铜铈复合氧化物上石化行业典型VOCs的氧化行为与动力学

采用共沉淀法和等体积浸渍法制备了CuCeO x复合催化剂,对材料的物化性质进行了XRD、低温N2吸脱附、H2-TPR和O2-TPD表征.以石化行业典型VOCs(苯、甲苯和正己烷)为探针污染物,研究了污染物组成与浓度、反应空速、O2浓度、H2O浓度和催化剂种类对其氧化行为的影响,并对反应动力学参数进行了模型拟合.共沉淀得到的催化剂具有均匀的活性相、好的低温可还原性能和较多的活性表面氧物种.甲苯氧化率随着污染物浓度升高而降低,高转化率下苯浓度与其氧化率无相关性,正己烷的氧化率与入口浓度呈正比.苯能够显著抑制甲苯的氧化,而甲苯加入有利于苯的氧化.正己烷对苯氧化的影响较小,但能够促进甲苯的转化,苯系物对正己烷氧化有明显的抑制作用.低空速和高氧浓度都有利于污染物的氧化,氧浓度的变化对正己烷和苯的氧化影响较小.水汽对甲苯的氧化有明显的抑制作用,而对苯和正己烷氧化有明显的促进作用.共沉淀催化剂具有更好的甲苯和苯氧化性能,而无水条件下浸渍催化剂具有更好的正己烷氧化性能.拟一级动力学模型能够很好地模拟不同条件下污染物的氧化行为.     

Acid-assisted hydrothermal synthesis of nanocrystalline TiO2 from titanate nanotubes: Influence of acids on the photodegradation of gaseous toluene

In order to efficiently remove volatile organic compounds (VOCs) from indoor air, onedimensional titanate nanotubes (TiNTs) were hydrothermally treated to prepare TiO₂ nanocrystals with different crystalline phases, shapes and sizes. The influences of various acids such as CH₃COOH, HNO₃, HCl, HF and H₂SO₄ used in the treatment were separately compared to optimize the performance of the TiO₂ nanocrystals. Comparedwith the strong and corrosive inorganic acids, CH₃COOH was not only safer andmore environmentally friendly, but also more efficient in promoting the photocatalytic activity of the obtained TiO₂. Itwasobserved that the anatase TiO₂ synthesized in 15 mol/L CH₃COOH solution exhibited the highest photodegradation rate of gaseous toluene (94%), exceeding that of P25 (44%) by a factor ofmore than two. The improved photocatalytic activity was attributed to the small crystallite size and surface modification by CH₃COOH. The influence of relative humidity (20%-80%) on the performance of TiO₂ nanocrystals was also studied. The anatase TiO₂ synthesized in 15 mol/L CH₃COOH solution was more tolerant tomoisture than the other TiO₂ nanocrystals and P25.     

矾土尾矿载体双活性组分甲苯催化燃烧催化性能研究

利用矾土尾矿制备催化剂载体,采用浸渍法将双活性组分氧化物载于催化剂载体,研究甲苯催化燃烧性能.结果表明,当Cu、Mn物质的量比为1∶2、负载量为14％、焙烧温度为500℃、焙烧2h时CuMn/ZrO2整体催化剂催化活性高,起燃温度为210℃,完全燃烧温度为230℃,有效降低了甲苯催化燃烧的起燃温度和完全燃烧温度.     

Comprehensive Environmental Investigation at Former Industrial/Petroleum Underground Storage Tank Sites in Long Beach,CA: A Forensic Perspective

Two industrial sites were investigated based on years of available hydrogeologic information and monitoring data for soil and groundwater. Collected data were forensically evaluated using age-dating and fingerprinting methods. The previous business uses of the project sites were as a gas station, laundry/dry-cleaning service, and car wash with petroleum underground storage tanks (USTs). As a result, these sites were exposed to a number of toxic contaminants at relatively high concentrations. Source control was necessary for successful remediation and the ultimate removal of the remaining compounds from these industrial sites. Although contaminated soil around the source was excavated during the remedial action and the high concentrations of contaminants were reduced, typical groundwater contaminants such as petroleum hydrocarbons as gasoline (TPH-G), benzene, toluene, ethylbenzene, xylenes (BTEX), and oxygenates including methyl tert-butyl ether (MTBE), diisopropyl ether (DIPE), ethyl tert-butyl ether (ETBE), tert-amyl methyl ether (TAME), and tert-butyl alcohol (TBA) were persistently found at the studied sites around the source points. The plume and concentration of contaminants had changed their shapes and strength for all monitoring periods. Thus, additional source control seems to be a requirement for the complete removal of source contamination, which must be ascertained with groundwater and soil monitoring on a regular time base. For the study sites, monitored natural attenuation was relatively feasible for the long-term plan; however, it did not offer a perfect remediation solution for an ultimate goal because of residual toxic compounds that might have affected the surrounding residential areas at higher concentrations than their health limits. Therefore, as a remediation strategy, the combination of clean-up technology and natural attenuation with monitoring activities are more highly recommended than either clean-up or natural attenuation used separately.     

