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1.
A Cambrian solid bitumen from northwestern Sichuan Basin, southern China was analyzed using two different flash pyrolysis methods coupled with gas chromatography–mass spectrometry analysis, including Pyroprobe® and analytical laser micropyrolysis. Results show that pyrolysis products from a Pyroprobe® (model 5000) analysis are dominated by mono-, di- and tricyclic aromatic hydrocarbons, whilst those from laser micropyrolysis are dominated by aliphatic hydrocarbons (n-alk-1-ene/n-alkane doublets), which is consistent with the results from an FT-IR spectrum of the solid bitumen. According to the molecular compositions of the pyrolysates from two types of pyrolysis, results from a 532 nm continuous wave laser may be more suitable for pyrolysis research of bitumen/asphaltene. Thus, differences in pyrolysis techniques must be considered when used to characterize oil asphaltenes or source rock kerogens.  相似文献   

2.
Very little is known about the macromolecular properties of biomass combustion residues referred to as black carbon (BC). Pyrolysis-gas chromatography–mass spectrometry (Py-GC/MS) was performed on: (i) peat from Spain at 400–1200 °C to investigate the effect of charring on pyrolysis fingerprint and (ii) natural charcoal from Laos in order to link molecular information to published chemical and reactivity parameters. Confirming earlier Py-GC/MS studies, the BC in the artificially charred peat and the natural charcoal produced predominantly benzene, toluene, C2-benzenes, PAHs and benzonitriles. Furthermore, some charcoal samples produced significant amounts of phenols, methoxyphenols, carbohydrate markers, n-alkanes and n-alkenes upon pyrolysis, reflecting non-charred and weakly charred biomass. A series of pyrolysis product ratios related to the degree of dealkylation of the pyrolysis products (benzene/toluene, naphthalene/C1-naphthalenes, C1-naphthalenes/C2-naphthalenes, benzofuran/C1-benzofurans and benzonitrile/C1-benzonitrile) increased with increasing artificial charring (peat) and, for the natural charcoal, these ratios were in accordance with established chemical and reactivity parameters related to charring intensity from other methods: proportion of aromatic C obtained from solid state 13C nuclear magnetic resonance spectroscopy (NMR), the proportion of charred material as estimated from NMR in conjunction with a molecular mixing model (NMR–MMM) and the resistance to acid dichromate oxidation. The alkyl side chains of aromatic pyrolysis products are probably inherited from short chain aliphatic C chains that cross link the predominantly aromatic building blocks of BC, and these linkages seem to disappear with increasing charring intensity. Thus, the degree of thermal alteration of BC can be discerned from the pyrolysis fragmentation pattern.  相似文献   

3.
Incubation of intact and oxidized α-tocopherol (vitamin E) in anaerobic sediment slurries allowed us to demonstrate that, as previously suggested by Goossens et al. (1984), the degradation of α-tocopherol in anoxic sediments results in the formation of pristane. The conversion of α-tocopherol to this isoprenoid alkane involves a combination of biotic and abiotic degradative processes, i.e. the anaerobic biodegradation (which seems to be mainly induced by denitrifying bacteria) of trimeric structures resulting from the abiotic oxidation of α-tocopherol. On the basis of the results obtained, it is proposed that in the marine environment most of the α-tocopherol present in phytoplanktonic cells should be quickly degraded within the water column and the oxic zone of sediments by way of aerobic biodegradation, photo- and autoxidation processes. Abiotic transformation of this compound mainly results in the production of trimeric oxidation products, sufficiently stable to be incorporated into anoxic sediments and whose subsequent anaerobic bacterial degradation affords pristane. These results confirm that the ratio pristane to phytane cannot be used as an indicator of the oxicity of the environment of deposition; in contrast, they support the use of PFI (Pristane Formation Index) as a proxy for the state of diagenesis of sedimentary organic matter.  相似文献   

