Methane reductions: Implications for global warming and atmospheric chemical change

Atmospheric methane (CH₄) concentrations have more than doubled over the last two centuries. These increases may contribute to global warming, enhance formation of tropospheric ozone, suppress OH and affect stratospheric ozone. Calculations show that stabilization of CH₄ could reduce projected temperature increases and possibly mitigate background tropospheric O₃ increases due to increasing levels of CH₄.     

On the mean daily and seasonal variations of the vertical ozone profiles in the lower troposphere

During the 15 year period that the Zugspitze cable car has operated between the valley (1 km a.s.l.) and Zugspitze peak (3 km a.s.l.) at the northern border of the Bavarian Alps, it has been used for investigating the profiles of meteorological and atmospheric electrical parameters, and Aitken nuclei. This cable railway is rather steep and is suspended mostly far away from the ground. From 1980 to 1982 nearly 2000 ozone profiles were additionalyrecorded. The data collected offer a profound basis in order to study the time variations of the lower tropospheric ozone profile depending on the hour of the day during all the seasons. In this paper the following are reported: the shape and time behaviour of ozone profiles in different seasons depending on the vertical mixing intensity, stratospheric intrusions and the penetration depth of the stratospheric O₃.     

Comparison of different disinfection processes in the effective removal of antibiotic-resistant bacteria and genes

This study compared three different disinfection processes(chlorination, E-beam, and ozone) and the efficacy of three oxidants(H2O2, S2O-8, and peroxymonosulfate(MPS)) in removing antibiotic resistant bacteria(ARB) and antibiotic resistance genes(ARGs) in a synthetic wastewater. More than30 mg/L of chlorine was needed to remove over 90% of ARB and ARG. For the E-beam method, only1 dose(kGy) was needed to remove ARB and ARG, and ozone could reduce ARB and ARG by more than 90% even at 3 mg/L ozone concentration. In the ozone process, CT values(concentration × time)were compared for ozone alone and combined with different catalysts based on the 2-log removal of ARB and ARG. Ozone treatment yielded a value of 31 and 33(mg·min)/L for ARB and ARGs respectively. On the other hand, ozone with persulfate yielded 15.9 and 18.5(mg·min)/L while ozone with monopersulfate yielded a value of 12 and 14.5(mg·min)/L. This implies that the addition of these catalysts significantly reduces the contact time to achieve a 2-log removal, thus enhancing the process in terms of its kinetics.     

Simulation of ozone intrusion caused by a tropopause fold and cut-off low

A tropopause fold and cut-off low developed over Europe at the end of April 1982 and enhanced the exchange of air between the stratosphere and troposphere. The episode has been simulated using the EURAD model which has been designed for long-range transport simulation for European conditions. Applying a linear relationship between potential vorticity and ozone, concentration fields of the tracer and their changes due to outflow of ozone-rich air from the stratosphere could be simulated. A considerable decrease of stratospheric ozone was also obtained. This indicates noticeable mixing of tropospheric air with reduced ozone content into the stratosphere during the episode. Strong downward fluxes more than an order of magnitude larger than normal when averaged over the model domain show up around levels close to the tropopause. Obviously, dynamical processes fovern teh ozone budget o the upper troposphere during the vigorous intrusion event. Drastic increases of ozone also occur in the lower troposphere but are probably underestimated since vertical mixing by clouds is not taken into account in the simulation experiments. It is intended to explore the interaction of ozone of stratospheric and tropospheric (anthropogenic) origin in further experiments.     

The ozone record at Payerne: An assessment of the cross-tropopause flux

Ozone soundings from the 21-year record at Payerne (47°N, 7°E) are analysed. At the 300 mb level a simple statistical technique makes it possible to distinguish between the ozone of tropospheric photochemical origin and that in stratospheric intrusions. It is estimated that stratospheric intrusion is the source of 25% of the observed ozone mixing ratio at 300 mb. The maximum stratosphere to troposhere flux of ozone occurs in late winter/spring.A box model is developed for a Northern Hemisphere troposphere with stratosphere-troposphere exchange parameterized in terms of the baroclinic eddy activity but no tropospheric in situ source of ozone. It shows the same seasoanlity in ozone mixing ratio as the Payerne data, suggesting the assumed exchange mechanism to be reasonable.     

