Inverse modeling of multicomponent reactive transport through single and dual porosity media

Compacted bentonite is foreseen as buffer material for high-level radioactive waste in deep geological repositories because it provides hydraulic isolation, chemical stability, and radionuclide sorption. A wide range of laboratory tests were performed within the framework of FEBEX (Full-scale Engineered Barrier EXperiment) project to characterize buffer properties and develop numerical models for FEBEX bentonite. Here we present inverse single and dual-continuum multicomponent reactive transport models of a long-term permeation test performed on a 2.5 cm long sample of FEBEX bentonite. Initial saline bentonite porewater was flushed with 5.5 pore volumes of fresh granitic water. Water flux and chemical composition of effluent waters were monitored during almost 4 years. The model accounts for solute advection and diffusion and geochemical reactions such as aqueous complexation, acid-base, cation exchange, protonation/deprotonation by surface complexation and dissolution/precipitation of calcite, chalcedony and gypsum. All of these processes are assumed at local equilibrium. Similar to previous studies of bentonite porewater chemistry on batch systems which attest the relevance of protonation/deprotonation on buffering pH, our results confirm that protonation/deprotonation is a key process in maintaining a stable pH under dynamic transport conditions. Breakthrough curves of reactive species are more sensitive to initial porewater concentration than to effective diffusion coefficient. Optimum estimates of initial porewater chemistry of saturated compacted FEBEX bentonite are obtained by solving the inverse problem of multicomponent reactive transport. While the single-continuum model reproduces the trends of measured data for most chemical species, it fails to match properly the long tails of most breakthrough curves. Such limitation is overcome by resorting to a dual-continuum reactive transport model.     

Identification of key parameters controlling dissolved oxygen migration and attenuation in fractured crystalline rocks

In the crystalline rocks of the Canadian Shield, geochemical conditions are currently reducing at depths of 500-1000 m. However, during future glacial periods, altered hydrologic conditions could potentially result in enhanced recharge of glacial melt water containing a relatively high concentration of dissolved oxygen (O2). It is therefore of interest to investigate the physical and geochemical processes, including naturally-occurring redox reactions, that may control O2 ingress. In this study, the reactive transport code MIN3P is used in combination with 2k factorial analyses to identify the most important parameters controlling oxygen migration and attenuation in fractured crystalline rocks. Scenarios considered are based on simplified conceptual models that include a single vertical fracture, or a fracture zone, contained within a rock matrix that extends from the ground surface to a depth of 500 m. Consistent with field observations, Fe(II)-bearing minerals are present in the fractures (i.e. chlorite) and the rock matrix (biotite and small quantities of pyrite). For the parameter ranges investigated, results indicate that for the single fracture case, the most influential factors controlling dissolved O2 ingress are flow velocity in the fracture, fracture aperture, and the biotite reaction rate in the rock matrix. The most important parameters for the fracture zone simulations are flow velocity in the individual fractures, pO2 in the recharge water, biotite reaction rate, and to a lesser degree the abundance and reactivity of chlorite in the fracture zone, and the fracture zone width. These parameters should therefore receive increased consideration during site characterization, and in the formulation of site-specific models intended to predict O2 behavior in crystalline rocks.     

Mixing-controlled biodegradation in a toluene plume--results from two-dimensional laboratory experiments