4.
分步瞬时热解法可以有效的用于研究干酪根（或其他相关样品）结构组分随温度变化而演变的详细特征。利用分步瞬时热解法从300℃到600℃共分七个温度点,依次对绿河页岩干酪根样品进行热模拟分析。结果表明:在300℃时,绿河页岩干酪根样品基本没有热解产物,在350℃时可检测到少量吸附烃但含量极少;400℃、450℃和500℃是热解产物十分丰富的三个温度点,主要产物是成对出现的正构烷烃和直链烯烃,同时含有一定量的异构烷烃和姥鲛-1-烯;随着热解温度升高,异构烷烃和长链烃类的相对含量逐渐减少;姥鲛-1-烯在400℃和450℃一直占据主要地位;550℃出现了长碳链烷烃（C27~C32）,很有可能是绿河页岩干酪根样品中类似于绿藻等的组分经高温裂解产生的;600℃之后热解产物基本消失,说明在低温阶段干酪根裂解作用就基本完全。另外,绿河页岩干酪根样品在不同温度点的瞬时热解均给出了相应的产物组分构成,对比研究发现,其产物种类及相对含量具有逐渐变化的特征,由此将更有利于研究干酪根的热演化及其成烃机制。  相似文献   

5.
The molecular composition of fossil resin from the Eocene Ameki Formation, southern Nigeria has been analyzed by infrared spectroscopy, pyrolysis–gas chromatography–mass spectrometry and thermochemolysis gas chromatography–mass spectrometry to determine the structural class and botanical source of the resin. The pyrolysis products were dominated by bicyclic products derived from regular labdatriene structure and lacked succinic acid indicating Class Ib type amber. The biomarker compositions in the pyrolysates are dominated by sesquiterpenoids of the cadinane and bisabolane classes that are common constituents of higher plants and labdane type diterpenoids. The exclusive presence of labdane type diterpenoids and the absence of higher plant triterpenoids strongly suggest that the amber was derived from a gymnosperm (conifer) botanical source. This observation contrasts with the angiosperm source previously suggested for the resin based on the palaeobotanical studies of the host sediments. The specific family source within the conifers could not be ascertained based on the molecular composition of the resin. However, the presence of methyl-16,17-dinor-callitrisate pointed to the Cupressaceae family although other Cupressaceae biomarker indicators were not detected in the resin.  相似文献   

6.
Influence of frothers (α-terpineol or n-amyl alcohol) on the floatability of chalcocite and quartz mixtures, with potassium ethyl xanthate as a collector at pH 5.5–6, was investigated with a Hallimond tube.Activation of quartz by the presence of chalcocite was observed and interpreted as due to copper ionic species originating from chalcocite oxidation products. Best selectivity of separation between chalcocite and quartz was obtained when the frother concentration was kept sufficiently low. Collector—frother interactions during formation of three-phase mineral grain/solution/gas bubble contacts were observed.  相似文献   

7.
A series of experiments have been conducted with polyethylene and polystyrene standards in an attempt to define the advantages and limitations of a vacuum pyrolysis—gas chromatography—mass spectrometry procedure for the characterization of kerogen and other macromolecular substances. Effects of variations in pyrolysis temperatures and times, sample sizes (weights) and thickness were evaluated together with the reproducibility of the nature and abundances of pyrolyzates. The effects of minerals (illite and quartz) admixed in the polymers were also considered with reference to the nature of the breakdown products. Optimal pyrolysis conditions, where primary pyrolyzates were sufficiently abundant and secondary products did not hinder characterization, were attained at 450°C and 60–90 min. The reproducibility of the nature and quantities of pyrolyzates was rather satisfactory at this temperature and pyrolysis time. However, relatively large samples of macromolecular matter, which is considerably volatile at this temperature, led to the synthesis of an abundant yield of secondary products, but sample thickness does not affect the nature of pyrolyzates. Admixed mineral matter affected the nature and relative abundances of the pyrolyzates but did not impede characterization of samples, as primary breakdown products were discernible. Macromolecular substances of limited volatility, heterogeneous chemical composition and containing intractable mineral matter, such as many kerogens, need to be pyrolyzed as relatively large samples. The vacuum procedure used in these studies may be to advantage, as compared with some other methods, to pyrolyze such samples. This method seems to be also suitable for the pyrolysis of volatile macromolecular matter, provided that small samples are employed.  相似文献   

