玻璃负载TiO2 膜光催化剂 ,应用XRD表征了不同实验条件下薄膜中TiO2 的晶相结构和粒度。分析了不同层数TiO2 膜的光催化活性和溶液 pH值对邻 氯酚 (2 CP)的影响。结果表明 :处理温度为 50 0℃时不同厚度薄膜中TiO2 均为锐钛矿晶型 ,粒径 8～ 33nm ,5层涂膜光催化活性最高。在高 pH值和低pH值区域 2 CP ,在TiO2 膜上的光催化降解速率较大。 2 CP初始浓度 (C0 )与反应速率 (r0 )的关系符合Langmuir Hinshelwood方程 ,当C0 ≤ 0 .6mmol·L- 1 时 ,降解反应可用一级动力学模式来描述。     

纳米TiN制备可见光活性TiO_2光催化剂的研究

在O2/N2混合气氛中煅烧TiN纳米粒子,制备出了一种响应可见光的氮掺杂TiO2光催化剂(TiO2-xNx)。紫外-可见吸收光谱表明,该光催化剂在可见光区具有明显的吸收。该光催化剂的XRD图谱表明,TiO2-xNx的晶型为锐钛矿相和金红石相的混合相。甲基橙溶液的降解实验结果表明,在O2/N2比例为1∶15(体积比),通氧时间为15 min,煅烧温度为650°C时,制得的催化剂活性最高。     

Toxic effects of acetochlor, methamidophos and their combination on nifH gene in soil

Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis （DGGE） and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity （both in gene richness and diversity index values） and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor （50 mg/kg） recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos （150 mg/kg） caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos （250 mg/kg） produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes （bands） responded differently to the impact of agrochemicals： four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.     

Arsenic uptake by arbuscular mycorrhizal maize （Zea mays L.） grown in an arsenic-contaminated soil with added phosphorus

The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.     

Removal of heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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Organochlorine pesticides in soils under different land usage in the Taihu Lake region, China

A field study was conducted in the Taihu Lake region, China in 2004 to reveal the organochlorine pesticide concentrations in soils after the ban of these substances in the year 1983. Thirteen organochlorine pesticides (OCPs) were analyzed in soils from paddy field, tree land and fallow land. Total organochlorine pesticide residues were higher in agricultural soils than in uncultivated fallow land soils. Among all the pesticides, ΣDDX (DDD, DDE and DDT) had the highest concentration for all the soil samples, ranging from 3.10 ng/g to 166.55 ng/g with a mean value of 57.04 ng/g and followed by ΣHCH, ranging from 0.73 ng/g to 60.97 ng/g with a mean value of 24.06 ng/g. Dieldrin, endrin, HCB and α-endosulfan were also found in soils with less than 15 ng/g. Ratios of p,p'-(DDD DDE)/DDT in soils under three land usages were: paddy field ＞ tree land ＞ fallow land, indicating that land usage inlfuenced the degradation of DDT in soils. Ratios of p,p'-(DDD DDE)/DDT ＞1, showing aged residues of DDTs in soils of the Taihu Lake region. The results were discussed with data from a former study that showed very low actual concentrations of HCH and DDT in soils in the Taihu Lake region, but according to the chemical half-lives and their concentrations in soils in 1980s, the concentration of DDT in soils seemed to be underestimated. In any case our data show that the ban on the use of HCH and DDT resulted in a tremendous reduction of these pesticide residues in soils, but there are still high amounts of pesticide residues in soils, which need more remediation processes.     

Single and joint effects of pesticides and mercury on soil urease

The influence of two pesticides including chlorimuron-ethyl and furadan and mercury （Hg） on urease activity in 4 soils （meadow burozem and phaeozem） was investigated. The soils were exposed to various concentrations of the two pesticides and Hg individually and simultaneously. Results showed that there was a close relationship between urease activity and organic matter content in soil. Chlorimuron-ethyl and furadan could both activate urease in the 4 soils. The maximum increment of urease activity by chlorimuronethyl was up to 14%-18%. There was almost an equal increase （up to 13%-21%） in the urease activity by furadan. On the contrary, Hg markedly inhibited soil urease activity. A logarithmic equation was used to describe the relationship （P〈0.05） between the concentration of Hg and the activity of soil urease in the 4 tested soils. Semi-effect dose （ED50） values by the stress of Hg based on the inhibition of soil urease in the 4 soils were 88, 5.5, 24 and 20 mg/kg, respectively, according to the calculation of the corresponding equations. The interactive effect of chlorimuron-ethyl or furadan with metal Hg on soil urease was mainly synergic at the highest tested concentrations.     

