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71.
地球表生环境在地质历史时期经历了剧烈的波动,为当前建设宜居地球提供了重要参照。铁组分是重建古海洋氧化还原状态演化的重要指标,但现有的研究集中于FeHR/FeT和Fepy/FeHR两个比值的应用,而对其中不同组分所携带的信息缺少深入的挖掘。本研究统计了已发表的、泥盆纪之前的、采用程序萃取方法获得的铁组分数据,对其中不同的组分所可能指示的海洋化学信息进行了研究。我们发现氧化环境中氧化铁的含量有可能用于追踪长周期上大气-海洋系统的氧含量波动、总铁含量与海洋中铁的含量密切相关、铁化环境中黄铁矿铁的含量对海洋硫酸盐库大小的演化有很好的响应。我们的工作表明,铁组分指标是指示海洋局部氧化还原状态的强大指标,其不同的组分与海洋中氧气、碳和硫酸盐等存在极强的交互过程,可以被用来重建海洋的化学演化。  相似文献   
72.
Microbial activity in permeable tidal flat margin sediments is enhanced by two main processes. First, organic matter is supplied by rapid sedimentation at prograding tidal flat margins. Second, surface and deep pore water advection lead to a replenishment of the dissolved organic matter and sulfate pools. Increasing microbial activity towards the low water line is reflected in sulfate and methane profiles as well as in total cell numbers, sulfate reduction rates, and remineralization products. The impact of high sedimentation rates on pore water biogeochemistry is confirmed by inverse modeling reproducing the depth profiles obtained by measurements. In central parts of the tidal flats, low sedimentation rates and pore water flow velocities limit microbial activity despite the high availability of electron acceptors for microbial respiration such as sulfate. Therefore, tidal flat margins with high microbial activity are of special importance for budgeting biogeochemical cycling in tidal flat areas.  相似文献   
73.
 Pore water concentration profiles of sediments at a site on the Amazon Fan were investigated and simulated with the numerical model CoTReM (column transport and reaction model) to reveal the biogeochemical processes involved. The pore water profiles for gravity core GeoB 4417-7 showed a distinct sulfate–methane transition zone in which deep sulfate reduction occurs. Only a small sulfide peak could be observed at the reaction zone. Due to high amounts of iron minerals, the produced sulfide is instantaneously precipitated in form of iron sulfides. We present a simulation which starts from a steady state system with respect to pore water profiles for methane and sulfate. Furthermore, sulfide, iron, pH, pE, calcium and total inorganic carbon (TIC) were included in the simulation. The program calculated mineral equilibria to mackinawite, iron sulfides (more stable than mackinawite), iron hydroxides and calcite via saturation indices (SI) by a module incorporating the program PHREEQC (Parkhurst 1995). The measured sulfide and iron profiles are obtained in the simulation output by using a constant SI (=0) for mackinawite and calcite, while a depth dependent SI distribution is applied for the PHREEQC phases “Pyrite” and “Fe(OH)3(a)”, representing a composition and the kinetics of different iron sulfides and iron hydroxides. These SI distributions control the results of sulfide and iron pore water profiles, especially conserving the sulfide profile at the reaction zone during the simulation. The results suggest that phases of iron hydroxides are dissolved, mackinawite is precipitated within, and other iron sulfides are precipitated below the reaction zone. The chemical reactivity of iron hydroxides corresponds to the rate of sulfide production. The system H2O–CO2–CaCO3 is generally successfully maintained during the simulation. Deviations to the measured pH profile suggest that further processes are active which are not included in the simulation yet. Received: 9 November 1998 / Accepted: 26 October 1999  相似文献   
74.
Precipitation of Aluminium and Phosphate Affected by Acidification Acidified waters often show elevated concentrations of Al (with up to 6 mg L–1 being not unusual). A pH increase resulting e.g. from mixing with non‐acidified water or from biological activities may be linked with Al precipitation. Up to now, this phenomenon was described for acid mine drainages. This investigation focuses on a whitish precipitate naturally formed in a brook of an atmospherically acidified catchment in the Ore Mountains, Germany. Based on infrared spectra the precipitate was identified as an Al‐hydroxosulfate with crystal water. A simulation of natural conditions in the laboratory showed that Al precipitated only if sulfate or phosphate ions were added to the solution. In the case of sulfate being added, the infrared spectrum of the precipitate was similar to the natural precipitate. 27Al NMR spectroscopy revealed tetrahedrally coordinated Al in some precipitates which evidences the participation of the tridecameric [Al13O4(OH)24(H2O)12]7+ cation beside other polymeric Al cations. Precipitation experiments subjected to the given conditions showed that the phosphate elimination from solution with Al was much higher than with Fe. With Al and Fe added together, the P elimination rate was likewise high, and phosphate was bound onto Al in the precipitate. This was demonstrated by SEM‐EDX spectroscopy. Based on these results we present a possible reaction mechanism. The precipitation of Al together with P allows a significant retention of both elements in sediments because in contrast to Fe, Al immobilizes phosphate even under anoxic conditions.  相似文献   
75.