8.
Total organic carbon (TOC) determination, Rock‐Eval pyrolysis, extractable organic matter content (EOM) fractionation, gas chromatography (GC) and gas chromatography–mass spectrometry (GC–MS) analyses, were carried out on 79 samples from eleven outcrop cross sections of the Bahloul Formation in central and northern Tunisia. The TOC content varied between 0.23 to 35.6%, the highest average values (18.73%, 8.46% and 4.02%) being at the east of the study area (at Ain Zakkar, Oued Bahloul and Dyr Ouled Yahia localities, respectively). The Rock‐Eval maximum pyrolysis temperature (Tmax) values in the 424–453°C range delineated a general east‐west trend increase in the organic matter (OM) maturity. The disparity in hydrogen index (HI) values, in the range 114–824 mg hydrocarbons (HC) g?1 TOC, is relevant for the discrepancy in the level of OM preservation and maturity among localities and samples. The n‐alkane distributions, maximizing in the C17 to C20 range, are typical for a marine planktonic origin, whereas pristine/phytane (Pr/Ph) average values in the 1–2 range indicate an oxic to suboxic depositional environment. Pr/n‐C17 and Ph/n‐C18 ratios in the 0.38–6.2 and 0.68–3.25 range, respectively, are consistent with other maturity indicators and the contribution of specific bacteria to phytol as a precursor of isoprenoids. The thermal maturity varies between late diagenesis to main‐stage of petroleum generation based on the optic and the cis‐trans isomerisation of the C29 sterane [20S/(20S+20R) and 14β(H),17β(H)/(14β(H),17β(H)+14α(H),17α(H)), respectively] and the terpane [18α(H)22,29,30‐Trisnorneohopane/(18α(H)22,29,30‐Trisnorneohopane+17α(H)22,29,30‐Trisnorhopane): Ts/(Ts+Tm)] ratios. The Bahloul OM is represented by an open marine to estuarine algal facies with a specific bacterial contribution as revealed by the relative abundance of the ααα‐20R C27 (33–44%), C28 (22–28%) and C29 (34–41%) steranes and by the total terpanes/total steranes ratio (1.2–5.33). These results attested that the Bahloul OM richness was controlled both by an oxygen minimum zone induced by high productivity and restricted circulation in narrow half graben structures and around diapirs of the Triassic salt.  相似文献   

9.
A series of biomarkers were analyzed in the 4000 a B.P. loess sediments in Balong, Dulan County at the north of the eastern Kunlun Mountain in Northwest China using gas chromatography-mass spectrometry. Olean-2,13 (18)-ene, olean-2,12-ene, urs-2,12-ene and 5α14α17 α20R-stigmasterane identified in an ancient culture bed were observed in association with charcoal grains, believed to be the products of paleofire due to the anthropogenic activity in Qijia culture. These triterpenes were proposed to be derived from dehydration of oleanolic acid and ursolic acid present in angiosperms, and 5α14α17α20R-stigmasterane was derived from stenols; they both were formed during incomplete combustion. The n-alkane distributions show a shift in the dominant carbon from C27 or C29 to C31, indicative of the abrupt change in paleovegetation from woody to herbaceous plants driven by the changing paleoclimate at 4000 a B.P. after the Holocene Optimum. Coincidently, the Qijia agriculture culture began to collapse during the 200-year cooling and dryness, and was replaced by nomadism in the mountainous area. The paleofire identified is such a record as to document the change of ancient culture induced by paleoclimate change.  相似文献   

10.
Active participation of gas–oil fluids in the processes of mineral formation and petrogenesis in travertines of the Arshan and Garga hot springs is substantiated. The parageneses of the products of pyrolytic decomposition and oxidation of the gas–oil components of hydrothermal fluids (amorphous bitumen, graphite-like CM, and graphite) with different genetic groups of minerals crystallized in a wide range of P–T conditions were established. Travertines of the Baikal rift zone were formed from multicomponent hydrous–gas–oil fluids by the following basic mechanisms of mineral formation: chemogenic, biogenic, cavitation, fluid pyrometamorphism, and pyrolysis.  相似文献   

