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1.
变质沉积岩普遍含有碳质物,其源自沉积母岩中有机质。在变质过程中这些有机质逐渐转变为碳质物或石墨,且碳质物结晶程度可以作为变质等级的可靠指示标志。拉曼光谱是表征碳质物结晶度的有效工具,Beyssac et al.(2002a)基于碳质物拉曼光谱参数(R1=D1/G,D1和G为碳质物拉曼光谱峰强;R2=D1/(G+D1+D2),G、D1和D2为碳质物拉曼光谱峰面积)与寄主岩变质温度之间的线性关系构建了碳质物拉曼光谱温度计:T(℃)=-445(R2)+641,其简单且实用,并被应用到阿尔卑斯和喜马拉雅造山带热结构与折返机制研究中;随后,Rahl et al.(2005)对该变质温度计进行修订,修订后温度估算表达式为:T(℃)=737.3+320.9R1-1067R2-80.638R12,并将变质温度估算范围扩展为100~700℃。本文对碳质物拉曼光谱变质温度计的基本原理、方法、应用条件及其在造山带热结构重建与演化方面的研究进展进行了综述,并对碳质物拉曼光谱温度计与传统温度计估算的变质温度进行了系统的对比分析,结果表明碳质物拉曼光谱温度计代表峰期变质温度,不会受后期退变质影响,当传统温度计结果代表峰期变质温度时,二者计算结果一致。碳质物拉曼光谱温度计已被用于造山带热结构重建、折返过程的热演化,以及高应变带、流体相关热异常等研究。尽管变质过程的压力、变质持续时间、碳质物前体类型等因素对于碳质物拉曼光谱温度计的影响尚待研究,但与传统矿物组合温压计相结合,该方法可以有效评价峰期变质条件和造山多期热演化。 相似文献
2.
M. Okuno B. Reynard Y. Shimada Y. Syono C. Willaime 《Physics and Chemistry of Minerals》1999,26(4):304-311
The densification processes in SiO2 glass induced by shock-wave compression up to 43.4 GPa are investigated by Raman spectroscopy. At first, densification increases
with increasing shock pressure. A maximum densification of 11% is obtained for a shock pressure of 26.3 GPa. This densification
is attributed to the reduction of the average Si−O−Si angle, which occurs first by the collapse of the largest ring cavities,
then by further reduction of the average ring size. For higher shock pressures, a different structural modification is observed,
resulting in decreasing densification with increasing shock pressure. Indeed, the recovered densification becomes very small,
with values of 1.8 and 0.5% at 32 and 43.4 GPa, respectively. This is attributed to partial annealing of the samples due to
high after shock residual temperatures. The study of the annealing process of the most densified glass by in situ high temperature
Raman spectroscopy confirms that relaxation of the Si−O−Si angle starts at a lower temperature (about 800 K) than that of
the siloxane rings (about 1000 K), thus explaining the high intensity of the siloxane defect bands in the samples schocked
at compressions of 32 and 43.4 GPa. The large intensity of the siloxane bands in the nearly undensified samples shocked by
compressions above 30 GPa may be explained by the relaxation during decompression of five- and six-fold coordinated silicon
species formed at high pressure and high temperature during the shock event.
Received: March 30, 1998 / Revised, accepted: August 21, 1998 相似文献
3.
Kerogen has been artificially matured under “hydrous pyrolysis” conditions in the presence of various minerals in order to investigate the influence of the latter on the organic products. In addition to three clay minerals (montmorillonite, illite, kaolinite), calcium carbonate and limonite were also employed as inorganic substrates. Kerogen (Type II) isolated from the Kimmeridge Blackstone band was heated in the presence of water and a 20-fold excess of mineral phase at two different temperatures (280 and 330°C) for 72 hr. Control experiments were also carried out using kerogen and water only and kerogen under anhydrous conditions. This preliminary study describes the bulk composition of the pyrolysates with detailed analyses of the aliphatic hydrocarbon distributions being provided by gas chromatography and combined gas chromatography-mass spectrometry.In the 280°C experiments, considerably more organic-soluble pyrolysate (15% by weight of original kerogen) was produced when calcium carbonate was the inorganic phase. At 330°C, all samples generated much greater amounts of organic-soluble products with calcium carbonate again producing a large yield (40% wt/wt). Biomarker epimerisation reactions have also proceeded further in the 330°C pyrolysate formed in the presence of calcium carbonate than with other inorganic phases. Implications of these and other observations are discussed. 相似文献
4.
