Pd/CeO2-Al2O3对烟气中多环芳烃的催化氧化性能研究

采用浸渍法制备了不同负载量及不同钯铈比(Pd:Ce)的Pd/CeO2-Al2O3催化剂,并结合XRD、BET、SEM、O2-TPD和H2-TPR等方法对催化剂的性质进行了表征,研究了所制备的催化剂对燃煤烟气中多环芳烃(PAHs)的催化转化效率.XRD和SEM结果表明,Ce和Pd在Al2O3表面呈高度分散状态,有利于PAHs的催化氧化.BET测试表明,Ce的引入改变了催化剂表面孔径结构,提高其比表面积.O2-TPD和H2-TPR测试表明,适当钯铈比条件下制备的催化剂有较强的储氧能力和活性.催化氧化实验结果表明,所制备的Pd/CeO2-Al2O3催化剂对PAHs具有较高的转化效率,其平均转化率均在80%以上,且PAHs的毒性当量显著降低,钯铈比对PAHs的催化氧化性能影响较大,当催化剂的钯铈比为1:1时,PAHs的转化率最高,可达90%以上.     

挥发性氯代烃在干燥土壤中的平衡吸附研究

吸附是挥发性氯代烃（volatile chlorinated hydrocarbons,VCHs）污染土壤的主要机制之一.采集长三角地区3类典型水稻土,用静态平衡吸附实验进行干燥土壤对6种VCHs的平衡吸附研究.结果表明,干燥土壤的平衡吸附等温线难以用Langmuir方程和BET方程描述,但用Dubinin-Astak...     

生物表面活性剂-微生物强化紫花苜蓿修复多环芳烃污染土壤

在温室盆栽条件下,通过单独或联合添加生物表面活性剂鼠李糖脂(RH)和接种多环芳烃专性降解菌(DB),研究了利用生物表面活性剂-微生物强化紫花苜蓿(Medicago sativa L.)修复多环芳烃(PAHs)长期污染土壤的效果.结果表明,添加鼠李糖脂和接种PAHs专性降解菌能促进紫花苜蓿的生长和土壤中PAHs的降解.培养90d后,RH、DB处理的PAHs的降解率分别为30.0%和49.6%,均高于对照处理(CK)(21.7%).RH+DB处理PAHs的降解率最高达53.9%,说明鼠李糖脂和PAHs专性降解菌协同作用显著.另外,随着PAHs苯环数的增加,其平均降解率逐渐降低,但是接种PAHs专性降解菌能够提高4环和5环PAHs的降解率.同时也发现土壤中脱氢酶活性和PAHs降解菌数量越高的处理,土壤PAHs的降解率也越高.所以添加鼠李糖脂和接种PAHs专性降解菌能够有效促进土壤多环芳烃降解.     

原位生物修复提高多环芳烃污染土壤农用安全性

为了减少多环芳烃(polycyclic aromatic hydrocarbons,PAHs)在作物体内的富集,降低食源性PAHs对人类的潜在风险,提高PAHs污染土壤的农用安全性,在受到PAHs污染的麦田中施用类球红细菌(Rhodobacter sphaeroide)菌剂(RS)进行原位修复.以叶面喷施(B)和根部喷施(D)50倍稀释的RS两种方式处理,以喷施等量清水的处理为对照(A),不做任何处理的麦田为空白(CK),从小麦苗期开始处理,到小麦成熟期测定了土壤和小麦籽粒中PAHs含量以及根际土壤微生物群落结构的变化,探讨了施用RS对PAHs污染土壤的强化修复作用.结果表明,施加RS的B区、D区与空白(CK)区相比,标识土壤微生物的磷脂脂肪酸(PLFAs)种类均有29.6%变异率;土壤PAHs的去除率分别提高了1.59倍和1.68倍;富集因子分别降低了58.9%和62.2%;50穗小麦籽粒的干重分别提高了8.95%和12.5%.RS的施用改变了土壤微生物群落结构,活化了土壤微生物的代谢活性,从而加快了土壤PAHs的降解;同时,RS的施用也降低了PAHs在小麦籽粒的富集量,提高了小麦的产量,显示出RS在提高PAHs污染土壤的农用安全性方面具有应用潜力.     