11.
Organic matter(OM)is intimately associated with minerals in clay-rich mudstones,leading to widespread organic-mineral interaction during hydrocarbon generation in argillaceous source rocks.What we are concerned is the effects of the different mineral properties on hydrocarbon generation process and mechanism during mineral transformation.In this way,pyrolysis experiments with smectite-octadecanoic acid complexes(Sm-OA and Ex-Sm-OA)were conducted to analyze correlation of mineralogy and pyrolysis behaviors.Based on organicmineral interaction,hydrocarbon generation process was divided into three phases.At 200–300℃,collapse of smectite led to desorption of OM,resulting in high yield of resin and slight increase in saturates.Subsequently,enhanced smectite illitization at 350–450℃was accompanied with large amounts of saturates and a mere gaseous hydrocarbon.Featured by neoformed plagioclase,ankerite,and illite,500C saw plenty of asphaltene and methane-rich gaseous hydrocarbons,revealing cracking reactions of OM.Noteworthy is that saturated and gaseous hydrocarbons in Ex-Sm-OA were considerably more than that in Sm-OA during second and third phases.Quantitative calculation of hydrogen revealed organic hydrogen provided by cross-linking of OM could not balance hydrogen consumed by cracking reactions,but supply of inorganic hydrogen ensured cracking could readily occur and consequently greatly promoted hydrocarbon generation.Further investigating characteristics of mineralogy and pyrolytic products,as well as effects of solid acidity on hydrocarbon generation,we concluded desorption of OM and decarboxylation promoted by Lewis acid were dominated at 200–300C,resulting in lowdegree hydrocarbon generation.While high yield of saturated and gaseous hydrocarbons in second and third phases,together with occurrence of ankerite,indicated predominance of decarboxylation and hydrogenation promoted by Lewis and Br?nsted acid,respectively.Variations in organic-mineral interactions indicated(1)the controls of mineral transformation on hydrocarbon generation process and mechanism include desorption,decarboxylation,and hydrogenation reactions;(2)clay minerals acted as reactants evolving together with OM rather than catalysts.These findings are profoundly significant for understanding the hydrocarbon generation mechanisms,organic-inorganic interactions,and carbon cycle.  相似文献   

12.
Analysis of noble gas proportions and their release kinetics during stepped pyrolysis and oxidation of meteoritic nanodiamonds, as well as their core-shell structure led to the following conclusions: (1) Noble gases of HL component with anomalous isotopic composition were presumably formed prior to implantation in the nanodiamonds owing to mixing of nucleosynthetic products of p- and r- process associated with explosion of type-II supernova with noble gases having “normal” isotopic composition; (2) isotopically normal P3 noble gases in the nanodiamonds grains are confined to the nondiamond (for instance, graphite-like) phase in the surface layer. The “layer” structure of nanodiamonds grains resulted from heating up to 800–900°C. Observed increase in contents of P3 noble gases with increasing grain sizes of meteoritic nanodiamonds is caused by the dependence of the degree of graphitization of the superfical layer at given temperature on the grain size and surface defect density; (3) bimodal release of noble gases during pyrolysis of the meteoritic nanodiamonds from weakly metamorphosed meteorites was caused by P3 and HL components, which are comparable in abundance but sharply differ in their release temperature.  相似文献   

13.
Air entrainment in fragmented magmas controls the dynamics of volcanic eruptions. Pyroclast oxidation kinetics may be applied to quantify the degree of magma–air interaction. Pyrrhotite (Po) in volcanic rocks is often oxidized to form magnetite (Mt) and hematite (Hm), and its reaction mechanisms are well constrained. To test utilizing Po oxidation as a marker for magma–air interactions, we compared the occurrence of Po oxidation products from three different eruption styles during the Sakurajima 1914–1915 eruption. Pumices from the Plinian eruption include columnar-type Fe oxides (Mt with subordinate width of Hm) often accompanied by relict Po. This columnar type is also found in clastogenic lava, where it is almost completely oxidized to Hm. The effusive lava contains framboidal aggregates of subhedral to anhedral Mt crystals without Hm. The formation mechanisms of columnar and framboidal Fe oxides were estimated. The columnar type Fe oxides were formed syn-eruptively through gaseous reactions, as opposed to the melt in a magma chamber, as demonstrated by the Ti-free nature of the columnar Mt and its synchronous oxidation to Hm. By contrast, the framboidal type was formed in a melt with decreasing fS2. The calculation of Hm growth in a conductively cooling pumice clast constrains the surface temperature of pumice in the eruption column. The paragenesis and oxidation degree of Po and Fe oxides are consistent with the eruption processes in terms of magma fragmentation, air entrainment, and welding, and can, therefore, be a responsive marker for the magma–air interaction.  相似文献   

