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791.
氯自由基(·Cl)的高氧化性及其内陆来源的新发现使得·Cl在评估有机污染物的大气归趋方面起着比以往更为重要的作用。含有NH_x(x=1,2)结构的有机化合物不仅是大气中一类潜在的有机污染物,也是大气中致癌性亚硝胺的前驱体—N中心自由基的重要来源。前人研究发现,·Cl与含有NH_x(x=1,2)结构的有机化合物具有独特的相互作用且其反应具有结构依赖性。目前,大多数研究只关注链状含有NH_x(x=1,2)结构有机化合物的反应,而对于环状含有NH结构有机化合物的反应研究却很少。本研究使用量子化学和动力学模拟相结合的方法研究·Cl引发3种环状含有NH结构有机化合物(吗啉(MOR)、哌啶(PIP)和吡咯烷(PYR))的大气转化机制及动力学。结果发现,·Cl夺取3种环状含有NH结构有机化合物中N—H的H原子形成N中心自由基是最可行的反应路径。在298 K和1 atm下,计算的反应速率常数分别为5.0!10-10(MOR)、5.1!10-10(PIP)和4.9!10-10(PYR) cm~3·molecule-1·s-1,且具有正的温度依附性。结合可获得的·OH引发反应的反应速率常数,评估·Cl对MOR和PIP转化的贡献分别为·OH的2.6%~26%和6.9%~69%。上述研究结果为将来建立·Cl引发含有NH_x(x=1,2)结构有机化合物反应的结构-活性关系、全面评估含有NH_x(x=1,2)结构有机化合物的大气归趋和环境风险提供数据支持。 相似文献
792.
793.
运用实时无标记细胞分析系统(RTCA)和Cell Counting Kit-8(CCK-8)法分别检测柴油废气颗粒物(DEP)致支气管上皮细胞(HBE)细胞毒性,从而对2种方法进行比较研究.分别以浓度为0、3.5、7、14、28和56 mg·L-1 2种柴油废气标准参考颗粒物(Standard Reference Material 1650b,SRM 1650b;Standard Reference Material 2975,SRM 2975)对 HBE 细胞进行暴露处理,分别暴露6、12、24和48 h后,检测不同DEP致HBE细胞毒性,比较各组之间细胞存活率或标准化细胞指数(normalized cell index,NCI)值的差异,考察2种方法的优缺点.并用细胞凋亡实验检测各差异组之间的凋亡率.在相同染毒浓度及暴露时间,与SRM 1650b相比,SRM 2975对HBE细胞的毒性更强.在RTCA检测DEP致HBE细胞毒性时,低浓度DEP组的NCI值已经表现出与对照组有统计学差异(P<0.05),而相同时间条件下,CCK-8法在更高浓度的DEP组才检测出显著的细胞活性下降(P<0.05).且由细胞凋亡实验证实,与对照组相比,低浓度DEP组的细胞凋亡率已经有统计学差异.相对于CCK-8法,RTCA更适用于检测DEP致贴壁HBE细胞毒性.CCK-8法更适用于检测DEP致悬浮细胞的细胞毒性或与气液暴露装置联用时的贴壁/悬浮细胞毒性. 相似文献
794.
Xinyu Wang Ye Jin Weirui Chen Ruini Zou Jinxin Xie Yiming Tang Xukai Li Laisheng Li 《Frontiers of Environmental Science & Engineering》2021,15(6):122
795.