Lin-gun Liu C.-C. Lin Y. J. Yung T. P. Mernagh T. Irifune 《Physics and Chemistry of Minerals》2009,36(3):143-149
K-lingunite is a high-pressure modification of K-feldspar that possesses the tetragonal hollandite structure. Variations of
the Raman spectra of K-lingunite were studied up to ~31.5 GPa at room temperature, and in the range 79–823 K at atmospheric
pressure. The Raman frequencies of all bands were observed to increase with increasing pressure, and decrease with increasing
temperature for K-lingunite. This behavior is in line with those observed for most of other materials. New sharp Raman bands
appear at pressures greater than 13–15 GPa, suggesting a phase transition in K-lingunite with increasing pressure. The transition
is reversible when pressure was released. The appearance of these new Raman bands may correspond to the phase transition revealed
earlier at around 20 GPa by X-ray diffraction studies. Instead of transforming back to its stable minerals, such as orthoclase,
microcline or sanidine, K-lingunite became amorphous in the temperature range 803–823 K at atmospheric pressure. 相似文献
5.
高压下多硅白云母的拉曼光谱学研究 总被引：1，自引：0，他引：1
在金刚石压腔中，通过原位拉曼光谱研究了多硅白云母在常温高压下的稳定性。实验获得了多硅白云母从常压到20GPa的拉曼光谱数据，研究了多硅白云母的266、708和3618cm^-1叫谱峰与压力的相关性。研究发现，多硅白云母的708cm^-1叫谱峰随压力增加有规律地向高频方向偏移，与压力的增加呈明显的正相关性，即y（拉曼位移，cm^-1）=0．5238x（压力，GPa）＋712．31，相关系数R^2=0．9656，并且该谱峰在压力4．7GPa时消失，这可能与多硅白云母中的Si、Al替代有关。羟基3618cm^-1谱峰则随压力增加向低频方向移动，谱峰的降低与压力的增加呈明显的线性关系变化（y=-0．3402X＋3617．8，R^2=0．9662），并且强度随着压力的增加也在逐渐减弱，在压力达18GPa时开始消失，推测该压力可能为多硅白云母在常温下脱羟基的极限压力。 相似文献
6.
干酪根是沉积有机质的主体,是石油地质工作研究的重要对象,目前利用激光拉曼光谱进行干酪根的研究较少.雪峰山地区干酪根的拉曼光谱测试结果表明:干酪根的一级拉曼光谱峰位差与镜质体反射率之间有着系统的规律性变化,在Ro＜ 2.4％时,峰位差随Ro的增大迅速增大,其相关系数为0.82;Ro在2.4％～2.9％之间时,二者关系不明显,离散度较大;Ro＞2.9％时,峰位差随Ro的增大逐渐减小,相关系数为0.88.镜质体反射率是衡量有机质成熟度和热演化程度的重要指标,干酪根的拉曼光谱特征与镜质体反射率之间的关系表明激光拉曼光谱法可以成为有机质成熟度和热演化程度研究的新方法. 相似文献
7.
Kerogen was isolated from a marine sediment from Tanner Basin, offshore California. Samples of the kerogen were heated under an inert atmosphere at various temperatures and times. The heated and unheated kerogens were subjected to alkaline potassium permanganate oxidation followed by GC/ MS analysis of the products. The kerogens yielded primarily aliphatic C2–C14 α,ω-dicarboxylic acids and benzene mono-to-pentacarboxylic acids. Yields of aliphatic dicarboxylic acids from kerogen decreased with increasing thermal alteration. Yields of benzenecarboxylic acids increased steadily with increasing thermal alteration. The data support the concept that thermal maturation during natural burial of this type of kerogen results in the generation of aliphatic hydrocarbons from an increasingly aromatic residue. 相似文献
8.