为了研究烟花爆竹燃放对空气质量的影响,利用动态滤膜校准系统-微量震荡天平法颗粒物分析仪、大气细颗粒化学组分在线离子色谱监测仪、有机碳(OC)/元素碳(EC)在线分析仪、气态污染物分析仪、常规自动气象站并结合云高仪和微波辐射计等设备于2015年2月18日至3月7日对天津市细颗粒物(PM2.5)及其主要化学组分,气态污染物(SO2、NO2、CO和O3)和气象参数进行连续观测。本文选取3个污染事件作为研究重点进行分析,研究发现:烟花爆竹禁放和限放政策导致除夕夜烟花爆竹燃放量减少,PM2.5峰值与2014年相比明显下降;烟花爆竹禁放和限放区的设立导致天津市PM2.5质量浓度在烟花爆竹密集燃放期间存在明显的空间差异;站点之间小时平均值差异最高达到394 μg/m3。受烟花爆竹燃放的影响,距地面80 m以下颗粒物后向散射强度相近,表明80 m以下颗粒物呈均匀分布。污染事件1是由于烟花爆竹密集燃放引起的,PM2.5主要化学组分为K+、SO42-和Cl-,同时SO2和CO质量浓度显著升高;但EC和OC质量浓度并未明显增加。污染事件2的形成是由于不利的气象条件(逆温、逆湿、下沉气流和较高的相对湿度)促进了SO2和NOx在烟花爆竹排放的颗粒物表面发生非均相化学反应,导致SO42-和NO3-浓度快速增加。污染事件3由元宵节烟花爆竹燃放引发,而后呈现二次无机组分与臭氧协同增长的复合型污染特征;此外区域传输对污染事件3也有重要贡献。  相似文献   
76.
中国地区硫酸盐气溶胶的第一间接气候效应研究   总被引:14,自引:6,他引:8  
将区域气候模式(RegCM3)与对流层大气化学模拟(TACM)耦合,建立区域气候化学模拟系统(RegCCMS),用以模拟中国地区硫酸盐气溶胶的空间分布、第一间接辐射强迫及其气候效应。研究结果表明,中国地区硫酸盐气溶胶主要集中在四川、河南、山东等地,秋冬季浓度较高而夏季浓度较低。1月份浓度最高值中心在四川,最高达到50μg/m3,而7月则出现在河南等地,浓度最高达10μg/m3。1、4、7、10月硫酸盐气溶胶的第一间接辐射强迫全国平均值分别为-1.80、-2.75、-3.43、-1.83 W/m2,局部地区可达-12 W/m2。敏感性试验结果表明,硫酸盐气溶胶的第一间接效应引起气温降低,降水减少,在不同季节和地区气温和降水的变化存在明显差异。  相似文献   
77.
Serial data from soil–sawdust column experiments were used to develop a mathematical model to describe the biological sulfate reduction processes in porous media. The mathematical model numerically solves the equation of solute transport in one-dimensional saturated state. Solute transport is coupled to sulfate reducing bacteria sub model. Bacterial growth is assumed to follow double Monod kinetic equation. Two bacterial groups (X1 and X2) were described. Bacterial group X1 uses under aerobic conditions oxygen and under anaerobic conditions nitrate as electron acceptor. Under anaerobic conditions bacterial groups X2, use sulfate as an electron acceptor. Sulfate rich wastewater is usually deficient in electron donor and requires external addition of electron donors in order to achieve complete sulfate reduction. The organic carbon as electron donor is one of the most important factors that affect sulfate reduction bacterial activity. In this study the possible source of organic carbon is the solid organic carbon supplied to the system in the form of sawdust. The results of this study indicate that sawdust could be employed as low-cost materials to enhance the biological sulfate reduction processes in porous media. While the availability of organic carbon as electron donor is one of the most important factors that affect the sulfate reducing bacterial activity in porous media, this study demonstrates that using sawdust as a carbon source can improve the bacterial activity and increase the column permeability.  相似文献   
78.