氯自由基(·Cl)内陆来源的新发现增强了其对转化大气有机污染物的贡献,因此,需要更深入地研究·Cl引发有机污染物的转化机制和动力学.萘(Nap)是一种重要的化学品,也是城市大气浓度最高的多环芳烃,前人针对羟基自由基(·OH)引发Nap的大气氧化开展了研究.然而,目前对于·Cl引发Nap的大气氧化机制还不清楚.本研究通过量子化学计算(ωB97XD/6-311++G(3 df,2pd)//ωB97XD/6-31 +G(d,p))和动力学模拟相结合的方法研究了·Cl引发Nap的大气氧化机制与动力学,发现·Cl主要加成到Nap分子的C5位置,形成加成中间体·C10H8Cl(R1).随后,O2加成到R1的C2和C6位置生成过氧自由基(RO2·)R1-2OO-s/a和R1-6OO-s/a(s/a=syn/anti,syn表示O2加成方向和·C1加成方向相同,anti表示O2加成方向和·C1加成方向相反).这4种RO2·的环化、氢迁移和氯迁移反应均很难(能垒>20 kcal· mol-1)发生.因此,在低NO浓度条件下,RO2·主要和HO2·反应生成氢过氧化合物(QOOH)和烷氧自由基(RO ·)R1-2O-s/a和R1-6O-s/a;在高NO浓度条件下,RO2·将主要与NO反应生成RO· (R1-2O-s/a和R1-6O-s/a)和有机硝酸酯(C10 H8 ClNO3).生成的RO·进一步通过单分子环化反应生成双环产物R1-21O-s/a和R1-61O-s/a.重要的是,生成的有机氢过氧化合物和有机硝酸酯的水生毒性比其母体化合物Nap更强,表明·Cl引发Nap反应增加了Nap释放的环境风险.揭示的机制对理解大气Nap化学及Nap释放导致的环境风险具有重要意义. 相似文献
796.
Xie M.Wu Z.Wang X.Gu J.Chen L.Wang Y. 《应用与环境生物学报》2018,(4):915-920
In an effort to remove BDE-47 residues from the environment, a bacterial strain that is capable of utilizing BDE-47 as the sole carbon source was isolated and screened from soil collected from an e-waste recycling area in Tianjin to analyze the degradation properties. The strain was preliminarily identified as Enterobacter sp. according to a 16S rDNA gene sequence analysis. The strain degraded 35.8% of 525 μg/L of BDE-47 in 35 d when the initial concentration of bacteria was 7.1 × 105 cells/ mL. The product of the biodegradation of BDE-47 was BDE-28. The biodegradation of BDE-47 fit well with first-order kinetics, and its degradation kinetics was ln Ct = - 0.104t + 6.22. With the addition of an electron acceptor, such as Fe3+, SO4 2- and NO3 -, the BDE-47 degradation rate was significantly increased to 49.8%, 59.1%, and 67.3%, respectively. The above results revealed that the strain could degrade BDE-47, which is of importance in the application of environmental bioremediation of BDE-47. © 2018 Science Press. All rights reserved. 相似文献
797.
Fine root decomposition is an important way in which nutrients are returned to plantation soil; thus, further study of this process will be helpful for understanding material cycling in forest ecosystems. We investigated a Toona sinensis plantation in the central Sichuan hilly region using litter bags containing T. sinensis fine roots to evaluate the dynamics of fine root decomposition and nutrient release for one year in forest gaps of 50 m2 (L1), 100 m2 (L2), and 150 m2 (L3). The results showed that T. sinensis fine root decomposition was fastest in the first 90 days. As time passed, the decomposition rate slowed. One year later, the residue rate was 75.44%, 73.92%, and 72.07%, respectively. The fine root decomposition rate of L3 was greater than that of L2, which was greater than that of L1. During fine root decomposition, the dynamics of the fine root nutrient concentrations changed. C, P, and K concentrations of the fine roots declined in forest gaps, while N, Ca, and Mg concentrations increased overall in the fine roots. In conclusion, forest gaps had effects on the fine root decomposition and nutrient release of T. sinensis, and different sized forest gaps produced different results. © 2018 Science Press. All rights reserved. 相似文献
798.