甘肃西成铅—锌矿田干酪根的特征 总被引：4，自引：0，他引：4
本文对西成矿田中泥盆统内含有机碳岩石中干酪根分析，认为该区内的干酪根主要由镜质体，壳质体，藻质体，惰质体，惰质组和矿物质组成，属于腐植型干酪根，颜色从淡黄到黑色，从西向东颜色加深，Ｒ０值也有同样的趋势，说明在矿区内成熟度不一致，热解分析发现Ｓ２峰有分叉现象，经过氯仿抽提后分叉消失，从可溶有机质的色谱分析中发现有大量氮硫氧化合物，证明分叉现象可能是由氮硫氧化合物引起。Ｒ０值越大，反映出干酪根的再改造 相似文献
9.
A unified equation for calculating methane vapor pressures in the CH4-H2O system with measured Raman shifts 总被引：2，自引：0，他引：2
A unified equation has been derived by using all available data for calculating methane vapor pressures with measured Raman shifts of C-H symmetric stretching band (υ1) in the vapor phase of sample fluids near room temperature. This equation eliminates discrepancies among the existing data sets and can be applied at any Raman laboratory. Raman shifts of C-H symmetric stretching band of methane in the vapor phase of CH4-H2O mixtures prepared in a high-pressure optical cell were also measured at temperatures between room temperature and 200 °C, and pressures up to 37 MPa. The results show that the CH4υ1 band position shifts to higher wavenumber as temperature increases. We also demonstrated that this Raman band shift is a simple function of methane vapor density, and, therefore, when combined with equation of state of methane, methane vapor pressures in the sample fluids at elevated temperatures can be calculated from measured Raman peak positions. This method can be applied to determine the pressure of CH4-bearing systems, such as methane-rich fluid inclusions from sedimentary basins or experimental fluids in hydrothermal diamond-anvil cell or other types of optical cell. 相似文献
10.
O. Amit 《Organic Geochemistry》1979,1(4):237-241
Kerogen from various samples of the Gevar'am Formation (Early Cretaceous, Israel) were analyzed for their elemental composition, and by I.R. and ESR spectroscopy. The results were compared with other organochemical characteristics of the basin (Amit, 1978, Bull. Am. Assoc. Pet. Geol., V. 62 p. 827–836). The types of organic material and their role in the formation of oil were investigated. It appears that the kerogen is mostly constituted of terrestrially derived organic matter. A small amount of marine-derived organic matter is also inferred. The kerogen of terrestrial origin is a poor oil producer and is expected to generate oil only at a higher stage of maturation than the Gevar'am Formation has attained. Any hydrocarbons that have been generated in this formation were probably generated from that part of the kerogen thought to be marine derived. Thus the Gevar'am Formation is considered as a potential source rock which has generated only a small amount of oil. 相似文献
11.
《矿物学报》2013,(Z1)
Graphite and graphite-like materials widely are present at black shale and magmatic ores. The nature of these carbon materials (CM) is multifarious. In what cause connects a mineralization with carbon. The great numbers of parameters, namely, the temperature, the pressure, the shear stress, the catalytic species, the host-rock lithology, the time and etc., have an influence on the graphitization process. Accumulations of gold and platinum group elements in black graphite shale and extraction of these metals from rocks depend in considerable degree from structural properties of CM. Raman spectroscopy has wide applied for various carbon modifications, including nano-structuring materials. The first and second-order Raman spectrum have been correlated with changes in the structure of graphite. There is a linear relationship between temperature and Raman R2 and R1 parameters (derived from the area and intensity of the defect band (D) relative to the ordered graphite band (G), respectively). The purpose of the present study is to characterize the rocks and CM from carbon-rich rocks of gold-ore deposits of the black-shale formation and magmatic ores using micro-Raman spectroscopy technique (Horiba Jobin Ivon LabRam spectrometer). Exciting was performed with 325 nm line of He-Cd laser. The graphite and graphite-like samples from many ore deposits of Russia and Kazahstan are investigations. R1 and R2 ratio indicate variable degree of organisation CM in the samples. The results show different spectral variations of CM with metamorphic grade: the well-ordered graphite from magmatic rocks, more - ordered and the disordered less graphitized CM from black-shale ores. For the first time in the world practice the Raman spectroscopy technique has been applied to determine the temperature of graphitizing for CM at gold-ore deposits of the black-shale formation. The temperatures obtained on carboniferous substance for the gold deposits range from 405°С to 280°С. Temperature of CM formation from Pt-low sulphide ores of the Talnakh deposit ranges from 4700C to 6500C. It has been shown that the carbon-rich phases from black-shale and magmatic rocks have various degrees of graphitization and different carbon forms. 相似文献
12.