Various abiotic and biotic processes such as sorption, dilution, and degradation are known to affect the fate of organic contaminants, such as petroleum hydrocarbons in saturated porous media. Reactive transport modeling of such plumes indicates that the biodegradation of organic pollutants is, in many cases, controlled by mixing and therefore occurs locally at the plume's fringes, where electron donors and electron-acceptors mix. Herein, we aim to test whether this hypothesis can be verified by experimental results obtained from aerobic and anaerobic degradation experiments in two-dimensional sediment microcosms. Toluene was selected as a model compound for oxidizable contaminants. The two-dimensional microcosm was filled with quartz sand and operated under controlled flow conditions simulating a contaminant plume in otherwise uncontaminated groundwater. Aerobic degradation of toluene by Pseudomonas putida mt-2 reduced a continuous 8.7 mg L(-1) toluene concentration by 35% over a transport distance of 78 cm in 15.5 h. In comparison, under similar conditions Aromatoleum aromaticum strain EbN1 degraded 98% of the toluene infiltrated using nitrate (68.5+/-6.2 mg L(-1)) as electron acceptor. A major part of the biodegradation activity was located at the plume fringes and the slope of the electron-acceptor gradient was steeper during periods of active biodegradation. The distribution of toluene and the significant overlap of nitrate at the plume's fringe indicate that biokinetic and/or microscale transport processes may constitute additional limiting factors. Experimental data is corroborated with results from a reactive transport model using double Monod kinetics. The outcome of the study shows that in order to simulate degradation in contaminant plumes, detailed data sets are required to test the applicability of models. These will have to deal with the incorporation of existing parameters coding for substrate conversion kinetics and microbial growth.     

Downward Migration of Dense Bottom Currents

The focus of this paper is on the dynamics of a dense current flowing along the continental slope, and the frictionally induced downward motion it experiences. In particular, the movement of the lateral boundaries where the isopycnals meet the bottom are considered. The current is taken to be wide compared to the Rossby radius, which is in accordance with observations and makes the dynamics quasigeostrophic. The time development of the plume thickness is studied, using three different parameterisations for the bottom friction.Independently of the choice of parameterisation, the following results are obtained: In the central part of the plume friction acts as a diffusive process to minimise the curvature of the upper surface of the plume. At the upper edge the plume quickly approaches a state with small slope, i.e. small geostrophic velocity and small frictionally induced downward flow. At the lower edge a tongue of dense water shoots out creating a widening layer. The thickness of the migrating layer is approximately equal to the boundary layer depth and its downward speed is comparable to the along-slope geostrophic velocity. The downslope end of the migrating layer may form a steep front which requires some precautions in the numerical procedure.     

粤北地区一次臭氧污染过程分析及数值模拟

2020年7月1日,粤北地区出现了一次O₃污染过程,其中韶关市录得全省最高值162μg·m^-3.本文利用常规观测资料以及再分析资料对影响此次韶关地区O₃污染过程的主要气象场特征进行分析,结果表明：6月28日—7月2日天气形势总体处于静稳状态,地面受到均压场控制,同时副热带高压较强,脊线位于韶关上空,导致中高层有下沉气流,抑制了垂直方向污染物的扩散.6月28—30日(污染积累阶段),风速较大,韶关在外来输送和污染扩散条件的共同作用下,O₃浓度上升但未超标.7月1日(污染持续阶段),韶关和清远两地风速减小,污染扩散条件不利;同时气温有所上升,光化学反应作用增强,有利于O₃浓度攀升;同时广州和佛山两地的风向从偏南风转为偏北风,韶关市维持偏南风,主导风向的差异是全省只有韶关O₃超标的主要原因.7月2日(污染消散阶段),O₃外来传输及本地生成作用减弱,全省O₃浓度下降.进一步利用HYSPLIT后向轨迹以及WRF-CMAQ空...     

