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1.
PM2.5是近年来影响我国城市大气环境的首要污染物,其成因机制复杂。本文采用扫描电镜和ICP-MS研究了广州市大气颗粒物PM2.5的显微形貌及其化学组成特征,并应用富集因子法进行源解析。结果表明,PM2.5的颗粒形态以无定形态为主;主要物质表现为含Fe、Mg、Al、K、Na的硅酸盐组合,具有道路扬尘、建筑施工排放等一次粒子特征;单个无定形颗粒物能谱表现出硫酸盐+硝酸盐的组合特征,为汽车尾气所排放的前体污染气体NOx和SO2进入大气环境中,在特定的物理化学条件下通过成核作用发生相态改变所形成的二次粒子。PM2.5中高度富集Cd、Se、Zn、Cu、Pb、As等重金属,异常富集的Br主要为当地普遍使用的阻燃剂十溴联苯醚和拆解电子垃圾所致,稀土元素的浓度在0.022~0.582 ng/m3之间,具有重稀土元素富集的特征。这些特征反映出广州市PM2.5颗粒物的组成既有一次粒子,也有二次粒子,物质来源具有多重性。 相似文献
2.
为了研究祁连山大雪山地区大气PM2.5细粒子中可溶性无机离子组分的变化特征, 于2010年7月至2011年7月在祁连山冰川与生态环境综合观测站附近采集46个大气PM2.5的Telfon滤膜样品, 并应用离子色谱对可溶性离子进行了分析.结果显示: 所测样品的阴、 阳离子中, SO42-、 NO-3、 Ca2+和NH+4的质量浓度分别为1.54μg·m-3、 0.38μg·m-3、 0.73μg·m-3和0.22μg·m-3, 累计约占到水溶性离子总量的88%.可溶性离子浓度呈现出春夏季节明显高于秋冬季节的特征, 夏季的浓度最高, 其次是春季、 冬季和秋季. Cl-、 Ca2+、 Na+和Mg2+之间的相关性极高, SO42-和NO-3与大部分阳离子的相关性都很高, 说明大部分硫酸盐是来自于中亚沙尘源区的自然源, 而并非是通过人类活动造成的一次污染物通过二次反应过程得到的. NH+4仅与SO42-通过相关性检验说明, 该地区NH3主要中和了大气中硫酸并生成(NH4)2SO4.该地区的大气环境主要来源于自然源的影响, 但夏季风期间人为污染排放已经不可忽视, 这也得到HYSPLIT后向轨迹模式的计算验证. 相似文献
3.
本次研究选择中国东部一个生态和环境空间分异极大的浅水湖泊（太湖）以及周围河流,分别于2003年7月和9月两次采集湖水和河水样品,分析其中的N2O浓度,并利用扩散模型公式估算水-气界面N2O交换通量。结果显示N2O饱和度的空间变化从70％不饱和到2708％过饱和变化范围很大。N2O饱和度的空间分布,N2O与CH4、无机氮、TDS（总溶解固体物质）之间的相关性都表明： 太湖重度富营养区N2O的产生极大地受到人为N输入的影响。然而,初步的通量分析显示湖泊N2O的释放因子不超过0.63％,小于河流中的默认值,N2O产率也略低于水环境中的平均值,太湖以面积为权重的释放通量平均值并不高,在7月和9月分别为14.0μmol/m2·d和9.7μmol/m2·d。这些结果表明流域人为N输入对整个湖泊N2O的促进作用是有限的,预计未来湖泊N2O释放不会因为人为活动增加而出现大幅度增加的状况。流域内各生态景观N2O释放量的比较,也表明富营养湖泊总体上仍然是一个十分有限的大气N2O释放源。相反,太湖周围河流存在较大的N2O释放速率,在7月和9月估算的N2O释放通量分别为142.1μmol/m2·d和28.8μmol/m2·d。将这一释放速率推广到整个流域后,预计河网的N2O释放量将占到耕作土壤的10％～50％,显示了河流对区域N2O质量平衡具有较重要的影响。 相似文献
4.