广州市小学生多环芳烃内暴露水平

为了解广州市小学生多环芳烃内暴露水平,于2014年9月15~20日在广州市居民区与工业区分别采集了78名、86名小学生的晨尿样品,并利用快速液相色谱-三重四级杆串联质谱仪同时检测了样品中10种羟基多环芳烃(OH-PAHs)含量.结果表明,居民区和工业区小学生尿液中ΣOH-PAHs分别为0.83~80.63μmol·mol~(-1)和1.06~72.47μmol·mol~(-1),几何平均值为6.18μmol·mol~(-1)和6.47μmol·mol~(-1),居民区略低于工业区(无统计学意义,P0.05).比较两个区域OH-PAHs不同组分的暴露水平,居民区小学生尿液中1-OHP的暴露水平明显高于工业区(具有统计学意义,P0.05),其他组分无显著差异,与国内外已有研究相比,本研究小学生尿液中OH-PAHs含量较高值得关注.其次,居民区小学生体内OH-PAHs单体之间均显著相关(P0.01),相关系数在0.511~0.928之间;工业区小学生尿液1-OHP与2-OHN、1-OHP与1-OHN之间无显著相关性,其他OH-PAHs单体之间均显著相关(P0.01),相关系数在0.338~0.855之间.这一差异可能指示不同功能区小学生多环芳烃暴露源的差异性,居民区相对单一,而工业区因工业企业、物流交通的排放呈现多源性.     

太原市采暖期大气PM_(2.5)中多环芳烃的污染特征

本研究对太原市采暖期PM2.5中多环芳烃(PAHs)的污染水平、组成特征、健康风险以及来源进行了分析。结果表明,太原市采暖期PM2.5的日均浓度水平为70.7~274.2μg/m3,90%的样品超过了我国《环境空气质量标准》(GB 3095-2012)中PM2.5的二级标准限值(75μg/m3)。PM2.5中16种PAHs的浓度水平为282.7~1 398.6ng/m3,平均值为915.7ng/m3。荧蒽(Fla)是浓度最高的单体,占PAHs总浓度的20.4%,其次是芘(Pry)和菲(Phe),分别占14.5%和13.2%。不同环数的PAHs质量浓度为4环5~6环2~3环。以苯并(a)芘(Bap)为参照对象的昼夜毒性当量浓度Bapeq分别为75.5和100.0ng/m3,高于我国和WHO对Bap的规定值(分别为2.5和1ng/m3),对人体健康存在潜在危害。根据PAHs环数分布及特征比值法判断PAHs的主要来源是煤燃烧,同时也存在一定的生物质燃烧和少部分石油燃烧。     

Anaerobic biodegradation of PAHs in mangrove sediment with amendment of NaHCO3

Mangrove sediment is unique in chemical and biological properties. Many of them suffer polycyclic aromatic hydrocarbon(PAH) contamination. However, the study on PAH biological remediation for mangrove sediment is deficient. Enriched PAH-degrading microbial consortium and electron acceptor amendment are considered as two effective measures. Compared to other electron acceptors, the study on CO2, which is used by methanogens, is still seldom. This study investigated the effect of Na HCO3 amendment on the anaerobic biodegradation of four mixed PAHs, namely fluorene(Fl), phenanthrene(Phe),fluoranthene(Flua) and pyrene(Pyr), with or without enriched PAH-degrading microbial consortium in mangrove sediment slurry. The trends of various parameters, including PAH concentrations, microbial population size, electron-transport system activities, electron acceptor and anaerobic gas production were monitored. The results revealed that the inoculation of enriched PAH-degrading consortium had a significant effect with half lives shortened by 7–13 days for 3-ring PAHs and 11–24 days for 4-ring PAHs. While Na HCO3 amendment did not have a significant effect on the biodegradation of PAHs and other parameters, except that CO2 gas in the headspace of experimental flasks was increased.One of the possible reasons is that mangrove sediment contains high concentrations of other electron acceptors which are easier to be utilized by anaerobic bacteria, the other one is that the anaerobes in mangrove sediment can produce enough CO2 gas even without adding Na HCO3.     

