The Soret effect and isotopic fractionation in high-temperature silicate melts

Diffusion in condensed phases is a ubiquitous but poorly understood phenomenon. For example, chemical diffusion, which is the transport of matter associated with chemical concentration gradients (Fick's law), is treated as a separate process from thermal transport (the Soret effect), which is mass transport induced by temperature gradients. In the past few years, large variations in the proportions of isotopes of Mg, Ca, Fe, Si and O found in silicate melts subject to thermal gradients have been found, but no physical mechanism has been proposed. Here we present a model of diffusion in natural condensed systems that explains both the chemical and isotopic fractionation of Mg, Ca and Fe in high-temperature geochemical melts. Despite the high temperatures associated with these melts (T>1,000 °C), we find that consideration of the quantum-mechanical zero-point energy of diffusing species is essential for understanding diffusion at the isotopic level. Our model explains thermal and chemical mass transport as manifestations of the same underlying diffusion mechanism. This work promises to provide insights into mass-transport phenomena (diffusion and evaporation) and associated isotopic fractionations in a wide range of natural condensed systems, including the atmospheric water cycle, geological and geochemical systems and the early Solar System. This work might also be relevant to studies of mass transport in biological and nanotechnological condensed systems.     

Aluminium control of argon solubility in silicate melts under pressure

Understanding of the crystal chemistry of the Earth's deep mantle has evolved rapidly recently with the gradual acceptance of the importance of the effect of minor elements such as aluminium on the properties of major phases such as perovskite. In the early Earth, during its formation and segregation into rocky mantle and iron-rich core, it is likely that silicate liquids played a large part in the transport of volatiles to or from the deep interior. The importance of aluminium on solubility mechanisms at high pressure has so far received little attention, even though aluminium has long been recognized as exerting strong control on liquid structures at ambient conditions. Here we present constraints on the solubility of argon in aluminosilicate melt compositions up to 25 GPa and 3,000 K, using a laser-heated diamond-anvil cell. The argon contents reach a maximum that persists to pressures as high as 17 GPa (up to 500 km deep in an early magma ocean), well above that expected on the basis of Al-free melt experiments. A distinct drop in argon solubility observed over a narrow pressure range correlates well with the expected void loss in the melt structure predicted by recent molecular dynamics simulations. These results provide a process for noble gas sequestration in the mantle at various depths in a cooling magma ocean. The concept of shallow partial melting as a unique process for extracting noble gases from the early Earth, thereby defining the initial atmospheric abundance, may therefore be oversimplified.     

基于热分级法的双向拉伸聚丙烯专用料制样条件的优化

采用连续自成核退火法(SSA)热分级方法对双向拉伸聚丙烯专用料的分子链结构进行研究.设计用连续自成核退火热分级方法评价双向拉伸聚丙烯成模稳定性的实验方法,通过对双向拉伸聚丙烯专用料的制样过程进行分析,确定最适宜的制样条件.结果表明:最适宜的制样条件为样品在200℃条件下用压板压制,可以消除不同产地铝坩埚的影响,成模稳定性显著提高.     

AZ91镁合金热扩渗涂层的研究

采用固体粉末法对AZ91镁合金实施了渗Al、Al-Ce共渗．通过扫描电子显微镜、X射线衍射、能谱和腐蚀测量系统对渗层组织进行了分析．结果表明，该方法能使镁合金表面得到良好的渗层组织，有一定的工程意义．经检验渗Al、Al-Ce渗层均能提高镁合金的耐腐蚀性能，渗Al-ce的耐蚀性更是明显高于渗纯铝．     

碳、氮同位素示踪法在农林业中的应用

对碳、氮同位素示踪法在相关的农林业研究中应用的基本原理、应用途径和方法及其研究进展进行了概括和总结。碳同位素主要应用于土壤碳循环、光合作用及其同化产物的传导和分布、植物水分利用效率、土地利用变化、农药残留代谢、降解和代谢等领域;氮同位素主要应用于农林N2O释放机理、固氮植物固氮量能力的分析以及氮素转化、氮肥利用率等方面的研究,为进一步在农林业及相关领域的应用提供参考。     

Diatom carbon export enhanced by silicate upwelling in the northeast Atlantic

Diatoms are unicellular or chain-forming phytoplankton that use silicon (Si) in cell wall construction. Their survival during periods of apparent nutrient exhaustion enhances carbon sequestration in frontal regions of the northern North Atlantic. These regions may therefore have a more important role in the 'biological pump' than they have previously been attributed, but how this is achieved is unknown. Diatom growth depends on silicate availability, in addition to nitrate and phosphate, but northern Atlantic waters are richer in nitrate than silicate. Following the spring stratification, diatoms are the first phytoplankton to bloom. Once silicate is exhausted, diatom blooms subside in a major export event. Here we show that, with nitrate still available for new production, the diatom bloom is prolonged where there is a periodic supply of new silicate: specifically, diatoms thrive by 'mining' deep-water silicate brought to the surface by an unstable ocean front. The mechanism we present here is not limited to silicate fertilization; similar mechanisms could support nitrate-, phosphate- or iron-limited frontal regions in oceans elsewhere.     