测定了新疆罗布泊地区湖相沉积物CK-2钻孔样品的总有机碳含量（TOC）及其同位素组成、碳酸盐含量和C/N比值等环境代用指标,以及石膏矿物的质谱-铀系年龄。测试结果表明,20～9kaB.P.期间沉积物δ13Corg.在-23.4‰～-16.1‰之间波动且阶段性明显,与TOC呈现良好的相关关系,整体变化趋势同南极Dome C冰芯中记录的全球大气CO2浓度一致;C/N比值表明有机碳来源主要是陆生高等植物。因此大气CO2浓度变化是影响20～9kaB.P.期间罗布泊湖相沉积物δ13Corg.值变化的主导因素,周围山体上C3/C4植物相对生物量的变化则是另一重要因素。依据δ13Corg.的变化序列将此时间段湖区古环境的演化分成6个阶段:20.0～14.1kaB.P.期间受到末次盛冰期的影响,气温偏低,湖水丰沛;14.1～13.3kaB.P.是一个气候不稳定期,冷暖波动较频繁,但以暖为趋势;13.3～12.8kaB.P.期间经历了一段冷期,于12.8kaB.P.结束了末次冰期,随后气候开始转暖至11.8kaB.P.;其后气温再次变冷并维持到10kaB.P.;最后从10kaB.P.进入全新世暖期。δ13Corg.序列明显向偏负方向变化,表明该地区变暖的趋势相当明显。罗布泊地区日益干旱化是全球气候变化的结果,尤其是受到全球CO2浓度的不断升高所制约。 相似文献
5.
临安一次沙尘暴过程影响气溶胶物理化学特性演变的初步分析 总被引：16，自引：4，他引：12
文章利用2002年3月29日～4月4日在浙江临安大气本底污染监测站观测的气溶胶粒子质量谱、离子与元素成分的数据,结合TOMS卫星的气溶胶指数资料和轨迹模式,重点分析在北方沙尘暴输送影响期间临安气溶胶质量浓度尺度分布的演变特点以及气溶胶化学成分与不同空气来源的关系。初步分析结果显示,受北方沙尘暴天气影响,临安气溶胶质量浓度、离子、元素浓度有明显的尺度分布演变。这种演变与污染物来源和大气污染物的气粒转化有关。沙尘影响前和结束后临安地区气溶胶主要以细粒子为主(<2.1μm),峰值粒径0.65～2.1μm,而受北方地区的沙尘暴影响,峰值粒径偏移到2.1～3.3μm,且在7～11μm间出现另一个峰值,同时临安气溶胶粗粒子中矿物元素显著增加。从离子成分看,在整个观测期间SO2-4与NH+4在细粒子段有很好的一致性,而SO2-4,NO-3与Ca2+在粗粒子段有很好的相关,尤其是沙尘影响期间NO-3与Ca2+有很好的对应关系,表现出较明显的表面非均相反应特征 相似文献
6.
对采自浙江西天目山地区的3株柳杉树盘,交叉定年后,测定了3株树轮δ13C的年序列,分析了3株树轮δ13C序列中所含的共同环境变化信息。用二项式拟合法去除气候因素引起的3个δ13C序列的高频变化,得到3个低频变化序列。分析了theLowDome冰芯记录的大气CO2浓度与树轮δ13C序列低频变化趋势的关系,建立了相应的转移函数,重建了天目山地区1685年以来大气CO2浓度变化。结果表明:用3株树轮δ13C序列重建的结果有较好的一致性,并与南极冰芯的记录及前人研究结果有很好的吻合。这一结果表明用同一地区不同树木个体的树轮δ13C序列的低频变化序列可以重建出基本一致的大气CO2浓度变化历史。 相似文献
7.