PbO_2复合电极预处理甲苯二胺废水

通过涂覆—热分解法与电沉积法制备了β-PbO_2/α-PbO_2/SnO_2-Sb2O3/Ti复合电极(PbO_2复合电极),采用X射线衍射(XRD)、扫描电子显微镜(SEM)、循环伏安法(CV)、线性极化法(LSV)和加速寿命试验对电极进行表征。将PbO_2复合电极用于处理甲苯二胺(TDA)废水,考察了电解质浓度、电流密度对TDA降解效果的影响。实验结果表明:α-PbO_2呈梭状,β-PbO_2呈花菜状,多层结构的PbO_2电极利于提高电极的稳定性和活性;PbO_2复合电极的析氧电位(1.9 V)明显高于TDA的氧化电位(1.28 V),其使用寿命长达486 d;在电流密度为60 m A/cm2、Na2SO4质量浓度为10 g/L、电解时间为240 min的条件下,对COD为4 791.74 mg/L、TDA质量浓度为486.4mg/L的废水进行处理,TDA去除率高达97.3%,COD去除率可达88.1%。     

甲苯对UASB反应器中溶解性微生物产物的影响

以乙酸钠为外加碳源,考察了UASB反应器内甲苯对可溶性微生物产物（SMP）的影响。实验结果表明：低质量浓度（20~70 mg/L）的甲苯对微生物有刺激作用,使得污泥增殖速率变小,SMP的质量浓度也逐渐减少,经过一段时间的驯化后,系统COD和TOC的去除率分别达到93%和94%以上,下降趋势较小；较高质量浓度（70~200 mg/L）的甲苯对微生物有抑制作用,污泥活性下降,反应器运行状况开始恶化,SMP的质量浓度也逐渐增大,经过一段时间的驯化后,系统COD和TOC的去除率分别维持在81%和83%以上；当甲苯质量浓度超过200 mg/L时,表现为污泥活性严重下降,对COD的去除效果极差。     

三苯类废气处理进展

综述了近年来三苯类废气处理所采用的方法,如吸收法、吸附法、催化氧化法、生物法、光催化法和低温等离子体法等,对各种方法的处理机理、处理效果以及优缺点进行了概括和分析,并指出联用技术将是未来的发展方向.     

光助芬顿反应催化降解气体中甲苯

以甲苯作为挥发性有机污染物(VOCs)的代表,利用连续进气动态实验装置,研究光助芬顿反应降解气体中甲苯的作用.考察了芬顿试剂溶液初始p H、H2O2浓度、Fe2+浓度以及甲苯初始浓度对降解甲苯的影响,并利用在线质谱和色谱对产物进行了定性、定量分析.结果表明,紫外光照加快了羟基自由基的生成,显著提高了气体中甲苯的去除率;p H=3.0、H2O2浓度为20 mmol·L-1、Fe2+浓度为0.3 mmol·L-1的条件下,甲苯去除率最高;当甲苯初始浓度为260 mg·m-3时,去除率能够达到98%;光助芬顿反应催化降解气体中甲苯实验未检测到CO2之外的中间产物,CO2产率分析表明去除的甲苯全部转化为CO2.     

双组分VOCs的催化氧化及动力学分析

考察了微波加热与管式炉加热下挥发性有机化合物(VOCs)甲苯与氯苯的催化氧化性能,并对双组分VOCs的反应动力学进行了分析.结果表明,VOCs的竞争吸附使得双组分中甲苯和氯苯的转化率比单组分降低3%~12%;微波的"热点效应"与"非热效应"使得VOCs转化效率明显优于管式炉加热,尤其是氯苯的转化率提高了31%~38%;微波加热降低了氧化反应温度和处理能耗.动力学分析表明,微波加热下甲苯和氯苯的反应活化能比管式炉加热下减少了2146 J·mol-1和1450J·mol-1,微波加热下氯苯的化学反应速率常数是管式炉加热的35倍,甲苯的反应速率常数提高了6倍.     

吸附增效低温等离子体法去除甲苯废气的研究

采用150Hz中频高压交流电源作为低温等离子体发生源,选用典型的微孔γ-Al2O3球形颗粒吸附剂(以下简称γ-Al2O3)作为等离子体反应器填充材料,协同低温等离子体法催化降解甲苯废气。考察了在不同条件下,γ-Al2O3的甲苯吸脱附效果和吸附增效低温等离子体法的甲苯去除效果。结果表明,甲苯降解反应主要发生在γ-Al2O3的表面,甲苯的去除率在一定的浓度范围内与γ-Al2O3表面吸附的甲苯量成正比关系;填充γ-Al2O3有利于提高甲苯去除率及等离子体反应器能量利用率;γ-Al2O3对臭氧的降解表现出一定的促进作用。