Parameterization of episodical cloud and rainout events in large-scale atmospheric chemistry models

A parameterization scheme taking into account the episodical nature of rainout and incloud chemical transformation has been tested in a 2-D channel model. In the liquid phase many soluble gases are observed in concentrations never experienced in the gas phase. The effects on the trace gases SO₂ and hydrogen peroxide, when they are modified by clouds and precipitation, are studied. When incloud interaction of SO₂ and hydrogen peroxide is taken into consideration, calculated hydrogen peroxide profiles are brought closer to observed distributions. The effect of varying the time periods between cloud and rain events is tested. The impact on the formation and destruction of tropospheric ozone is also discussed.     

Effect of clouds on photolysis rates at the surface: A practical method of estimation and its application to a modeling study of the formation of photochemical oxidants

Up to now, theoretical parametrization of the influence of clouds on photolytic reactions still meets with difficulties. Thus we developed a practical method relying on measurements of the u.v. flux compared to that expected for cloudless conditions, over a diurnal range, on successive days. The impact of the depletion in the photolytic constants, varying according to five different groups of reactions, has been estimated by a simulation of photochemical smog with various chemical mechanisms. Under current weather conditions, the ozone and PAN decreases varied from 11 to 20%; on the contrary NO₂ and HNO₂ were found to increase. Limitations of the method are discussed.     

Relationships between synoptic-scale atmospheric circulation and ozone concentrations in Metropolitan Pittsburgh,Pennsylvania

A synoptic climatology demonstrates the relationships between the atmospheric circulation and surface ozone (O₃) concentrations. To deduce these associations, a subjective synoptic classification scheme is applied to 10 years' O₃ data from the Pittsburgh metropolitan area. The results focus on four aspects of the atmospheric circulation-O₃ relationship: average, extreme-event, between season and year-to year conditions. On average, each of the nine circulation types is related to a characteristic O₃ concentration level and cumulative O₃ dose. Extreme high-O₃ events are associated with either the western side of a slowly migrating anticyclone or a stagnating extended high-pressure ridge; low-O₃ events are experienced under cool and cloudy cyclonic conditions. Between-season variations in the average and extreme circulation-O₃ relationshipsare observed: the high-pressure features that produce the high st O₃ levels in summer are related to low levels in winter, while circulation patterns that contribute very little to summertime O₃ build-up are associated with the highest levels of wintertime O₃. The latter situation could be caused by tropopause folding and the introduction of stratospheric ozone in winter months. While zonal (meridional) circulation regimes tend to produce lower (higher) mean annual O₃ levels, such year-to-year changes in synoptic-type frequencies do not appear to be strongly related to interannual variations in O₃, and other non-climatic factors appear to be of greater importance.     

冬小麦田O3气孔与非气孔沉降及风险评估

为了深入了解农田生态系统的O_3干沉降过程,并基于O_3通量(尤其是气孔O_3累积通量)指标进行风险评估,利用涡度相关系统对冬小麦田的O_3干沉降过程进行了连续动态观测,初步分析O_3浓度和总O_3通量的变化过程,着重探析气孔O_3沉降和非气孔O_3沉降的变化特征及其与主要气象因子的关系,并基于剂量指标(AOT40)和通量指标(DF_s06)分别推算出冬小麦的产量损失率.结果表明,观测期间(自2016年3月16日至5月30日)日平均O_3浓度(cO_3)为32.9 n L·L-1;白天(08:00~18:00)和夜间平均总O_3通量(F_(O3))分别为-7.6 nmol·(m~2·s)~(-1)和-3.1 nmol·(m~2·s)~(-1),日均F_(O3)为-5.1nmol·(m~2·s)~(-1).逐日平均气孔O_3通量(F_s)的变化范围为0~-5.1 nmol·(m~2·s)~(-1),日均F_s为-1.43 nmol·(m~2·s)~(-1).逐日平均非气孔O_3通量(F_(ns))的变化范围为-1.43~-10.31 nmol·(m~2·s)~(-1),日均F_(ns)为-3.66 nmol·(m~2·s)~(-1).较强的太阳辐射(SR)、较高的温度(T)和适度湿润的条件有利于冬小麦气孔沉降;较强的SR、适度的T和湿润条件是有利于冬小麦非气孔沉降.在整个观测期间,总O_3累积吸收通量(DF_(O3))、气孔O_3累积吸收通量(DF_s)和非气孔O_3累积吸收通量(DF_(ns))分别为31.58、9.99和21.59 mmol·m~(-2),总DF_s和总DF_(ns)分别占总DF_(O3)的32%和68%.通过剂量指标AOT40和通量指标DF_s06响应方程计算出的冬小麦产量损失率分别为11.58%~20.37%和20%~23.56%.     