采集煤矿区城市义马、平顶山、永城夏季大气PM10样品,采用带能谱的扫描电镜(SEM-EDX)研究了PM10中的矿物颗粒组成、成因及来源。结果表明,矿区矿物颗粒按化学成分共有5种主要类型,分别为"富Si"、"富Ca"、"富S"、"富K"、"富Cl"型。其中平顶山地区"富Si"颗粒占百分比最高(78%),矿物颗粒硫酸盐化程度小;永城地区硫酸盐化程度中等,几乎所有的"富Ca"碱性碳酸盐颗粒都硫酸盐化成石膏;义马地区矿物硫酸盐化程度最大,除石膏以外,还有一定量硫酸铵形成。永城和义马地区还出现了一定量的"富K"(12.7%)和"富Cl"(10.6%)颗粒,与秸秆焚烧活动有关。通过对3个矿区城市PM10硫酸盐化程度对比可以发现,偏碱性的碳酸盐矿物、煤炭燃烧和秸秆焚烧燃烧释放出大量的酸性SO2以及较高的空气湿度,均有利于硫酸盐化的进行,硫酸盐颗粒的形成对煤矿区城市的区域性气候具有一定影响。 相似文献
8.
文章通过2002年8月12~27日和2003年7月20日~8月1日在浙江临安县的WMO区域空气污染本底站临安站所采集的气溶胶样品的质量浓度,水溶性离子,有机碳/元素碳(OC/EC)及部分化学元素的特征分析,并与1991年夏季(8月22~28日)气溶胶的某些特征比较,初步研究结果为:1991年至2003年夏季的气溶胶TSP,PM11和PM2.1浓度均呈现出减少的趋势,但是PM11/TSP和PM2.1/PM11则有增加的趋势。1991年、2002年和2003年PM11/TSP的值为90 % 左右,PM2.1/PM11 分别为46.52 % , 69.33 % 和72.29 % ,说明气溶胶以小粒子为主,小粒子又以细粒子为主。1991年、2002年和2003年浓度最高的离子为SO2-4,其次为NH＋4。其中SO2-4占所测离子浓度的百分数分别为65.39 % ,57.75 % 和57.27 % ,并且主要以(NH4)2SO4,(K)2SO4和(Na)2SO4的形式存在。各离子浓度占所测离子浓度的百分数基本上不随年代变化,具有一定稳定性。2002年和2003年气溶胶中的OC浓度分别为29.91μg/m3和14.14μg/m3,均为各自的组分之首。2002年和2003年OC的比值PM2.1/PM11分别为64.63 % 和77.71 % ,EC的比值PM2.1/PM11分别为69.89 % 和87.17 % ,可见气溶胶中OC和EC主要存在于PM2.1的粒子中。元素富集因子分析表明,自然源与人为源对气溶胶中的元素都有重要的贡献。主因子分析结果显示PM2.1和PM11元素源基本相同,自然源主要是地壳、土壤尘和海盐, 人为源主要是煤飞灰(煤和焦碳)、冶炼工业和道路机动车辆的排放、废物处理、垃圾焚烧及建筑工业粉尘等。 相似文献
9.
川南普格杏仁状玄武岩气孔中产出硅铁灰石、绿泥石、石英、方解石、沥青等5种不同成分类型的杏仁体。硅铁灰石杏仁体呈圆形或椭圆形,其直径多为5～8 mm,由杏仁体壁至中心,依次分别产出石英→铁镁绿泥石→硅铁灰石。硅铁灰石晶体呈铁黑色、薄板状,由5个平行双面单形组成。微区X射线衍射分析结果显示,硅铁灰石属三斜晶系,空间群为P1 。化学成分分析表明,硅铁灰石氧化物含量(ωB/%)为SiO2 53.55%、CaO 18.84%、Fe2O3 13.65%、FeO 9.68%、MgO 1.44%、H2O+1.74%,FeO/Fe2O3=0.71;铁镁绿泥石氧化物含量(ωB/%)为SiO2 33.17%、Al2O3 13.03%、Fe2O3 8.45%、FeO 13.06%、MgO 18.82%、H2O+12.12%、CaO 0.87%,FeO/Fe2O3=1.55。硅铁灰石杏仁体的矿物组合变化表明,玄武岩晚期的成矿热液由富Mg、Fe向富Si、Ca演化,硅铁灰石是由偏酸性、弱还原环境向偏碱性、弱氧化环境转化时所形成的过渡性产物。 相似文献
10.
