Progress in quantitative research on the relationship between atmospheric oxidation and air quality

Atmospheric oxidizing capacity (AOC) is an essential driving force of troposphere chemistry and self-cleaning, but the definition of AOC and its quantitative representation remain uncertain. Driven by national demand for air pollution control in recent years, Chinese scholars have carried out studies on theories of atmospheric chemistry and have made considerable progress in AOC research. This paper will give a brief review of these developments. First, AOC indexes were established that represent apparent atmospheric oxidizing ability (AOIe) and potential atmospheric oxidizing ability (AOIp) based on aspects of macrothermodynamics and microdynamics, respectively. A closed study refined the quantitative contributions of heterogeneous chemistry to AOC in Beijing, and these AOC methods were further applied in Beijing-Tianjin-Hebei and key areas across the country. In addition, the detection of ground or vertical profiles for atmospheric OH·, HO₂·, NO₃· radicals and reservoir molecules can now be obtained with domestic instruments in diverse environments. Moreover, laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O₃ and NO₂, which are typical oxidants in the surface/interface atmosphere, and the evolutionary and budgetary implications of atmospheric oxidants reacting under multispecies, multiphase and multi-interface conditions were obtained. Finally, based on the GRAPES-CUACE adjoint model improved by Chinese scholars, simulations of key substances affecting atmospheric oxidation and secondary organic and inorganic aerosol formation have been optimized. Normalized numerical simulations of AOIe and AOIp were performed, and regional coordination of AOC was adjusted. An optimized plan for controlling O₃ and PM_2.5 was analyzed by scenario simulation.     

VOC emission caps constrained by air quality targets based on response surface model: A case study in the Pearl River Delta Region, China

Because of the recent growth in ground-level ozone and increased emission of volatile organic compounds (VOCs), VOC emission control has become a major concern in China. In response, emission caps to control VOC have been stipulated in recent policies, but few of them were constrained by the co-control target of PM_2.5 and ozone, and discussed the factor that influence the emission cap formulation. Herein, we proposed a framework for quantification of VOC emission caps constrained by targets for PM_2.5 and ozone via a new response surface modeling (RSM) technique, achieving 50% computational cost savings of the quantification. In the Pearl River Delta (PRD) region, the VOC emission caps constrained by air quality targets varied greatly with the NO_x emission reduction level. If control measures in the surrounding areas of the PRD region were not considered, there could be two feasible strategies for VOC emission caps to meet air quality targets (160 µg/m³ for the maximum 8-hr-average 90th-percentile (MDA8-90%) ozone and 25 µg/m³ for the annual average of PM_2.5): a moderate VOC emission cap with <20% NOx emission reductions or a notable VOC emission cap with >60% NO_x emission reductions. If the ozone concentration target were reduced to 155 µg/m³, deep NO_x emission reductions is the only feasible ozone control measure in PRD. Optimization of seasonal VOC emission caps based on the Monte Carlo simulation could allow us to gain higher ozone benefits or greater VOC emission reductions. If VOC emissions were further reduced in autumn, MDA8-90% ozone could be lowered by 0.3-1.5 µg/m³, equaling the ozone benefits of 10% VOC emission reduction measures. The method for VOC emission cap quantification and optimization proposed in this study could provide scientific guidance for coordinated control of regional PM_2.5 and O₃ pollution in China.     

改性ACF－PAN吸附SO_2前后表面结构变化及机机理究

以自制ＰＡＮ－基聚丙烯腈活性碳纤维ＡＣＦ－ＰＡＮ（ＡＣＦ－活性碳纤维、ＰＡＮ－聚丙烯腈）和改性处理的ＡＣＦ－ＰＡＮ吸附ＳＯ_２，借助ＩＲ、ｘ－光电子能谱分析等研究ＡＣＦ－ＰＡＮ改性处理及吸附ＳＯ_２前后表面结构变化。结果表明：各型ＡＣＦ－ＰＡＮ吸附ＳＯ_２的活性中心为表面结构中的含氮官能团以及引入的金属氧化物，其吸附机理是活性氮催化或电子传递。     

生存环境与物种生命的演化

达尔文进化论的缺环就是连续性。相同自然条件下，动物进化的机遇和概率是相等的。进化就是物种在新环境中所做的一系列适应改变。当一个物种减少至某一极限数量时必将走向灭绝。     

中温两相UBF反应器处理养鸡场离心废水的试验分析

在中温 35℃采用两相 UBF反应器处理养鸡场离心废水 ,结果表明 :进水 CODcr为 190 0 0 mg/ L,系统容积负荷 2 1.5 4kg CODcr/ m3· d,水力停留时间 2 1.17hr,CODcr去除率为 81.98% ,BOD5 去除率为 90 .45 % ,产气率为 0 .44 6 m3/kg CODcr     