臭氧在冰晶及硫酸铵和亚硫酸铵渗溶冰晶上的粘着系数

利用流动管式反应器,在220-260K温度范围内,实验测量了臭氧在低温冰晶及硫酸铵和亚硫酸铵渗溶冰晶表面上的粘着系数.结果表明:臭氧在低温冰晶表面上的粘着系数随温度升高而增大, 其粘着系数为1.3×10-7-2.7×10-6; 臭氧在硫酸铵和亚硫酸铵渗溶冰晶表面上的粘着系数与二者浓度呈非线性关系; 利用实验结果估算了臭氧在极地平流层云中存留寿命约为56d, 臭氧在主要组成为水的冰晶表面上的损耗不容忽视.     

Effects of O3/Cl2 disinfection on corrosion and opportunistic pathogens growth in drinking water distribution systems

The effects of O_3/Cl_2 disinfection on corrosion and the growth of opportunistic pathogens in drinking water distribution systems were studied using annular reactors(ARs).The corrosion process and most probable number(MPN) analysis indicated that the higher content of iron-oxidizing bacteria and iron-reducing bacteria in biofilms of the AR treated with O_3/Cl_2 induced higher Fe_3O_4 formation in corrosion scales.These corrosion scales became more stable than the ones that formed in the AR treated with Cl_2 alone.O_3/Cl_2 disinfection inhibited corrosion and iron release efficiently by changing the content of corrosion-related bacteria.Moreover,ozone disinfection inactivated or damaged the opportunistic pathogens due to its strong oxidizing properties.The damaged bacteria resulting from initial ozone treatment were inactivated by the subsequent chlorine disinfection.Compared with the AR treated with Cl_2 alone,the opportunistic pathogens M.avium and L.pneumophila were not detectable in effluents of the AR treated with O_3/Cl_2,and decreased to(4.60 ± 0.14) and(3.09 ± 0.12) log10(gene copies/g corrosion scales) in biofilms,respectively.The amoeba counts were also lower in the AR treated with O_3/Cl_2.Therefore,O_3/C_l2 disinfection can effectively control opportunistic pathogens in effluents and biofilms of an AR used as a model for a drinking water distribution system.     

氮掺杂生物炭催化臭氧对于布洛芬的降解特性与机制

系统研究了新型氮掺杂生物炭材料(N-C)催化臭氧对于水中布洛芬(IBP)的氧化降解效能及机制,并深入探究了初始pH、臭氧投加量、催化剂投加量、不同阴离子和背景水质条件对IBP降解效率的影响.结果 表明,相较于一些常见的碳基催化剂(g-C3N4、生物炭、颗粒活性炭)及金属催化剂(MnO2、Fe3O4),N-C催化臭氧体系...     

高能电子沉降对北半球冬季中高层大气活性氮和臭氧影响的数值模拟

高纬度地区平流层臭氧浓度对极地地表生物地球化学过程影响巨大,近年来高能电子沉降对大气臭氧和活性氮的影响成为新的关注点。本工作基于化学-气候耦合模式SOCOL3.0,参考第六次耦合模式比较计划（CMIP6）推荐的低能量电子（LEE）和中能量电子（MEE）的参数化方案构建了SOCOL-EPP-ECNU化学-气候模式,利用该模式对高能电子沉降对中高层大气活性氮（NO_x）和臭氧的影响进行了敏感性试验和评估。结果表明,中高层大气对于LEE效应产生的NO_x通量的上边界条件设定敏感度很高,该设定对模式模拟效果有决定性意义。加入LEE和MEE通量后,模式对北半球冬季平流层中下层NO_x浓度的模拟精度得到提高,同时也使北半球冬季平流层中下层气温的模拟得到改善。模拟结果指示,加入LEE和MEE,进一步完善对高能粒子沉降的模式描述,有助于提高模式对大气化学成分及气候要素模拟的准确度。     