Electrokinetic (EK) process was performed to restore sulfate‐originated saline soil and to evaluate the effect of treatment duration. Sulfate and potassium were the major ionic salts in the saline soil used in this study. A constant voltage gradient of 1 V/cm was applied for 8, 12, and 16 days. After EK treatment, anions and cations were transported toward anode and cathode, respectively, by electromigration. Chloride was completely removed, and 85.6% of nitrate was removed after 8 days of treatment. The increase of treatment period from 8 to 12 days had a negligible effect on the enhancement in the rate of sulfate removal; however, over 70% was removed after16 days. At the end of experiment, the electrical conductivity (EC) of the soil, an indicator of soil salinity, decreased to 1.93 dS/m from an initial value of 5.3 dS/m, and the distribution of sulfate was similar to that of EC. The operation time of 16 days was sufficient to restore the sulfate‐originated saline soil using the EK process.  相似文献   
79.
The accretionary wedge of offshore southwestern Taiwan contains abundant deposits of gas hydrate beneath the sea floor. High concentrations of methane in pore waters are observed at several locations with little data concerning historical methane venting available. To understand temporal variation of methane venting in sediments over geologic time, a 23-m-long Calypso piston core (MD05-2911) was collected on the flank of the Yung-An Ridge. Pore water sulfate, dissolved sulfide, dissolved iron, methane, sedimentary pyrite, acid volatile sulfide, reactive iron, organic carbon and nitrogen as well as carbonate δ13C were analyzed.Three zones with markedly different pyrite concentration were found at the study site. Unit I sediments (>20 mbsf) were characterized with a high amount of pyrite (251–380 μmol/g) and a δ13C-depleted carbonate, Unit II sediments (15–20 mbsf) with a low pyrite (15–43 μmol/g) and a high content of iron oxide mineral and Unit III sediments (<10 mbsf) by a present-day sulfate–methane interface (SMI) at 5 m with a high amount of pyrite (84–221 μmol/g) and a high concentration of dissolved sulfide.The oscillation records of pyrite concentrations are controlled by temporal variations of methane flux. With an abundant supply of methane to Unit I and III, anaerobic methane oxidation and associated sulfate reduction favor diagenetic conditions conducive for significant pyrite formation. No AOM signal was found in Unit II, characterized by typical organically-limited normal marine sediments with little pyrite formation. The AOM induced pyrite formation near the SMI generates a marked pyrite signature, rendering such formation of pyrite as a useful proxy in identifying methane flux oscillation in a methane flux fluctuate environment.  相似文献   
80.
为了获取锂钠钾共存硫酸盐体系298.2 K下各盐结晶形式,采用等温溶解平衡法研究了298.2 K下四元体系Li2SO4+Na2SO4+K2SO4+H2O的相平衡关系,测定了该体系的溶解度和密度,采用X-ray粉晶衍射法测定了平衡固相组成,并绘制了相应的稳定相图和多温对比图。研究表明,298.2 K下该四元体系为复杂四元体系,有复盐2Li2SO4·Na2SO4·K2SO4、Li2SO4·3Na2SO4·12H2O、LiKSO4、Na2SO4·3K2SO4生成。其稳定相图由6个四元共饱点、12条单变量曲线以及7个结晶区组成。其中,复盐Na2SO4·3K2SO4结晶区最大,表明其在该体系中最易结晶析出;Li2SO4·H2O结晶区最小。对比273.2 K、288.2 K、298.2 K、323.2 K、373.2 K四元体系多温相图可知,273.2 K时未发现复盐Na2SO4·3K2SO4和2Li2SO4·Na2SO4·K2SO4结晶形式;Na2SO4·10H2O和Li2SO4·3Na2SO4·12H2O结晶形式在323.2 K和373.2 K时转变为Na2SO4和Li2SO4·Na2SO4。288.2~373.2 K时随温度升高,K2SO4和Na2SO4·10H2O结晶相区减小,Li2SO4·H2O、Na2SO4、LiKSO4和Li2SO4·Na2SO4结晶相区增大;Na2SO4·3K2SO4结晶相区先增大后减小,在298.2 K时结晶相区最大;2Li2SO4·Na2SO4·K2SO4结晶相区先减小后增大,298.2 K时结晶相区最小。  相似文献   
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