用EXAFS研究Zn在水锰矿上的吸附-解吸机理

用延展X光吸收精细结构光谱(EXAFS)研究了重金属Zn(Ⅱ)在水锰矿(γ-MnOOH)上吸附产物的微观结构及其吸附机理.结果表明,Zn(Ⅱ)-水锰矿体系中(pH 7.5,0.1mol/LNaNO₃介质,25℃),Zn²⁺主要是通过共用水合Zn²⁺的O原子及水锰矿表面上的O原子形成Zn-O键,从而结合到水锰矿固体表面上的.平均Zn-O原子间距为1.998±0.010 A(n=3).这个Zn-O键键长是六配位的Zn(H₂O)²⁺₆及其水解产物四配位的Zn(OH)₂或Zn(OH)₄^2-各以一定比例混合吸附于水锰矿表面而形成的.同时,对第二配位层(Zn-Mn相互作用)的EXAFS图谱分析证明存在2个典型的Zn-Mn原子间距,即R₁=3.08±0.024A(n=3)和R2=3.54±0.018 A(n=3).这2个Zn-Mn原子距分别对应于水锰矿结构单元MnO6八面体与Zn水合离子ZnO多面体结合的2种方式,即共用2个O原子的边-边结合与共用1个O原子的角-角结合.边-边结合是较强的吸附位,Zn-Mn原子距较短(R₁=3.08A),吸附较不可逆.角-角结合是较弱的吸附位,Zn-Mn原子距较长(R₂=3.54A),吸附较为可逆.这一结果从微观上证明了亚稳平衡态吸附理论(MEA理论)的基本假设,即具有相同吸附密度的同一吸附质由于吸附力强弱以及微观构型的不同可具有不同的化学位,因而证明了修正传统吸附热力学的基本假设(吸附密度为热力学状态函数)的必要性.宏观的吸附-解吸热力学实验表明Zn(Ⅱ)在水锰矿上的吸附是不可逆的,EXAFS结果指出这种不可逆性主要是由Zn水合离子中ZnO多面体与水锰矿结构单元MnO₆八面体之间的边-边结合所导致的.     

崇明东滩沉积物再悬浮对沉积物-水界面氮、磷交换行为的影响

2002年7月采集崇明东滩低潮滩沉积物样和水样,运用模拟实验研究沉积物再悬浮作用对沉积物-水界面三态氮和可溶磷交换行为的影响实验发现,在沉积物不断发生再悬浮的过程中,水体中三态氮的含量明显增加,其中NO₃^--N变化最为显著,升高浓度值达11.869μmol·L^-1,NH₄⁺-N增长2.1713μmol·L^-1,NO₂^--N的释放约为0.2μmol·L^-1,可溶磷的含量也有少量的增加.同时,再悬浮作用对沉积物-水界面三态氮和可溶磷的环境地球化学行为也有一定的影响,与静置状态相比,NH₄⁺-N和NO₃^--N表现出与静置状态截然相反的变化规律,NO₂^--N受多种因素的影响,变化比较复杂,初期与静置状态相反而后表现一致.再悬浮颗粒物浓度也是制约沉积物-水界面三态氮和可溶磷变化的主要因子之一.实验结果显示,NH₄⁺-N在前7h以内的变化和悬浮颗粒物浓度表现出较好的相关关系,后5h呈负相关关系;NO₂^--N和可溶磷在整个过程中与悬浮颗粒物浓度的变化都有着很好的相关性,只有NO₃^--N的变化与其关系比较薄弱.     

6种挥发性有机物在甲苯驯化微生物中的好氧生物降解性能

利用振荡摇瓶法测定了6种典型挥发性有机物,甲苯、邻二甲苯、间二甲苯、对二甲苯、苯和氯苯在甲苯驯化微生物中的好氧生物降解性能.结果表明,在本研究的液相浓度范围内(甲苯＜174mg/L,邻二甲苯＜149mg/L,间二甲苯＜129mg/L,对二甲苯＜133mg/L,苯＜234mg/L,氯苯＜146mg/L),3种二甲苯、苯和氯苯的降解速率随其初始浓度的增大而增加,符合一级反应,这5种VOCs未对微生物产生明显的抑制或毒害作用;甲苯的液相浓度大于85mg/L时,其降解速率不随初始浓度的增大而改变,其降解规律符合Monod方程.     

地下水除草剂阿特拉津污染微生物治理的实验研究

采用了从农药厂阿特拉津生产车间排污口污泥中分离出的菌种AT菌,进行了农药阿特拉津的静态降解实验及其污染地下水的微生物治理模拟实验研究结果表明,AT菌在pH值为5.0～10.0时对农药污染质阿特拉津均具有降解能力,且适宜的pH值范围为6.5～8.0;在实验条件(t=10℃,pH=7.5)与野外含水层的条件基本一致情况下,难于生物降解的污染质阿特拉津的一次投菌降解率达到31.08%;同时环境因素也随着AT菌作用的变化而变化,其中,DO、pH随AT菌作用加强而其值减小.另外,设计了细菌的投放方式以模拟野外条件下的菌种投加条件.并且AT菌的作用会造成被治理含水层的渗透性能降低,实验后含水层的渗透系数下降60.54%.清水冲洗10d的渗透性恢复率为48.96%,说明清水渗透恢复的方法效果明显.     

大气过氧化氢及有机过氧化物的测定

采用ＨＰＬＣ柱后衍生荧光法测定了５、６月份中关村地区大气中的Ｈ２Ｏ２和有机过氧化物,除Ｈ２Ｏ２外,共测出了７种以上有机过氧化物。有３种通过ＨＰＬＣ色谱保留时间得到了鉴定。分别是甲基过氧化氢,羟甲基过氧化氢和乙基过氧化氢。