佛山臭氧浓度预报方程的建立与应用

臭氧作为大气中的二次污染物,其形成和变化复杂,臭氧预报更是当下空气污染治理的难题之一.通过分析2014~2017年佛山地区近地面O₃浓度与高低层气象要素的关系,建立了佛山O₃浓度预报方程,并进行了检验和应用.结果表明,佛山近地面O₃的变化与高低层气象要素关系密切,气温和日照时数等气象要素与O₃浓度呈显著正相关,相对湿度、总（低）云量和风速等与其呈负相关;高浓度O₃污染发生的气象条件为小风速、晴间少云、低相对湿度、较长的日照时间和较高的温度,高浓度O₃潜势指数（HOPI）和风向指数（WDI）的定义可以较好地衡量O₃污染气象条件的好坏;综合考虑HOPI和不同高度WDI等13种气象要素,采用多指标叠套和多元逐步回归建立了佛山地区臭氧浓度预报方程;利用2018年资料检验发现,模拟值与实测值二者的相关系数R可达0.82,预报方程具有良好的拟合效果和可预报性.     

Evaluation of a number of chemical mechanisms for their application in models describing the formation of photochemical ozone in Europe

A series of 24 chemical mechanisms from the literature are compared against each other using harmonized emissions, photolysis rate coefficients for simple inorganic chemistry and life cycle data for ozone, PAN and H₂O₂. The evaluation sought to understand the impact of parameterizing hydrocarbon oxidation on the peak concentrations of photochemically-generated secondary pollutants. Only seven of the 24 chemical mechanisms gave peak concentrations of ozone, PAN and H₂O₂ simultaneously in their respective central ranges. PAN and H₂O₂ were generally calculated with a much lower precision compared to ozone. Only 11 mechanisms out of 24 gave responses to both 50% hydrocarbons and NO_x emissions controls in their respective central bands. The lack of coordinated ozone, PAN and hydrogen peroxide measurements across Europe currently limits the adequacy of model comparisons and hence the confidence which may be placed in assessments of likely impacts of future control strategies.     

Degradation of endocrine disruptor bisphenol A in drinking water by ozone oxidation

The ozone oxidation of endocrine disruptor bisphenol A in drinking water was investigated. A stainless completely mixed reactor was employed to carry out the degradation experiments by means of a batch model. With an initial concentration of 11.0 mg/L, the removal efficiencies of BPA (bisphenol A) could be measured up to 70%, 82%, and 90% when the dosages of ozone were 1, 1.5, and 2 mg/L, respectively. The impacts on BPA degradation under the conditions of different ozone dosages, water background values, BPA initial concentrations, and ozone adding time were analyzed. The results showed that ozone dosage plays a dominant role during the process of BPA degradation, while the impact of the contact time could be ignored. UV wavelength scanning was used to confirm that the by-products were produced, which could be absorbed at UV254. The value of UV254 was observed to have changed during the ozonation process. Based on the change of UV254, it could be concluded that BPA is not completely degraded at low ozone dosage, while shorter adding time of total ozone dosage, high ozone dosage, and improvement of dissolved ozone concentration greatly contribute to the extent of BPA degradation. The effects of applied H₂O₂ dose in ozone oxidation of BPA were also examined in this study. The O₃-H₂O₂ processes proved to have similar effects on the degradation of BPA by ozone oxidation. Translated from Environmental Science, 2006, 27(2): 294–299 [译自: 环境科学]     