Isolation and preliminary characterization of a 3-chlorobenzoate degrading bacteria

A study was conducted to compare the diversity of 2-, 3-, and 4-chlorobenzoate degraders in two pristine soils and one contaminated sewage sludge. These samples contained strikingly different populations of mono-chlorobenzoate degraders. Although fewer cultures were isolated in the uncontaminated soils than contaminated one, the ability of microbial populations to mineralize chlorobenzoate was widespread. The 3- and 4-chlorobenzoate degraders were more diverse than the 2-chlorobenzoate degraders. One of the strains isolated from the sewage sludge was obtained. Based on its phenotype, chemotaxonomic properties and 16S rRNA gene, the organism S-7 was classified as Rhodococcus erythropolis. The strain can grow at temperature from 4 to 37℃. It can utilize several （halo）aromatic compounds. Moreover, strain S-7 can grow and use 3-chlorobenzoate as sole carbon source in a temperatures range of 10-30℃ with stoichiometric release of chloride ions. The psychrotolerant ability was significant for bioremediation in low temperature regions. Catechol and chlorocatechol 1,2-dioxygenase activities were present in cell free extracts of the strain, but no （chloro）catechol 2,3- dioxygenase activities was detected. Spectral conversion assays with extracts from R. erythropolis S-7 showed accumulation of a compound with a similar UV spectrum as chloro-cis,cis-muconate from 3-chlorobenzoate. On the basis of these results, we proposed that S-7 degraded 3-chlorobenzoate through the modified ortho-cleave pathway.     

Alterations of organ histopathology and metallolhionein mRNA expression in silver barb, Puntius gonionotus during subchronic cadmium exposure

Common silver barb,Puntius gonionotus,exposed to the nominal concentration of 0.06 mg/L Cd for 60 d,were assessed for histopathological alterations(gills,liver and kidney),metal accumulation,and metallothionein(MT)mRNA expression.Fish exhibited pathological symptoms such as hypertrophy and hyperplasia of primary and secondary gill lamellae,vacuolization in hepatocytes,and prominent tubular and glomerular damage in the kidney.In addition,kidney accumulated the highest content of cadmium,more than gills and liver.Expression of MT mRNA was increased in both liver and kidney of treated fish.Hepatic MT levels remained high after fish were removed to Cd-free water.In contrast,MT expression in kidney was peaked after 28 d of treatment and drastically dropped when fish were removed to Cd-free water.The high concentrations of Cd in hepatic tissues indicated an accumulation site or permanent damage on this tissue.     

Sorption of 1-naphthol by plant cuticular fractions

The contribution of aliphatic-rich plant biopolymer to sorption of hydrophobic organic compounds is significantly important because of their preservation and accumulation in the soil environment,but sorption mechanism is still not fully understood.In this study, sorption of 1-naphthol by plant cuticular fractions was examined to better understand the contributions of respective fraction.Toward this end,cuticular materials were isolated from the fruits of tomato by chemical method.The tomato cuticle sheet consisted of waxes (6.5 wt%),cuticular monomer (69.5 wt%),and polysaccharide (24.0 wt%).Isotherms of l-naphthol to the cuticular fractions were nonlinear (N value (0.82-0.90)) at the whole tested concentration ranges.The KodKow ratios for bulk cuticle (TC1),dewaxed cuticle (TC2),cutin (TC4),and desugared cuticle (TC5) were larger than unity,suggested that tomato bulk cuticle and cutin are much powerful solption medium.Sorption capability of cutin (TC4) was 2.4 times higher than the nonsaponifiable fraction (TC3).The 1-naphthol interactions with tomato cuticular materials were governed by both hydrophobic-type interactions and polar (H-bonding) interactions. Removal of the wax and polysaccharide materials from the bulk tomato cuticle caused a significant increase in the sorption ability of the cuticular material.There was a linear negative trend between K_(oc) values and the amount of polysaccharides or fraction's polarities ((N O)/C);while a linear positive relationship between K_(oc) values and the content of cutin monomer (linear R~2=0.993) was observed for present in the cuticular fractions.Predominant sorbent of the hydrophobic organic compounds (HOCs) in the plant cuticular fraction was the cutin monomer,contributing to 91.7% of the total sorption of tomato bulk cuticle.     

Seed selections for crystallization of calcium phosphate for phosphorus recovery

Seed induces and promotes the crystallization of calcium phosphate, and acts as carrier of the recovered phosphorus （P）. In order to select suitable seed for P recovery from wastewater, three seeds including Apatite （AP）, Juraperle （JP） and phosphate-modified Juraperle （M-JP） were tested and compared. Batch and fixed-bed column experiments of seeded crystallization of calcium phosphate were undertaken by using synthetic wastewater with 10 mg/L P phosphate. It shows that AP has bad enduring property in the crystallization process, while JP has better performance for multiple uses, and M-JP is a hopeful seed for P recovery by crystallization of calcium phosphate.