Autoxidation of N(III), S(IV), and other Species in Frozen Solution – A Possible Pathway for Enhanced Chemical Transformation in Freezing Systems

The chemistry of glycolaldehyde (hydroxyacetaldehyde) relevant to the troposphere has been investigated using UV absorption spectrometry and FTIR absorption spectrometry in an environmental chamber. Quantitative UV absorption spectra have been obtained for the first time. The UV spectrum peaks at 277 nm with a maximum cross section of (5.5± 0.7)×10^–20 cm² molecule^–1. Studies of the ultraviolet photolysis of glycolaldehyde ( = 285 ± 25 nm) indicated that the overall quantum yield is > 0.5 in one bar of air, with the major products being CH₂OH and HCO radicals. Rate coefficients for the reactions of Cl atoms and OH radicals with glycolaldehyde have been determined to be (7.6± 1.5)×10^–11 and (1.1± 0.3)×10^–11 cm³ molecule^–1 s^–1, respectively, in good agreement with the only previous study. The lifetime of glycolaldehyde in the atmosphere is about 1.0 day for reaction with OH, and > 2.5 days for photolysis, although both wet and dry deposition should also be considered in future modeling studies.     

Behaviour of H2O2, NH3, and black carbon in mixed-phase clouds during CIME

We investigated the partitioning of trace substances during the phase transition from supercooled to mixed-phase cloud induced by artificial seeding. Simultaneous determination of the concentrations of H₂O₂, NH₃ and black carbon (BC) in both condensed and interstitial phases with high time resolution showed that the three species undergo different behaviour in the presence of a mixture of ice crystals and supercooled droplets. Both H₂O₂ and NH₃ are efficiently scavenged by growing ice crystals, whereas BC stayed predominantly in the interstitial phase. In addition, the scavenging of H₂O₂ is driven by co-condensation with water vapour onto ice crystals while NH₃ uptake into the ice phase is more efficient than co-condensation alone. The high solubility of NH₄⁺ in the ice could explain this result. Finally, it appears that the H₂O₂–SO₂ reaction is very slow in the ice phase with respect to the liquid phase. Our results are directly applicable for clouds undergoing limited riming.     

漂浮通量箱法和扩散模型法测定内陆水体CH_4和N_2O排放通量的初步比较研究

采用漂浮通量箱法和扩散模型法同步地观测了模拟内陆水体在不同条件下的CH4和N2O的水-气交换通量,旨在比较两类方法取得结果的异同。结果显示:这两类方法所测得的绝大多数CH4排放通量都与水中溶解氧呈显著线性负相关(显著性系数P0.001)。同时N2O排放通量与表层水温及水中铵态氮、硝态氮、溶解碳和溶解氧的关系可用包含所有上述水环境因素的Arrhenius动力学方程来表达,这些因素可以共同解释86%~90%的N2O通量变化(P0.0001),且不同方法测定的N2O通量的表观活化能和对表层水温的敏感系数分别介于47~59 kJ mol-1和1.92~2.27之间;扩散模型法所获得的CH4和N2O通量分别是箱法测定值的13%~175%和15%~240%,差异程度因模型而异;不同模型取得通量间相差20%~1200%,平均相差2.3倍。上述结果表明:仅用一种模型方法来取得CH4或N2O排放通量易形成较大偏差;不同扩散模型法和箱法测定的通量在反映CH4和N2O排放的内在规律方面具有一致性,但它们对真实气体通量的测量是否都存在不同程度的系统误差,尚需进一步研究。     

藻型湖区氧化亚氮排放特征及其影响因素

湖泊等内陆水体是大气N₂O潜在的重要排放源,也是全球N₂O收支估算的重要组成部分。目前全球湖泊普遍面临富营养化和蓝藻暴发等问题,明晰藻型湖泊N₂O排放强度及其环境影响因子对准确估算湖泊N₂O排放和预测其未来变化至关重要。本研究选择太湖藻型湖区为研究对象,同时选取人为活动影响较小的湖心区作为对比区域,基于2011年8月至2013年8月为期2年的逐月连续观测,探讨藻型湖区N₂O排放特征及其影响因素。结果表明,藻型湖区呈现极强的N₂O排放,其排放通量为(4.88±3.05) mmol/(m²·d),是参考区域(湖心:(2.10±4.31) mmol/(m²·d))的2倍多。此外,在藻型湖区中不同点位N₂O排放差异显著,受河流外源输入影响,近岸区是N₂O的热点排放区,其年均排放通量高达10.93 mmol/(m²·d)。连续观测表明N₂     