化学预氧化对苏氨酸生成三氯乙醛的影响

以具有最大比三氯乙醛生成潜能(SCHFP)的苏氨酸为研究对象,分析了次氯酸钠(NaClO)、二氧化氯(ClO_2)、高锰酸钾(KMnO_4)、过氧化氢(H_2O_2)、臭氧(O_3)和臭氧过氧化氢(O_3/H_2O_2)等预氧化剂对三氯乙醛(CH)生成的影响,以确定合适的预氧化剂及其适宜投加量,为CH的控制提供指导.结果表明,能够有效去除一天CH生成量(CH1d)的预氧化方式依次为H_2O_2、ClO_2、KMnO_4和NaClO,适宜投加量分别为3、0.5、0.6和0.5mg·L-1,对CH1d相应的去除率分别为61.54%、47.63%、29.77%和10.94%;能够有效去除CH生成潜能(CHFP)的预氧化方式依次为KMnO_4、NaClO、H_2O_2和ClO_2,适宜投加量分别为0.6、0.5、3和0.5mg·L~(-1),对CHFP相应的去除率分别为41.01%、33.38%、8.36%和2.40%;O_3和O_3/H_2O_2预氧化能够使CH1d和CHFP增加,不适用于对CH的控制.     

Pathway of the ozonation of 2,4,6-trichlorophenol in aqueous solution

The reaction mechanism and pathway of the ozonation of 2,4,6-trichlorophenol (2,4,6-TCP) in aqueous solution were investigated. The removal efficiency and the variation of H₂O₂, Cl⁻ formic acid, and oxalic acid were studied during the semi-batch ozonation experiments (continuous for ozone gas supply, fixed volume of water sample). The results showed that when there was no scavenger, the removal efficiency of 0.1 mmol/L 2,4,6-TCP could reach 99% within 6 min by adding 24 mg/L ozone. The reaction of molecular ozone with 2,4,6-TCP resulted in the formation of H₂O₂. The maximal concentration of H₂O₂ detected during the ozonation could reach 22.5% of the original concentration of 2,4,6-TCP. The reaction of ozone with H₂O₂ resulted in the generation of a lot of OH• radicals. Therefore, 2,4,6-TCP was degraded to formic acid and oxalic acid by ozone and OH• radicals together. With the inhibition of OH• radicals, ozone molecule firstly degraded 2,4,6-TCP to form chlorinated quinone, which was subsequently oxidized to formic acid and oxalic acid. Two reaction pathways of the degradation of 2,4,6-TCP by ozone and O₃/OH• were proposed in this study. Translated from Acta Scientiae Circumstantiae, 2005, 25(12): 1619–1623 [译自: 环境科学学报]     

The role of non-precipitating clouds in producing ambient sulfate during summer: Results from simulations with the Acid Deposition and Oxidant Model (ADOM)

A comprehensive acid deposition model was used to investigate the importance of non-precipitating stratus clouds for the production of ambient sulfate. A comparison of model estimates of ambient sulfate and SO₂ concentrations with corresponding observations for an episode in the summer of 1988 showed that the model underestimated ambient sulfate concentrations and overestimated ambient SO₂ concentrations when non-precipitating stratus clouds were ignored in the model formulation. When the model was modified to include non-precipitating stratus clouds, a distinct improvement in model performance was obtained.     

我国PM2.5与臭氧污染协同控制策略研究

近年来,我国大气污染格局发生了深刻变化,PM_2.5与臭氧（O₃）成为影响我国城市和区域空气质量的主要空气污染物,二者协同控制已成为我国空气质量改善的焦点和打赢蓝天保卫战的关键.PM_2.5与臭氧之间具有复杂的关联性,使得二者的协同控制具有复杂性与艰巨性.分析了PM_2.5与臭氧成因的关联性及其相互影响,阐明了PM_2.5与臭氧污染协同控制所涉及的重要科学问题,并在此基础上研究了目前我国PM_2.5与臭氧的污染形势及二者的关联性,梳理了我国自2013年以来在PM_2.5与臭氧污染控制中已采取的重要举措,论述了目前我国PM_2.5与臭氧协同控制在科学与管理上所面临的挑战.结合对国外成功经验的分析,提出推进我国PM_2.5与臭氧污染协同控制工作的相关建议:①加快监测能力建设,完善管理体系;②强化科技支撑,提高PM_2.5与臭氧污染控制精准性;③加快构建VOCs与NO_x治理技术体系;④加大VOCs与NO_x的协同减排力度,保障减排方案落实到位.