江浪穹窿位于扬子陆块西缘,本文作者在穹窿南部新发现一套侵入于二叠系及志留系的超基性岩,岩石主要由蛇纹石(约60%)、橄榄石(约30%)和少量磁铁矿(约5%)、角闪石(约5%)组成。为探讨超基性岩的成因,本文进行了LA-ICP-MS锆石U-Pb定年、岩石地球化学及Sr-Nd同位素研究。定年结果表明,超基性岩中发育大量2427~430 Ma的捕获锆石,最年轻一组岩浆锆石206Pb/238U加权平均年龄为222.3±4.4 Ma(MSWD=1.9,n=6)。主微量元素分析显示岩石：(1)具有低的SiO2含量(46.76%~39.07%)、高的Mg#值(82.3~74.0)与Cr、Co、Ni丰度;(2)稀土元素含量(ΣREE平均31.8 μg/g)与(La/Yb)N值(5.26~1.38)偏低,稀土配分型式较为平坦,具有较弱的Ce负异常(Ce/Ce*=0.80~0.67);(3)富集大离子亲石元素Rb、Ba和U,亏损高场强元素Zr和Hf;(4)(Th/Yb)PM值(29.8~1.56)、(Th/Ta)PM值(0.22~0.03)、(La/Nb)PM值(1.91~0.39)及La/Sm值(5.88~1.11)较低。Sr-Nd同位素分析显示,超基性岩具有较低的(87Sr/86Sr)i值(0.706872~0.702598)和高的εNd(t)值(8.02~5.64),成分接近于亏损地幔和岛弧玄武岩,计算表明地壳物质的混染程度低于5%。结合前人研究成果,本文认为超基性岩结晶年龄为222.3 Ma,可能形成于古特提斯洋闭合阶段的岛弧背景;原始岩浆来自高度部分熔融的地幔源区,上升侵位过程中可能经历了铬铁矿与橄榄石的分离结晶作用。此外,捕获锆石的年龄谱反映江浪穹窿很可能存在太古宙—古元古代变质基底,并且具有Rodinia超大陆会聚—裂解以及泛非事件的地质年龄记录。 相似文献
11.
Elastic and thermoelastic constants of large single crystals of Ca2MgSi2O7 and Ca2ZnSi2O7 have been derived from ultrasonic resonance frequencies of plane-parallel plates and their shift upon variation of temperature, respectively. In addition, coefficients of thermal expansion and dielectric constants were determined. Both species possess quite similar properties. As observed in other isotypic magnesium and zinc compounds, the mean elastic stiffness and the deviation from the Cauchy relations are significantly larger in the zinc compound, due to a covalent contribution of the Zn–O bond. Positive thermoelastic constants T44 and T66 in Ca2MgSi2O7 allow temperature-independent ultrasonic generators and oscillators to be manufactured. 相似文献
12.
含Ti硅酸盐玻璃在基础科学研究和应用技术开发上均有重要价值,亟需对其进行准确的成分分析,为进一步的科研工作提供重要的数据支撑.对玻璃进行电子探针分析时,由于样品的易损性和其中(Na和K)阳离子在电子束轰击下极易发生迁移和扩散,因此往往需要经过条件实验来确定合适的分析条件,确保样品在该条件下能够保持尽量稳定的状态,才能获... 相似文献
13.
Hydrometallurgical processing and recovery of molybdenum trioxide from spent catalyst 总被引：5，自引：0，他引：5
Kyung Ho Park B. Ramachandra Reddy D. Mohapatra Chul-Woo Nam 《International Journal of Mineral Processing》2006,80(2-4):261-265
Hydrometallurgical processing of spent hydrodesulphurisation (HDS) catalyst for the recovery of molybdenum using sodium carbonate and hydrogen peroxide mixtures was investigated. The results indicated that the recovery of molybdenum was largely dependent on the concentrations of Na2CO3 and H2O2 in the reaction medium, which controls the acidity of the leach liquor and carry over of impurities such as Al, Ni, P, Si and V. Leaching process was exothermic and leaching efficiency of molybdenum decreased with increasing solid to liquid ratio. Large scale leaching of spent catalyst, under optimum conditions: 20% pulp density, 85 g/L Na2CO3, 10 vol.% H2O2 and 1 h reaction, resulted a leaching efficiency of 84% Mo. The obtained leach liquor contained (g/L): Mo — 22.0, Ni — 0.015 and Al — 0.82, P — 1.1, Si — 0.094 and minor quantities of V — 8 mg/L, As and Co — < 1 mg/L. Recovery of Mo from leach solution as MoO3 of 97.30% purity was achieved by ammonium molybdate precipitation method. 相似文献
14.