Adsorption of Au(III) and Au(I) complexes on δ-MnO2

The sorption of AuCl₄ ⁻,AuCl₂ ⁻ and Au(S₂O₃)^3- on δ-MnO₂ was investigated at pH2–11.6, 0.01 mol/L and 0.1 mol/L NaNO₃ solutions. At pH 4 in two electrolyte strength solutions, Au sorption densities on δ-MnO₂ are 0.18–0.21 and 0.28μmoL/m² for AuCl₄ ⁻ and Au(S₂O₃)₂ ^3-, respectively, and the Au surface coverage is approximate to or lower than 1%. This adsorption of the two Au complexes decreases as the solution pH increases, which conforms to the sorption regularity of the anion on δ-MnO₂. The Au sorption decreases in the sequence of Au(S₂O₃)₂ ^3- >AuCl₄ ⁻ >AuC1₂ ⁻. The intrinsic equilibrium constants (logK ^int) of the three Au complexes are 1.17–2.7, much higher than those of Cu and Cd. The hydrolysis products of AuCl₄ ^- are preferentially adsorbed by δ-MnO₂ and the inner-sphere Au-surface complexes are formed on the surface. Project supported by the National Studying-abroad Foundation, the National Natural Science Foundation of China (Grant No. 49573200) and the Australian Mining Industry.     

Application of diffracted wave analysis to time‐lapse seismic data for CO2 leakage detection

Time‐lapse seismic analysis is utilized in CO₂ geosequestration to verify the CO₂ containment within a reservoir. A major risk associated with geosequestration is a possible leakage of CO₂ from the storage formation into overlaying formations. To mitigate this risk, the deployment of carbon capture and storage projects requires fast and reliable detection of relatively small volumes of CO₂ outside the storage formation. To do this, it is necessary to predict typical seepage scenarios and improve subsurface seepage detection methods. In this work we present a technique for CO₂ monitoring based on the detection of diffracted waves in time‐lapse seismic data. In the case of CO₂ seepage, the migrating plume might form small secondary accumulations that would produce diffracted, rather than reflected waves. From time‐lapse data analysis, we are able to separate the diffracted waves from the predominant reflections in order to image the small CO₂ plumes. To explore possibilities to detect relatively small amounts of CO₂, we performed synthetic time‐lapse seismic modelling based on the Cooperative Research Centre for Greenhouse Gas Technologies (CO2CRC) Otway project data. The detection method is based on defining the CO₂ location by measuring the coherency of the signal along diffraction offset‐traveltime curves. The technique is applied to a time‐lapse stacked section using a stacking velocity to construct offset‐traveltime curves. Given the amount of noise found in the surface seismic data, the predicted minimum detectable amount of CO₂ is 1000–2000 tonnes. This method was also applied to real data obtained from a time‐lapse seismic physical model. The use of diffractions rather than reflections for monitoring small amounts of CO₂ can enhance the capability of subsurface monitoring in CO₂ geosequestration projects.     

基于SVD和BRD的二维核磁共振测井正则化反演算法研究

二维核磁共振能从"弛豫-扩散"两个维度上展现流体性质,在识别稠油储层方面具有理论优势,是当前核磁共振测井技术的研究热点.本文深入研究二维核磁共振测井原理,系统分析CPMG-DE脉冲序列测量扩散系数与弛豫时间的方法,结合核磁共振二维谱数理模型,提出一种基于SVD和BRD的正则化反演算法.该算法通过SVD压缩数据,采用带非负约束的Tikhonov正则化方法求解流体"弛豫-扩散"分布,并基于BRD算法迭代确定最佳正则化因子.模拟实验与数值分析表明,该算法无需先验信息、运算效率高、相对误差小,在原始数据信噪比低至50时,仍可有效获取流体(T2,D)二维分布.在二维核磁共振测井数据实时解释应用中,该方法较传统反演算法(如TSVD)具有较大优势.同时,在自主研发的核磁共振测井仪测量CuSO4溶液(T2,D)分布的实验显示,本文设计算法对弛豫时间和扩散系数的反演误差分别仅为2%和4%,较TSVD算法有较大改善.     