Measurements are presented of volume changes in granite during room-temperature compression to 100, 200 and 300 MPa confining pressure followed by temperature increase to 900°C. Comparison with thermal expansion and compressibility data for the constituent minerals allows changes in porosity to be estimated. Under confining pressure, porosity is found to decrease with heating to 200°C through expansion of the minerals into cracks which are thought to be related to the geological cooling history of the rock. Between 200°C and 840°C porosity increases as a result of differential thermal expansion of the constituent minerals, but crack opening is increasingly suppressed at higher confining pressures. Extrapolation of the results indicates that differential thermal expansion can no longer cause crack opening in dry granite at confining pressures in excess of 450 MPa. The quartz α-β transition temperature in granite is marked by a kink in the thermal expansion curve of the rock, and it is found to increase by 60°C–70°C per 100 MPa confining pressure, as opposed to the published value of 26°C per 100 MPa for single crystals of quartz. Equations are presented which allow calculation of the effects of confining pressure and temperature on the stresses and displacements in and around a spherical inclusion embedded in a matrix of different elasticity and thermal expansion. The theory, together with a simple self-consistent model for granite, accounts semiquantitatively for the observations of thermal expansion and the effect of confining pressure thereon, and for the observed α-β transition temperatures for quartz in granite. 相似文献
13.
The hydroxyl stretching frequencies of four phyllosilicates have been measured at high pressures and temperatures using an externally heated diamond-anvil cell and synchrotron infrared spectroscopy. Spectra were measured up to 26, 31, 21 and 8 GPa at room temperature for samples of talc, pyrophyllite, muscovite and 10-Å phase, respectively. Spectra were also measured in the range 273–500 K at ambient pressure for all samples and at 8–9 GPa for talc and pyrophyllite. The frequency of the Mg3OH band in talc increases with pressure due to the absence of hydrogen bonding. The different orientation of the hydroxyl group in pyrophyllite and muscovite leads to hydrogen bonding and a decrease in the frequency of the Al2OH band with pressure. 10-Å phase is approximately equivalent to talc with the addition of interlayer H2O. In a spectrum of a sample synthesised for 143 h, two hydroxyl stretching bands are clearly resolved on compression. One is the same as the Mg3OH band in talc, indicating the presence of intra-layer hydroxyl in a talc-like environment with no hydrogen bonding. The other, which separates from the talc-like band at 1 GPa, is associated with intra-layer hydroxyl that is hydrogen bonded to interlayer H2O. There are equivalent bands in high-pressure spectra of a sample of deuterated 10-Å phase, synthesised for 400 h. This sample shows a greater extent of hydrogen bonding at ambient pressure than the 143 h sample. For all of the phases studied, increasing temperature leads to a decrease in frequency for every hydroxyl stretching vibration, both at low and high pressures. The shifts in frequency with temperature are an order of magnitude greater than the shifts with pressure when normalised to previously measured structural parameters. 相似文献
14.
B. Reynard M. Okuno Y. Shimada Y. Syono C. Willaime 《Physics and Chemistry of Minerals》1999,26(6):432-436
Structural modifications induced by shock-wave compression up to 40 GPa in anorthite glass are investigated by Raman spectroscopy.
In the first investigation, densification increases with increasing shock pressure. A maximum densification of 2.2% is obtained
for a shock pressure of 24 GPa. This densification is attributed to a decrease of the average ring size, favoring three-membered
rings. The densification is much lower than in silica glass subject to shock at similar pressures (11%), because the T-O-T
bond angle decrease is impeded in anorthite glass. For higher shock pressures, the decrease of the recovered densification
is attributed to partial annealing of the samples due to high after-shock residual temperatures. The study of the annealing
process of the most densified glass by in-situ high temperature Raman spectroscopy confirms that relaxation of the three-membered
rings occurs above about 900 K.
