Fenton法和类Fenton法降解土壤中的二苯砷酸

本文对Fenton法与类Fenton法降解土壤中的二苯砷酸(diphenylarsinic acid,DPAA)进行了研究.考察了H2O2投加量和催化剂种类(Fe2+/Fe3+)对红壤及黑土中DPAA降解效果的影响,并采用高效液相色谱-质谱联用法(HPLC-MS/MS)对降解中间产物进行了初步鉴定.结果显示,针对红壤与黑土分别采用类Fenton法与Fenton法,在H2O2投加浓度为1 mol·L-1,含铁催化剂浓度为0.25 mol·L-1,土水比为1∶3,反应时间为1h的条件下,红壤及黑土中DPAA的降解率均可达到65%以上.HPLC-MS/MS的分析结果表明,DPAA可脱苯环形成降解产物苯砷酸(phenylarsinic acid,PAA),而PAA进一步氧化生成无机砷,这可能是Fenton/类Fenton法降解DPAA的途径之一.     

广州地区孕妇羊水中PCBs暴露水平初步研究

随机采集广州地区非职业PCBs(polychlorinated biphenyls,多氯联苯)暴露单胎孕妇分娩时羊水,分析羊水中PCBs浓度水平;结合孕妇临床资料(年龄、孕周、身体质量指数(body mass index,BMI))以及孕妇居住环境信息等,阐明了广州地区非职业暴露孕妇羊水PCBs蓄积的影响因素。结果表明,∑33PCBs浓度为15.91-324.38 ng·g-1,平均值为114.34±83.52 ng·g-1,中值为84.8 5ng·g-1;其中十氯含量最低,平均浓度为2.66±3.46 ng·g-1,中值为1.47 ng·g-1;六氯PCBs含量最高,平均浓度为28.79±33.84 ng·g-1,中值为17.48 ng·g-1。样本中有31种PCBs同分异构体在孕妇羊水中检出,分别为PCB 8、28、30、49、52、70、74、77、82、87、99、101、105、114、118、126、128、138、153、156、158、166、169、170、179、180、183、187、189、198和209;羊水主要的PCBs暴露以五氯PCBs、六氯PCBs和七氯PCBs为主,主要的同分异构体为PCB 138(4.73%)、179(4.15%)、153(3.92%)、183(3.89%)、166(3.77%)、187(3.74%)以及180(3.67%);暴露水平与美国、西班牙、加拿大等地区相比属于严重水平。统计结果显示,年龄、身体质量指数和孕周与PCBs蓄积有显著性正相关关系;工业区居住的孕妇相与非工业区居住孕妇相比,上述统计结果更为显著。     

有机化学品不同温度下(过冷)液体蒸气压预测模型的建立与评价

(过冷)液体蒸气压(PL)是评价化学品在环境中分配、迁移和归趋行为的重要参数。PL具有较强的温度依附性。发展一种能够精确预测不同环境温度下化学品PL的方法,有助于填补化学品生态风险评估的大量数据缺失。本研究收集整理了661种有机化合物在不同温度下(200~830 K)共计10 478个log PL值。在此基础上,采用偏最小二乘(PLS)回归和支持向量机(SVM)方法,构建了PL的线性和非线性预测模型。结果表明:2种模型均具有良好的拟合度、稳健性及预测能力,SVM模型的预测性能略高于PLS模型(PLS:R2adj.tra=0.912,RMSEtra=0.477,Q2ext=0.910;SVM:R2adj.tra=0.997,RMSEtra=0.092,Q2ext=0.967)。机理分析表明,温度是影响PL的主要因素,温度越高,蒸气压越大;其次,X1sol也影响PL大小,X1sol用来描述分子间的色散作用,分子间色散力越小,蒸气压越大;此外,化合物的氢键个数、极性和分子构型等因素也影响PL大小。采用Wiliams plot方法表征了PLS模型应用域。所建立的模型可用来预测烷烃、烯烃、醇、酮、羧酸、苯、酚、联苯、卤代芳香烃、含N化合物及含S化合物在不同温度下的PL数据。     