风云二号F星太阳X射线探测器在轨探测初步成果

风云二号系列卫星以自旋稳定方式工作于地球静止轨道,太阳X射线探测器是该系列卫星的重要有效载荷,监测太阳耀斑爆发过程,并对太阳质子事件等灾害性的空间天气事件进行预警.卫星自旋一周,该探测器完成一次全日面观测,记录太阳X射线的能谱与流量.2012年初,太阳活动进入第24周峰年,风云二号卫星太阳X射线探测器的在轨运行取得了良好的观测结果.相比于过去的太阳X射线探测器,风云二号F星的太阳X射线探测器应用了硅漂移探测(Silicon Drift Detector,SDD)技术,对GEO轨道海量的高能带电粒子采取了有效的屏蔽措施,可以对更"软"的X射线进行观测,能谱分辨率本领达到国际先进水平,对太阳耀斑的量化定级精度更高,在轨初步观测结果表明,精确的能谱探测能力可提高太阳质子事件预警能力,能道响应的时间特性比过去的探测数据更准确地反映了太阳耀斑的加热过程和带电粒子加速特性.本文介绍了风云二号F星太阳X射线探测器的设计及其发射前的标定试验结果,并且对发射后在轨运行获得的初步探测成果进行分析和讨论.     

Delineation of the northern limit of the Congo Craton based on spectral analysis and 2.5D modeling of aeromagnetic data in the Akonolinga-Mbama area,Cameroon

Aeromagnetic data of the Akonolinga-Mbama region are analyzed in order to elucidate the subsurface geology of the area. The available data in the form of a residual aeromagnetic map is interpreted as a vast magnetically quiet region, and complex zones which do not correlate with the surface geology of the region.Within the magnetically quiet zone, a high negative circular elongated anomaly zone seems to represent an intrusion of a plutonic rock into the metamorphic formations of the region. Spectral analysis and two-and-a-half dimensional (2½-D) modeling are used to estimate the depth of the causative bodies and determine the source rocks along three profiles crossing the suspected areas. Models from various zones of granitic intrusions are obtained, thereby proposing some shallow fault lines along zones of contact. This permits us to mark out the northern margin of the Congo Craton, thus enabling us to distinguish the cratonic formations from the Pan African fold belt. Part of the belt has been thrust over the northern portion of the Congo Craton in Cameroon.     

The oxygen minimum zone (OMZ) off Chile as intense source of CO2 and N2O

The oxygen minimum zones (OMZs) are recognized as intense sources of N₂O greenhouse gas (GHG) and could also be potential sources of CO₂, the most important GHG for the present climate change. This study evaluates, for one of the most intense and shallow OMZ, the Chilean East South Pacific OMZ, the simultaneous N₂O and CO₂ fluxes at the air–sea interface. Four cruises (2000–2002) and 1 year of monitoring (21°–30°–36°S) off Chile allowed the determination of the CO₂ and N₂O concentrations at the sea surface and the analysis of fluxes variations associated with different OMZ configurations. The Chilean OMZ area can be an intense GHG oceanic local source of both N₂O and CO₂. The mean N₂O fluxes are 5–10 times higher than the maximal previous historical source in an OMZ open area as in the Pacific and Indian Oceans. For CO₂, the mean fluxes are also positive and correspond to very high oceanic sources. Even if different coupling and decoupling between N₂O and CO₂ are observed along the Chilean OMZ, 65% of the situations represent high CO₂ and/or N₂O sources. The high GHG sources are associated with coastal upwelling transport of OMZ waters rich in N₂O and probably also in CO₂, located at a shallow depth. The integrated OMZ role on GHG should be better considered to improve our understanding of the past and future atmospheric CO₂ and N₂O evolutions.