Interstellar extinction by graphite, iron and silicate grains

Recent data on the interstellar extinction curve and on the diffuse galactic light may be accounted for by a mixture of graphite, iron and silicate grains.     

聚丙烯酰胺改性聚硅硫酸铁絮凝剂结构表征及絮凝性能

以无机高分子絮凝剂聚硅硫酸铁(PFSS)和非离子聚丙烯酰胺(NPAM)为原料,采用不同的配比,制备出复合絮凝剂PFSS-PAM.进行pH值、zeta电位、电导、硅铁聚合态含量、红外谱图表征和絮凝性能实验,确定絮凝效果最佳的PFSS与PAM的配比.结果表明:V(PFSS)∶V(PAM) =0.2的PFSS-PAM的稳定时间为5d,n(Si)∶n(Fe)=1,V(PFSS)∶V(PAM) =0.5时,投加量为0.4～1.2 mg/L,PFSS-PAM处理制药废水的去浊率可达99.1％,COD去除率可达26.6％.     

水玻璃固化黏土矿物的试验研究

采用扫描电镜(SEM)、X线衍射(XRD)和X线光电子能谱(XPS),对常温下不同密度水玻璃固化的蒙脱石、伊利石和高岭石试样进行测试与分析.结果表明:黏土矿物由固化前的粒状、片状结构转变为固化后的团块状的网状结构.黏土矿物固化样中出现明显的非晶态弥散峰群,未出现新的晶体;固化样衍射强度变小、晶层间距变小、颗粒变得更细小,结晶构造有序性变差,但晶体主体依然是黏土矿物的晶体.固化样中,仅1.15 g/cm3水玻璃固化的蒙脱石样的Ca-2p电子结合能减少了0.624 6 eV,其余元素的相应值未变化.水玻璃固化黏土矿物的机理是:硅酸盐离子和硅酸胶粒在黏土矿物表面如蒙脱石的晶层平面与端面存在复杂的吸附作用,形成了团粒,具有很大表面能的团粒进一步失水缩聚,形成非晶质硅酸盐凝胶和晶质黏土矿物共存的网状结构产物,限制了黏土矿物的活性,固化了黏土矿物.     

An interconnected network of core-forming melts produced by shear deformation

The formation mechanism of terrestrial planetary cores is still poorly understood, and has been the subject of numerous experimental studies. Several mechanisms have been proposed by which metal--mainly iron with some nickel--could have been extracted from a silicate mantle to form the core. Most recent models involve gravitational sinking of molten metal or metal sulphide through a partially or fully molten mantle that is often referred to as a 'magma ocean'. Alternative models invoke percolation of molten metal along an interconnected network (that is, porous flow) through a solid silicate matrix. But experimental studies performed at high pressures have shown that, under hydrostatic conditions, these melts do not form an interconnected network, leading to the widespread assumption that formation of metallic cores requires a magma ocean. In contrast, here we present experiments which demonstrate that shear deformation to large strains can interconnect a significant fraction of initially isolated pockets of metal and metal sulphide melts in a solid matrix of polycrystalline olivine. Therefore, in a dynamic (non-hydrostatic) environment, percolation remains a viable mechanism for the segregation and migration of core-forming melts in a solid silicate mantle.     

Identification of multiple structural species in silicate glasses by 29Si NMR

Knowledge of the structure of silicate glasses is one key to understanding their chemical and physical properties, as well as those of the high-temperature liquids from which they form. Because first-neighbour ordering into SiO4 tetrahedra is well known, much of the recent discussion about glass structure has concerned intermediate-range order. One of the most fundamental questions that can be posed is the distribution of silicate tetrahedra with n bridging oxygens (shared between two tetrahedra), labelled as 'Qn' (0 less than or equal to n less than or equal to 4). This distribution is probably important in determining the properties of melts and glasses, but considerable controversy exists concerning the identification and quantification of such species. Here I present new evidence from 29Si NMR (nuclear magnetic resonance) spectroscopy that clearly resolves one significant part of this dispute: at least in sodium silicate glasses, a variety of species is present that is greater than that required by composition alone.     

超细粉末材料改性水玻璃粘结剂

从几种可能的超细材料里面筛选出一种最合适的超细材料,就这种材料对水玻璃粘结剂的具体性能影响展开研究.结果表明:用经过特殊处理后的超细粉末材料改性水玻璃粘结剂,具有常温强度高、残留强度低等优点;超细粉末材料改性的水玻璃粘结剂采用酯硬化工艺,可使水玻璃粘结剂的加入量低于3.0%,在水玻璃砂常温强度有所提高的前提下,其溃散性显著改善.较佳的超细粉末材料改性水玻璃粘结剂的测试结果为(与不改性水玻璃相比):常温24h强度提高了30.7%,残留强度下降了40.1%.     