一株贫营养异养硝化-好氧反硝化菌的筛选及脱氮特性

为了探究并优化菌剂应用于微污染水源水体修复的机制和条件,主要针对水库沉积物内筛选出的贫营养好氧反硝化菌进行了菌种鉴定及脱氮特性研究,考察菌株在不同环境条件下的脱氮效果,明确了该菌株的最适宜生长条件,并基于水库水体中贫营养条件对菌株进行水源水库原水的驯化培养试验研究,以期实现该菌株对微污染水源水库原水中氮源污染物的脱除,为原位投菌技术实际工程应用提供理论依据。从微污染水源水库沉积物中驯化筛分出一株高效异养硝化-好氧反硝化菌A14,通过扫描电镜观察、生理生化特征、16S rRNA基因测序和Biolog GenⅢ鉴定,确定该菌株为革兰氏阴性短杆菌,鉴定为皮特不动杆菌（Acinetobacter pittii）。在好氧条件下,菌株细胞内表达反硝化功能基因napA,以NO3-为唯一氮源进行反硝化作用时,36 h时NO3-去除率为78.89%。以NH4+为唯一氮源时,48 h NH4+去除率为95.25%,TN去除率达80.42%,TOC去除率达98.30%,表明该菌株具有异养硝化-好氧反硝化特性。在改变环境条件过程中,该菌株在以乙酸钠为碳源,温度为30℃,C/N为12,pH为7,接种量为10%时,NO3-去除率最高为86.62%,并且在10℃下脱氮率达到40.18%。在水源水库原水脱氮实验中,接种处理TN去除率为50.95%,NO3-去除率为80.25%。结果表明,菌株A14在微污染水源水体菌剂脱氮修复中具有良好的应用潜力。     

Role of goethite dissolution in the oxidation of 2-chlorophenol with hydrogen peroxide.

It is well known that the dissolution of goethite plays an important role in catalyzing the oxidation of organic chemicals. Therefore, this study investigates how surface dissolution of goethite affects 2-chlorophenol oxidation in the goethite/H2O2 process. Experimental results indicate that ligand and reductant can enhance the dissolution rate of goethite, which is surface-controlled. Our results further indicate 2-chlorophenol degradation depends on goethite concentration. In addition, the oxidation rate of 2-CP is correlated with reductive dissolution rate at various dosages of goethite. Moreover, the oxidation mechanism of 2-CP is also a surface-controlled reaction. A mechanism proposed herein indicates that, in addition to the contaminant, its intermediate species affect the oxidation rate as well.     

Future carbon balance of China's forests under climate change and increasing CO2

The possible response of the carbon (C) balance of China's forests to an increase in atmospheric CO(2) concentration and climate change was investigated through a series of simulations using the Integrated Terrestrial Ecosystem Carbon (InTEC) model, which explicitly represents the effects of climate, CO(2) concentration, and nitrogen deposition on future C sequestration by forests. Two climate change scenarios (CGCM2-A2 and -B2) were used to drive the model. Simulations showed that China's forests were a C sink in the 1990 s, averaging 189 Tg C yr(-1) (about 13% of the global total). This sink peaks around 2020 and then gradually declines to 33.5 Tg C yr(-1) during 2091-2100 without climate and CO(2) changes. Effects of pure climate change of CGCM2-A2 and -B2 without allowing CO(2) effects on C assimilation in plants might reduce the average net primary productivity (NPP) of China's forests by 29% and 18% during 2091-2100, respectively. Total soil C stocks might decrease by 16% and 11% during this period. China's forests might broadly act as C sources during 2091-2100, with values of about 50 g Cm(-2)yr(-1) under the moderate warming of CGCM2-B2 and 50-200 g Cm(-2)yr(-1) under the warmer scenario of CGCM2-A2. An increase in CO(2) might broadly increase future C sequestration of China's forests. However, this CO(2) fertilization effect might decline with time. The CO(2) fertilization effects on NPP by the end of this century are 349.6 and 241.7 Tg C yr(-1) under CGCM2-A2 and -B2 increase scenarios, respectively. These effects increase by 199.1 and 126.6 Tg C yr(-1) in the first 50 years, and thereafter, by 150.5 and 115.1 Tg C yr(-1) in the second 50 years under CGCM2-A2 and -B2 increase scenarios, respectively. Under a CO(2) increase without climate change, the majority of China's forests would be C sinks during 2091-2100, ranging from 0 to 100 g Cm(-2)yr(-1). The positive effect of CO(2) fertilization on NPP and net ecosystem productivity would be exceeded by the negative effect of climate change after 2050. Under the CGCM2-A2 climate scenario and with direct CO(2) effects, China's forests may be a small C source of 7.6 Tg C yr(-1) during 2091-2100. Most forests act as C sources of 0-40 g Cm(-2)yr(-1). Under the CGCM2-B2 climate scenario and with direct CO(2) effects, China's forests might be a small C sink of 10.5 Tg C yr(-1) during 2091-2100, with C sequestration of most forests ranging from 0 to 40 g Cm(-2)yr(-1). Stand age structure plays a more dominant role in determining future C sequestration than CO(2) and climate change. The prediction of future C sequestration of China's forests is very sensitive to the Q(10) value used to estimate maintenance respiration and to soil water availability and less sensitive to N deposition scenario. The results are not yet comprehensive, as no forest disturbance data were available or predicted after 2001. However, the results indicate a range of possible responses of the C balance of China's forests to various scenarios of increase in CO(2) and climate change. These results could be useful for assessing measures to mitigate climate change through reforestation.     