Liwen Zhang Deming Dong Yaojing Xie Zhiyong Guo Xiuyi Hua 《Environmental Chemistry Letters》2018,16(3):1043-1048
The real behavior of water organic contaminants such as pesticides and pharmaceuticals is not well known because research experiments usually simplify the conditions by studying the sorption of a pure compound on a single solid. However, in natural waters, biofilms, suspended particles, and sediments are solid substances that coexist, and thus may change the contaminant fate. Therefore, we studied here the sorption of lindane and ciprofloxacin by three single-solid and three double-solid sorbents using batch experiments. We also compared the effect of dissolved organic matter (DOM) between single- and double-solid sorption systems. Results show that the sorption quantity of lindane to the double-solid system of suspended particles and sediments is lower, of 0.99 L/g, than the sum of sorption quantity in the single-solid system, of 1.39 L/g. The sorption quantity of ciprofloxacin is higher, of 2.70 L/g, than the sum of sorption quantity in the single-solid system, of 1.90 L/g. These findings are explained by changes in DOM that suppress or promote sorption. To our best knowledge, this is the first study to present evidence that coexisting river solids modify lindane and ciprofloxacin sorption. 相似文献
799.
合理确定重金属土壤筛选值是污染场地风险识别和调查评估的基础,过松或过严的标准都会增加风险评估的不确定性,甚至可能会导致风险管控措施失效或修复资金浪费,确定重金属土壤筛选值的关键影响因子是合理确定重金属土壤筛选值的前提。选择工业污染场地中检出频率高、毒性大的砷作为研究对象,通过假设工商业用地下的暴露情景,根据《污染场地风险评估技术导则》(HJ25.3—2014)得到砷筛选值计算公式,利用基于蒙特卡罗模拟的Crystal Ball模型计算公式中各参数对结果的敏感性和贡献率来确定关键影响因子,通过调研国内外砷筛选值现状,从计算模型、毒性评估及关键影响因子等方面对引起各国砷筛选值差异的原因进行了分析探讨。结果表明:工商业用地下土壤砷筛选值取值为0.84~175.7 mg·kg~(-1),均值为21.4 mg·kg~(-1),95%的置信上限为24.19 mg·kg~(-1);风险可接受水平、每日土壤摄入量(IR)、暴露频率(EF)和暴露周期(ED)对砷筛选值的贡献率依次为41.3%、-27.3%、-16.3%和-12.7%,其余因子的贡献率均小于1%;关键影响因子按贡献率绝对值从大到小分别为风险可接受水平、每日土壤摄入量(IR)、暴露频率(EF)、暴露周期(ED)。计算模型和毒性评估存在差异是国内外土壤砷筛选值差异的基础原因,当计算模型和毒性评估差异不大时,关键影响因子才是决定性因素,其影响程度与模拟计算的结果一致。建议我国完善筛选值计算模型,对砷的毒性效应和符合我国暴露人群特征的关键影响因子展开深入研究。 相似文献
800.
Jie Mao Xie Quan Jing Wang Cong Gao Shuo Chen Hongtao Yu Yaobin Zhang 《Frontiers of Environmental Science & Engineering》2018,12(6):10
Heterogeneous Fenton-like reaction has been extensively investigated to eliminate refractory organic contaminants in wastewater, but it usually shows low catalytic performance due to difficulty in reduction from Fe(III) to Fe(II). In this study, enhanced catalytic efficiency was obtained by employing Cu-doped BiFeO3 as heterogeneous Fenton-like catalysts, which exhibited higher catalytic performance toward the activation of H2O2 for phenol degradation than un-doped BiFeO3. BiFe0.8Cu0.2O3 displayed the best performance, which yielded 91% removal of phenol (10 mg L–1) in 120 min. The pseudo first-order kinetic rate constant of phenol degradation in BiFe0.8Cu0.2O3 catalyzed heterogeneous Fenton-like reaction was 5 times higher than those of traditional heterogeneous Fenton-like catalysts, such as Fe3O4 and goethite. The phenol degradation efficiency could still reach 83% after 4 cycles, which implied the good stability of BiFe0.8Cu0.2O3. The high catalytic activity of BiFe0.8Cu0.2O3 was attributed to the fact that the doping Cu into BiFeO3 could promote the generation of Fe(II) in the catalyst and then facilitate the activation of H2O2 to degrade the organic pollutants.
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