188Re-放射性同位素支架置入治疗食管恶性狭窄

目的置入188Re放射性同位素支架,解除食管梗阻,姑息治疗食管狭窄,提高患者生存质量.方法对30例食管恶性狭窄病例,随机分为2组,分别置入188Re放射性支架、普通覆膜支架作前瞻性研究.结果188Re放射性支架初始活度128 MBq经3个半衰期2.12 d,皮下0.5 mm粘膜参考点吸收剂量21.62 Gy,皮下4 mm肌层参考点吸收剂量4.07 Gy.全部病例均一次置入成功,定位准确,支架复张良好.恶性狭窄缓解率93%(14/15,CR 4+PR 10),中位生存时间14个月,一年生存率66.67%.而对照组中多数病例于置入普通覆膜支架后3～6月因肿瘤向支架上下端生长造成再次狭窄,其中位生存时间9个月,一年生存率33.33%,较放射支架组差异显著(P＜0.01).放射支架组与对照组部分病例置入支架后出现胸骨后疼痛、暂时发热及出血,经治疗后缓解.结论188Re放射性支架治疗食管恶性狭窄近期疗效好、急性放射反应小,可作为姑息治疗手段.     

Fe同位素地球化学进展

Fe同位素是近年来发展起来的一门新兴的同位素地球化学方法,影响Fe同位素分馏的因素主要有生物有机作用和无机作用两种方式,研究证明,生物有机过程可以使Fe同位素产生大的分馏效应,因此根据Fe同位素组成的变化可以推测古环境中生命活动的存在,在一定的条件下无机作用也可能产生大的分馏效应,并可用于研究沉积物源的变化和古海洋环境的演化,Fe同位素有可能成为地球科学中具有巨大应用前景的一种新的地球化学方法。     

用壳聚糖重量法测定硅酸盐中的二氧化硅

采用壳聚糖为凝聚剂，重量法测定二氧化硅，试验了凝聚剂用量，溶液酸度、蒸发体积．放置时间及温度等对硅酸凝聚的影响，得出了最佳的沉淀条件，并测定了标准样品，测定结果的偏差较小．     

水玻璃固化黄土过程中电阻率参数的试验研究

为探究电阻率法在黄土硅化加固过程中应用的可行性,对施加上部荷载的重塑黄土注射水玻璃,同步测试不同电流频率下的土体横向及竖向电阻率,结合土体结构对电阻率参数的变化进行了分析。试验结果显示:随着不断升高的电流频率,黄土电阻率先逐渐减小并最终趋于稳定,当电流频率范围为5×104~1×106Hz时,电流频率对黄土电阻率实测值影响较小;随着固化时间的增加,黄土竖向和横向电阻率先减小并最终趋于稳定,且减小趋势均集中在初始阶段(200 min前)。随固化时间的增加,平均结构因子和平均形状因子均呈现先减小后稳定的趋势。各向异性系数随固化时间的增加先快速增大并最终趋于稳定。     

聚硅硫酸铝净化长江水的试验研究

以工业水玻璃、工业硫酸铝为原料制得聚硅硫酸铝（PASS）复合絮凝剂,用其净化长江水,处理后的长江水剩余浊度为0.5 NTU,pH=6.65,符合饮用水水质要求;用电子显微镜观察了PASS的形貌,用激光粒度仪分析了絮凝后形成絮体的粒度,与聚合氯化铝（PAC）进行比较,结果发现,PASS中形成了分子链更长、聚合度更大的聚合物,显示出比PAC更强的吸附架桥能力和更好的除浊效果;研究了聚硅硫酸铝与淀粉复合后对形貌及絮体粒度的影响,结果显示,淀粉加入聚硅硫酸铝中,PASS的形貌和粒度均未发生大的改变。     

Trace-element fractionation in Hadean mantle generated by melt segregation from a magma ocean

Calculations of the energetics of terrestrial accretion indicate that the Earth was extensively molten in its early history. Examination of early Archaean rocks from West Greenland (3.6-3.8 Gyr old) using short-lived 146Sm-142Nd chronometry indicates that an episode of mantle differentiation took place close to the end of accretion (4.46 +/- 0.11 Gyr ago). This has produced a chemically depleted mantle with an Sm/Nd ratio higher than the chondritic value. In contrast, application of 176Lu-176Hf systematics to 3.6-3.8-Gyr-old zircons from West Greenland indicates derivation from a mantle source with a chondritic Lu/Hf ratio. Although an early Sm/Nd fractionation could be explained by basaltic crust formation, magma ocean crystallization or formation of continental crust, the absence of coeval Lu/Hf fractionation is in sharp contrast with the well-known covariant behaviour of Sm/Nd and Lu/Hf ratios in crustal formation processes. Here we show using mineral-melt partitioning data for high-pressure mantle minerals that the observed Nd and Hf signatures could have been produced by segregation of melt from a crystallizing magma ocean at upper-mantle pressures early in Earth's history. This residual melt would have risen buoyantly and ultimately formed the earliest terrestrial protocrust.