Classical atomistic simulation techniques have been used to investigate the energies of hydrogen defects in Mg2SiO4 and Mg2GeO4 spinels. Ringwoodite (γ-Mg2SiO4) is considered to be the most abundant mineral in the lower part of the transition zone and can incorporate large amounts
of water in the form of hydroxyls, whereas the germanate spinel (γ-Mg2GeO4) corresponds to a low-pressure structural analogue for ringwoodite. The calculated defect energies indicate that the most
favourable mechanisms for hydrogen incorporation are coupled either with the reduction of ferric iron or with the creation
of tetrahedral vacancies. Hydrogen will go preferentially into tetrahedral vacancies, eventually leading to the formation
of the hydrogarnet defect, before associating with other negatively charged point defects. The presence of isolated hydroxyls
is not expected. The same trend is observed for germanate, and thus γ-Mg2GeO4 could be used as a low-pressure analogue for ringwoodite in studies of water-related defects and their effect on physical
properties. 相似文献
16.
Gianluca Iezzi Mario Tribaudino Giancarlo Della Ventura Fabrizio Nestola Fabio Bellatreccia 《Physics and Chemistry of Minerals》2005,32(7):515-523
The synthetic amphibole Na0.95(Li0.95Mg1.05)Mg5Si8O22(OH)2 was studied in situ at high-T, using IR OH-stretching spectroscopy and synchrotron X-ray powder diffraction. At room-T the sample has P21
/m symmetry, as shown by the FTIR spectrum. It shows in the OH region two well-defined and intense absorptions at 3,748 and
3,712 cm−1, respectively, and two minor bands at 3,667 and 3,687 cm−1. The main bands are assigned to the two independent O–H groups in the primitive structure. The two minor bands evidencing
the presence of small amount of vacant A-site (A□0.05). With increasing T, these bands shift continuously and merge into a unique absorption at high temperature. A change as a function of increasing
T is revealed by the evolution of the refined unit-cell parameters, whose trend shows a transition to C2/m at about 320–330°C. The spontaneous scalar strain, fitted with a tricritical 2–6 Landau potential, gives a T
c of 325(10)°C (β parameter = 0.27). Comparison with the second-order P21
/m ⇔ C2/m phase transition at 255°C for synthetic amphibole ANa0.8B(Na0.8Mg1.2)CMg5Si8O22(OH)2 indicates that the substitution of Na with Li at the B-sites strongly affects the thermodynamic character and the T
c of the phase transition. The comparison of LNMSH amphiboles with cummingtonitic ones shows that the high-T thermodynamic behaviour is affected by A-site occupancy. 相似文献
17.
We present results from low-temperature heat capacity measurements of spinels along the solid solution between MgAl2O4 and MgCr2O4. The data also include new low-temperature heat capacity measurements for MgAl2O4 spinel. Heat capacities were measured between 1.5 and 300 K, and thermochemical functions were derived from the results.
No heat capacity anomaly was observed for MgAl2O4 spinel; however, we observe a low-temperature heat capacity anomaly for Cr-bearing spinels at temperatures below 15 K. From
our data we calculate standard entropies (298.15 K) for Mg(Cr,Al)2O4 spinels. We suggest a standard entropy for MgAl2O4 of 80.9 ± 0.6 J mol−1 K−1. For the solid solution between MgAl2O4 and MgCr2O4, we observe a linear increase of the standard entropies from 80.9 J mol−1 K−1 for MgAl2O4 to 118.3 J mol−1 K−1 for MgCr2O4. 相似文献
18.