Received: 21 July 1998 / Revised and accepted: 27 January 1999 相似文献
15.
Variations of Raman spectra of hydroxyl-clinohumite were studied up to ∼370 kbar at room temperature, and in the range 81–873 K
at atmospheric pressure. With the exception of the symmetric OH-stretch bands, the Raman frequencies of all bands were observed
to increase monotonically with increasing pressure, and decrease with increasing temperature. This behavior is in line with
those observed for other humite members (norbergite and chondrodite) so far studied. The symmetric OH-stretching band shows
a mode softening with increasing pressure, and splits into two bands at either high pressure or low temperature. In the quasihydrostatic
experiment, the compression and decompression paths of one of the asymmetric OH-stretch bands form a hysteresis loop, but
the same behavior was not observed in the nonhydrostatic experiment. These results indicate that the two kinds of OH groups
in hydroxyl-clinohumite have nonequivalent movement paths on compression, and with one OH group experiencing a release of
spatial hindrance during compression. This behavior appears to be modified by shear stress. The same complication of the OH
groups was not observed in the temperature variation study. The pressure and temperature variations of the Raman frequencies
for the various vibrations involving the SiO4 tetrahedra and MgO6 octahedra below ∼1000 cm−1 for clinohumite behave similarly to other hydrous magnesium silicates. On the basis of the relationship between isothermal
bulk modulus and Raman data, it is suggested that the linear pressure dependences of vibrational frequencies of various Raman
bands reported in the literature are inadequate.
Received: 20 March 1999 / Revised, accepted: 24 August 1999 相似文献
16.
本文应用金刚石压腔装置结合拉曼光谱分析技术原位观测了高温高压条件下水镁石的结构变化特征。结果表明：常温升至300℃过程中,随温度升高,水镁石中表征H-O对称伸缩振动的3652 cm-1拉曼特征峰向低波数移动,拉曼特征峰波数与对应的体系温度呈现良好的线性相关关系。常温条件下体系加压过程中,当压力升高至1.19 GPa时,水镁石中表征H-O振动的3652 cm-1拉曼峰向高波数移动并逐渐消失,同时产生表征方镁石的1078 cm-1拉曼特征峰,表明水镁石脱水相变为方镁石。随后压力降低过程中,表征水镁石H-O振动的3652 cm-1拉曼特征峰没有重新出现,脱水相变过程不可逆。 相似文献
17.
Anke Putschew Christine Schaeffer-Reiss Philippe Schaeffer Martin P Koopmans Jan W de Leeuw Michael D Lewan Jaap S Sinninghe Damsté James R Maxwell 《Organic Geochemistry》1998,29(8):1875-1890
An immature sulfur-rich marl from the Gessosso-solfifera Formation of the Vena del Gesso Basin (Messinian, Italy) has been subjected to hydrous pyrolysis (160 to 330°C) to simulate maturation under natural conditions. The kerogen of the unheated and heated samples was isolated and the hydrocarbons released by selective chemical degradation (Li/EtNH2 and HI/LiAlH4) were analysed to allow a study of the fate of sulfur- and oxygen-bound species with increasing temperature. The residues from the chemical treatments were also subjected to pyrolysis–GC to follow structural changes in the kerogens. In general, with increasing hydrous pyrolysis temperature, the amounts of sulfide- and ether-bound components in the kerogen decreased significantly. At the temperature at which the generation of expelled oil began (260°C), almost all of the bound components initially present in the unheated sample were released from the kerogen. Comparison with an earlier study of the extractable organic matter using a similar approach and the same samples provides molecular evidence that, with increasing maturation, solvent-soluble macromolecular material was initially released from the kerogen, notably as a result of thermal cleavage of weak carbon–heteroatom bonds (sulfide, ester, ether) even at temperatures as low as 220°C. This solvent-soluble macromolecular material then underwent thermal cleavage to generate hydrocarbons at higher temperatures. This early generation of bitumen may explain the presence of unusually high amounts of extractable organic matter of macromolecular nature in very immature S-rich sediments. 相似文献
18.