常州市臭氧污染传输路径和潜在源区

利用NCEP全球再分析资料和HYSPLIT4模式,计算了2013—2015年常州市臭氧(O_3)超标日的气流后向轨迹。结合聚类分析方法和常州市PM2.5、PM10、SO2、NO2、O_3数据,分析了O_3超标日不同类型气团来源对各污染物浓度的影响,并利用引入权重因子后的潜在污染源贡献函数分析了影响常州市O_3超标的潜在污染源区分布特征。结果表明:常州市O_3超标期间易受到东南和西南方向气流影响,其中从东海和黄海途经浙江东北部、上海、江苏南部等地的东南气流占比达50%以上。自内陆途经黄山-湖州-宜兴到常州的气流对应的O_3平均质量浓度最高,为116μg/m3。自山东经枣庄-宿迁-淮安-泰州-苏州-无锡到常州的气流对应的O_3平均质量浓度最低,为78μg/m3,但该气流对应的SO2和NO2平均值为各聚类中的最高。影响常州市O_3的潜在污染源区主要在常州周边200 km以内的区域,且集中在从南京至上海的长江下游沿线区域和杭州湾区域;其中太湖湖区为重点污染源源区之一。O_3超标日影响常州NO2的潜在污染源区主要集中在江苏南部、浙江东北部和上海3个区域,太湖周边的常州、无锡、苏州和湖州等几个临近城市为潜在的重点污染源区。与影响常州O_3的WPSCF高值区相比,影响NO2的高值区分布范围更大、距离更远。影响常州O_3的潜在污染源区分布,与长江三角洲地区人为源大气污染物的高排放区域较为一致,说明长江三角洲地区的O_3污染与本区域的人为源大气污染物排放有着极为密切的关联。     

海口市臭氧污染特征

基于2013—2015年海口市4个空气质量自动监测站点数据,结合气象资料,分析了海口市O_3的污染特征。结果表明:海口市O_3总体优良,优良天数比例为99.4%,污染天数均为轻度污染;在良和污染天数中,O_3作为首要污染物的天数占40%,超过其他5项污染物占比。海口市10月O_3浓度最高。O_3月均浓度与温度呈负相关关系,同时与风向有密切关系:5—8月气温较高,以南风为主,O_3浓度较低;1月北风频率较高,易受外来污染传输作用,O_3浓度相对较高。O_3超标日以东北风为主,日变化并未呈现单峰型特征,12:00—22:00时段O_3浓度在10%范围内小幅变化。台风外围型和北方冷高压底部型是造成海口市O_3超标的2类典型天气形势。     

微生物-光-电化学耦合技术降解污染物和回收能源的研究进展

微生物电化学技术能同时实现污染物去除和能量回收,但存在污染物去除种类有限及产能效率低的局限,近几年将可再生的太阳能引入微生物电化学技术的微生物-光-电化学耦合技术应运而生。本文简要介绍了微生物-光-电化学耦合技术的发展背景和研究现状,对该技术现有的耦合形式进行分类,并对各种形式的耦合机理进行详细的阐释,最后对其未来的发展进行了展望。     

非平衡式双极性离子风消电技术与应用

为实现风送管道物料静电监测与控制,预防料仓静电燃爆事故,提高聚烯烃装置料仓安全水平,基于非平衡式双极性离子风消电技术,开发了双极性离子风消电器;基于离子风消电器和静电监测器,探讨了石化粉体料仓用离子风消电控制系统组成、电路、气路布局;对非平衡式双极性离子风消电系统进行现场应用测试。结果表明:基于此管道粉体消静电技术,合理调节正、负侧控制电压,可有效控制管道物料荷质比稳定在±0.3 μC/kg以内,保障聚烯烃装置料仓安全、稳定运行。     

Changes in Streambed Composition in Salmonid Spawning Habitat of the Elwha River during Dam Removal

One uncertainty associated with large dam removal is the level of downstream sediment deposition and associated short‐term biological effects, particularly on salmonid spawning habitat. Recent studies report downstream sediment deposition following dam removal is influenced by proximity to the source and river transport capacity. The impacts of dam removal sediment releases are difficult to generalize due to the relatively small number of dam removals completed, the variation in release strategies, and the physical nature of systems. Changes to sediment deposition and associated streambed composition in the Elwha River, Washington State, were monitored prior to (2010‐2011) and during (2012‐2014) the simultaneous removal of two large dams (32 and 64 m). Changes in the surface layer substrate composition during dam removal varied by year and channel type. Riffles in floodplain channels downstream of the dams fined and remained sand dominated throughout the study period, and exceeded levels known to be detrimental to incubating salmonids. Mainstem riffles tended to fine to gravel, but appear to be trending toward cobble after the majority of the sediment was released and transported through system. Thus, salmonid spawning habitats in the mainstem appear to have been minimally impacted while those in floodplain channels appear to have been severely impacted during dam removal.