The influence on the structure of Fe2+ Mg substitution was studied in synthetic single crystals belonging to the MgCr2O4–FeCr2O4 series produced by flux growth at 900–1200 °C in controlled atmosphere. Samples were analyzed by single-crystal X-ray diffraction, electron microprobe analyses, optical absorption-, infrared- and Mössbauer spectroscopy. The Mössbauer data show that iron occurs almost exclusively as IVFe2+. Only minor Fe3+ (<0.005 apfu) was observed in samples with very low total Fe. Optical absorption spectra show that chromium with few exceptions is present as a trivalent cation at the octahedral site. Additional absorption bands attributable to Cr2+ and Cr3+ at the tetrahedral site are evident in spectra of end-member magnesiochromite and solid-solution crystals with low ferrous contents. Structural parameters a0, u and T–O increase with chromite content, while the M–O bond distance remains nearly constant, with an average value equal to 1.995(1) Å corresponding to the Cr3+ octahedral bond distance. The ideal trend between cell parameter, T–O bond length and Fe2+ content (apfu) is described by the following linear relations: a0=8.3325(5) + 0.0443(8)Fe2+ (Å) and T–O=1.9645(6) + 0.033(1)Fe2+ (Å) Consequently, Fe2+ and Mg tetrahedral bond lengths are equal to 1.998(1) Å and 1.965(1) Å, respectively. 相似文献
19.
The high-pressure behavior of a vanadinite (Pb10(VO4)6Cl2, a = b = 10.3254(5), c = 7.3450(4) Å, space group P63/m), a natural microporous mineral, has been investigated using in-situ HP-synchrotron X-ray powder diffraction up to 7.67 GPa with a diamond anvil cell under hydrostatic conditions. No phase transition has been observed within the pressure range investigated. Axial and volume isothermal Equations of State (EoS) of vanadinite were determined. Fitting the P–V data with a third-order Birch-Murnaghan (BM) EoS, using the data weighted by the uncertainties in P and V, we obtained: V 0 = 681(1) Å3, K 0 = 41(5) GPa, and K′ = 12.5(2.5). The evolution of the lattice constants with P shows a strong anisotropic compression pattern. The axial bulk moduli were calculated with a third-order “linearized” BM-EoS. The EoS parameters are: a 0 = 10.3302(2) Å, K 0(a) = 35(2) GPa and K′(a) = 10(1) for the a-axis; c 0 = 7.3520(3) Å, K 0(c) = 98(4) GPa, and K′(c) = 9(2) for the c-axis (K 0(a):K 0(c) = 1:2.80). Axial and volume Eulerian-finite strain (fe) at different normalized stress (Fe) were calculated. The weighted linear regression through the data points yields the following intercept values: Fe a (0) = 35(2) GPa for the a-axis, Fe c (0) = 98(4) GPa for the c-axis and Fe V (0) = 45(2) GPa for the unit-cell volume. The slope of the regression lines gives rise to K′ values of 10(1) for the a-axis, 9(2) for the c-axis and 11(1) for the unit cell-volume. A comparison between the HP-elastic response of vanadinite and the iso-structural apatite is carried out. The possible reasons of the elastic anisotropy are discussed. 相似文献
20.
Mathematical models of hydrocarbon formation can be used to simulate the natural evolution of different types of organic matter and to make an overall calculation of the amounts of oil and/or gas produced during this evolution. However, such models do not provide any information on the composition of the hydrocarbons formed or on how they evolve during catagenesis.From the kinetic standpoint, the composition of the hydrocarbons formed can be considered to result from the effect of “primary cracking” reactions having a direct effect on kerogen during its evolution as well as from the effect of “secondary cracking” acting on the hydrocarbons formed.This report gives experimental results concerning the “primary cracking” of Types II and III kerogens and their modelling. For this, the hydrocarbons produced have been grouped into four classes (C1, C2–C5, C6–C15 and C15+). Experimental data corresponding to these different classes were obtained by the pyrolysis of kerogens with temperature programming of 4°C/min with continuous analysis, during heating, of the amount of hydrocarbons corresponding to each of these classes.The kinetic parameters of the model were optimized on the basis of the results obtained. This model represents the first step in the creation of a more sophisticated mathematical model to be capable of simulating the formation of different hydrocarbon classes during the thermal history of sediments. The second step being the adjustment of the kinetic parameters of “secondary cracking”. 相似文献