拉曼光谱能够反映碳材料结构的有序程度和结构缺陷,可用来表征高煤级煤—隐晶质石墨演化过程中结构变化。通过对受岩浆热变质影响的不同变形变质程度样品的拉曼参数与面网间距（d002）之间关系的研究表明:G峰位置与d002呈现阶梯变化,能较好地区分出石墨与高煤级煤,S2峰位、D1、G半峰宽与d002呈较好的线性关系;D1与G峰峰位差和半峰宽比随d002减小而减小,S2与S4峰的峰位差随d002减小先增大后减小,而其强度比及面积比逐渐增大;d002与拉曼参数关系显示两次明显的结构演化跃变,即无烟煤至变质无烟煤阶段,Rmax>6.5%、P（D1-G）<235 cm-1、P（S2-S4）>525 cm-1以及半峰宽比显著下降、La/Lc迅速降低,为芳构化、芳环缩合作用增强向芳环叠片拼叠转变;半石墨至石墨演化阶段,P（D1-G）、ID1/IG与AD1/AG显著降低,La、Lc迅速增加。以d002为标度能较好地反映煤结构在不同演化阶段的Raman光谱特征。 相似文献
19.
使用配备Linkam冷热台的显微激光拉曼光谱仪,采用融合二氧化硅毛细管样品,在-120～31℃温度区间,1 200～1 500cm-1光谱区间上,原位采集H2O-CO2体系流体包裹体的拉曼光谱,并针对CO2特征拉曼光谱展开分析。结果表明,融合二氧化硅毛细管样品中的流体具有代表性。通过对毛细管样品进行拉曼光谱采集,该实验获得了流体包裹体中CO2气相、CO2液相、CO2固相、CO2水合物相和CO2水溶液相的特征光谱。光谱分析结果显示,在实验温度区间上,CO2固相和CO2水合物相特征峰的稳定性,有助于鉴别拉曼光谱;同时,CO2气相、CO2液相和CO2水溶液相费米共振峰峰位因CO2压力或密度影响而发生变化。此外,该实验在温度变化过程中,鉴定了不同相的拉曼特征光谱。结果表明,激光拉曼光谱结合显微测温技术能够有效鉴别包裹体中不同的流体相,获得相变过程,确定相变温度。 相似文献
20.
M. Koch-Müller P. Dera Y. Fei H. Hellwig Z. Liu J. Van Orman R. Wirth 《Physics and Chemistry of Minerals》2005,32(5-6):349-361
We synthesized superhydrous phase B (shy-B) at 22 GPa and two different temperatures: 1200°C (LT) and 1400°C (HT) using a
multi-anvil apparatus. The samples were investigated by transmission electron microscopy (TEM), single crystal X-ray diffraction,
Raman and IR spectroscopy. The IR spectra were collected on polycrystalline thin-films and single crystals using synchrotron
radiation, as well as a conventional IR source at ambient conditions and in situ at various pressures (up to 15 GPa) and temperatures
(down to −180°C). Our studies show that shy-B exists in two polymorphic forms. As expected from crystal chemistry, the LT
polymorph crystallizes in a lower symmetry space group (Pnn2), whereas the HT polymorph assumes a higher symmetry space group (Pnnm). TEM shows that both modifications consist of nearly perfect crystals with almost no lattice defects or inclusions of additional
phases. IR spectra taken on polycrystalline thin films exhibit just one symmetric OH band and 29 lattice modes for the HT
polymorph in contrast to two intense but asymmetric OH stretching bands and at least 48 lattice modes for the LT sample. The
IR spectra differ not only in the number of bands, but also in the response of the bands to changes in pressure. The pressure
derivatives for the IR bands are higher for the HT polymorph indicating that the high symmetry form is more compressible than
the low symmetry form. Polarized, low-temperature single-crystal IR spectra indicate that in the LT-polymorph extensive ordering
occurs not only at the Mg sites but also at the hydrogen sites. 相似文献