Spatial scaling between leaf area index maps of different resolutions

We developed algorithms for spatial scaling of leaf area index (LAI) using sub-pixel information. The study area is located near Liping County, Guizhou Province, in China. Methods for LAI spatial scaling were investigated on LAI images with 960 m resolution derived in two ways. LAI from distributed calculation (LAID) was derived using Landsat ETM+ data (30 m), and LAI from lumped calculation (LAIL) was obtained from the coarse (960 m) resolution data derived through resampling the ETM+ data. We found that lumped calculations can be considerably biased compared to the distributed (ETM+) case, suggesting that global and regional LAI maps can be biased if surface heterogeneity within the mapping resolution is ignored. Based on these results, we developed algorithms for removing the biases in lumped LAI maps using sub-pixel land cover-type information, and applied these to correct one coarse resolution LAI product which greatly improved its accuracy.     

性能退化对民机巡航阶段污染物排放的影响研究

发动机性能退化将会影响污染物排放,以往污染物排放估算模型未充分考虑性能退化对排放量的影响.因此本文对原有污染物估算模型进行修正,将民机实际运行中表征发动机健康状态的主要参数EGT作为特征量融入到污染物排放估算模型中,提出改进的形成氧化法以及P3-T3方法,定量估算性能退化对污染物排放的影响.使用GE90-115B发动机历史QAR数据,计算航空发动机处于不同健康水平下的巡航阶段污染物排放特性.研究结果表明：航空发动机性能退化将会显著影响巡航阶段污染物排放特性.其中,性能退化严重时航空发动机CO、UHC以及黑碳的巡航阶段平均排放指数较健康状态时分别升高87.52%、247.76%以及19.68%,而NO_x的平均排放指数则下降55.33%.因此在对性能退化的发动机进行污染物评估时必须考虑性能退化的影响.     

福建省生产废水和生活污水污染物排放的驱动力及其时空分异

采用对数平均迪氏指数方法,区分生产和生活两个体系,构建时空分解分析模型,追踪了福建省9个设区市2011—2019年水污染物排放变化的关键驱动力及其贡献的时空差异.结果显示：研究期内福建省工业废水污染物排放持续减少,并且各驱动力贡献的区域差距明显变小,趋于平衡;生活污水污染物排放量仍保持高位,各驱动力贡献的区域差距基本保持不变.其中,经济规模扩张是福建省水污染物排放的主导驱动力,主要源于福州、厦门、泉州经济赶超发展影响;城镇化发展对区域生活污水污染物排放的驱动影响表现为增排效应,以福州和厦门尤为显著;工业化发展对区域工业废水污染物排放的影响效应由正驱动逐渐转变为负驱动,这主要归功于三明和泉州产业结构调整优化的拉动 效应;技术效应一直是福建省水污染物排放控制的重要驱动力,但部分地区已逐渐步入生活污染物技术减排攻坚期.     

长三角重点生态功能县域生态资产损益核算

限制开发的重点生态功能县域承担着生态保护与经济发展双重使命,如何实现生态与发展互促共进及生态产品价值化是当前面临的极大难点,生态资产损益核算为量化区域资源有偿使用、生态保护修复、生态文明绩效评价等提供了有效途径。以浙江省嵊州市作为长三角地区重点生态功能区的典型县域,基于栅格尺度评估了近20年生态资产存量与流量时空动态变化,并利用地理探测器结合人类活动类型监测分析了生态资产损益的驱动因素。结果表明：2000—2018年,由于森林生态资产质量降低及面积减少,嵊州市近60%区域的生态资产存量呈减少趋势,而生态资产流量总价值与单位面积价值均增益10%以上。相对于自然因素,社会经济因素对嵊州市生态资产损益平均贡献度更大,为17%。县域城镇化导致粮食供给轻微减损,70%以上乡镇生态资产增益,特别是石璜镇生态保护成效较突出。