Characterizations of organic compounds in diesel exhaust particulates

To characterize how the speed and load of a medium-duty diesel engine affected the organic compounds in diesel particle matter (PM) below 1 μm, four driving conditions were examined. At all four driving conditions, concentration of identifiable organic compounds in PM ultrafine (34–94 nm) and accumulation (94–1000 nm) modes ranged from 2.9 to 5.7 μg/m³ and 9.5 to 16.4 μg/m³, respectively. As a function of driving conditions, the non-oxygen-containing organics exhibited a reversed concentration trend to the oxygen-containing organics. The identified organic compounds were classified into eleven classes: alkanes, alkenes, alkynes, aromatic hydrocarbons, carboxylic acids, esters, ketones, alcohols, ethers, nitrogen-containing compounds, and sulfur-containing compounds. At all driving conditions, alkane class consistently showed the highest concentration (8.3 to 18.0 μg/m³) followed by carboxylic acid, esters, ketones and alcohols. Twelve polycyclic aromatic hydrocarbons (PAHs) were identified with a total concentration ranging from 37.9 to 174.8 ng/m³. In addition, nine nitrogen-containing polycyclic aromatic compounds (NPACs) were identified with a total concentration ranging from 7.0 to 10.3 ng/m³. The most abundant PAH (phenanthrene) and NPACs (7,8-benzoquinoline and 3-nitrophenanthrene) comprise a similar molecular (3 aromatic-ring) structure under the highest engine speed and engine load.     

百色市大气可吸入颗粒物PM2.5中多环芳烃污染特征及健康风险评价

为调查百色市大气颗粒物PM2.5中16种多环芳烃(PAHs)的污染特征,于2013年冬、夏两季采集了百色市城、郊2个不同采样点的大气样品,采用HPLC分析了16种US EPA优控PAHs的质量浓度、组分特征,运用同分异构体比率法揭示其污染来源.结果表明:百色市大气PM25中∑PAHs质量浓度为4.7～ 142.3 ng/m3,低于我国制定的PM2.5中PAHs的年均值(35 μg/m3);百色市城区、郊区2个采样点大气PM2.5中PAHs的质量浓度分别为6.9～ 142.3 ng/m3和4.7～ 109.6ng/m3,平均值为37.2 ng/m3和24.7 ng/m3,不同环数PAHs质量浓度从大到小为4环、5环、3环、6环、2环,4环、5环PAHs分别占∑PAHs的42.9％～ 50.7％和18.4％～22.4％;主要的单种PAHs为茚并[1,2,3-cd]芘、苯并[g,h,i]苝、(苊)、苯并[b]荧蒽和苯并[k]荧蒽.冬季∑PAHs质量浓度高于夏季.PM2.5中苯并[a]芘等效毒性(BEQ)为2.3～7.4,与其他城市相比,BEQ属于中下等水平.PM2.5中的PAHs源自煤及机动车辆燃油的燃烧.     

我国部分城市大气颗粒物中多环芳烃的分布特征

主要研究中国大气颗粒物中多环芳烃污染状况,对多环芳烃的浓度水平、时间和空间分布、组成及在不同粒径颗粒物上的分布特征进行了综述.北方城市大气颗粒物中多环芳烃的浓度普遍高于南方城市.大气颗粒物中多环芳烃以4～6环为主,占多环芳烃总量的60％～ 80％.大多数多环芳烃分布于细粒子中,且多环芳烃在PM2.5中的分布占在PM1o中分布的70％以上.多环芳烃质量浓度有明显的季节变化特征,多数研究中多环芳烃浓度从高到低的季节变化规律为冬季、秋季、春季、夏季.不同功能区大气颗粒物中多环芳烃污染,城区高于郊区,交通区和工业区高于商业区、居住区和文化区.