14.
Asphaltenes extracted from crude oils are proposed to possess structural features of the related source rock kerogen. For the present study micro-scale sealed vessel pyrolysis (MSSV) and combustion isotope ratio mass spectrometry (GC–C–IRMS) were used to compare gas generation from a whole rock (type II-S kerogen) from southern Italy with that from related sulfur rich asphaltenes isolated from a low maturity heavy crude oil. The purpose of was to determine whether experimental pyrolysis of oil asphaltenes can be used to predict the timing and the chemical and isotopic composition of hydrocarbon gases generated from genetically related kerogen in the source rock during burial maturation. The results show that parameters such as (gas to oil ratio) GOR and oil and gas formation timing are very similar for these two sample types, whereas gas composition, product aromaticity and sulfur content are remarkably different. Slight differences in GOR are mainly due to differences in gas formation characteristics at very high levels of thermal alteration. Secondary gas formation from the whole rock covers a much broader temperature range under geological conditions than that from the asphaltene products. However, it is remarkable that both the onset and the maximum temperature are nearly identical under geological conditions. The observed differences in gas generation characteristics are supported by discrepancies in the carbon isotopic characteristics of the gas range compounds and indicate different precursors and/or mechanisms for gas generated from whole rock and asphaltenes.  相似文献   

15.
Class Ib resinites are the most common subclass of amber and are found throughout the world. They have a macromolecular structure based on co-polymerized communic acid, communol and biformenes. Because this class of resinite does not contain succinic acid, crosslinking of the polymer through esterification of communol moieties has never been theorized. Analysis of Class Ib resinites from Grassy Lake and Cedar Lake in western Canada was performed using pyrolysis–gas chromatography–mass spectrometry with in situ hexamethyldisilazane derivatization, using a thermal separation probe to perform the pyrolysis and sample introduction. This has allowed larger, more complex fragments to be released from the polymer matrix than previously possible using instantaneous pyrolysis methodologies. The results show for the first time that Class Ib resinite can undergo self-crosslinking between the communol and communic acid moieties in the polylabdane matrix. The chromatographic results also show that a portion of the monoterpenes and non-polymerizable diterpenes in the resinite are bound to the polymer matrix and not fully occluded as was previously theorized. Fourier transform infrared (FTIR) spectra of the resinites are presented and a more accurate spectral interpretation is proposed, based on the chromatographic results.  相似文献   

16.
The El Sela area is a part of the basement complex of the Eastern Desert of Egypt and the Pan-African Shield. The area comprises outcrops of dismembered ophiolites thrust over arc volcano-sedimentary sequence and intruded by different syn- to post-tectonic granitoids. Structural analysis of the area enabled the separation and definition of four structural episodes: (E1) folding–thrusting episode associated with the cratonization of the arc/inter-arc rock association and the intrusion of the syntectonic (Older) granites. (E2) Upright folding episode associated with the compression and shortening to the ENE–WSW direction which is different from the NNW–SSE shortening direction during E1; at the end of E2, late tectonic granites were intruded. (E3) Post-tectonic granitic intrusion episode: two mica granite and granitic dikes were intruded during this episode. (E4) Fracturing, faulting, and post-granitic dike extrusion episodes caused different faults that took place after cratonization until the present. There are three generations of folds during ductile deformation (E1 and E2). The F2 folds are nearly coaxial (along ENE–WSW trend) with the F1 folds. The F3 folding is displayed by folds generally trending NNW–SSE. Therefore, the ENE–WSW and NNW–SSE trends can considered as preexisting discontinuities and mechanical anisotropy of the crust in the following structure episodes. Brittle deformation (E3 and E4) reveals the importance of those trends which control the multi-injections and many alteration features in the study area. During reactivation, a simple shear parallel to the inherited ductile fabrics was responsible for the development of mineralized structures along the ENE–WSW and NNW–SSE trends. So they can be considered as paleochannel trends for deep-seated structures and can act as a good trap for uranium and/or other mineral resources. Most of the uranium anomalies are delineated along ENE–WSW and NNW–SSE shear zones where quartz-bearing veins bounded the lamprophyre dike and microgranites and dissected them in relation to the successive fracturation and brecciation corresponding to the repeated rejuvenation of the structures. Therefore, the structural controls of the uranium mineralizations in the El Sela area appear to be related to the interaction between inherited ductile fabrics and overprinting brittle structures.  相似文献   

17.
Peat cores provide decadal to centennial records of climatic and environmental change, including evidence for human/environment interaction. Existing palaeoenvironmental proxies (macrofossils, pollen, humification, testate amoebae, lipid composition) require multiple laboratory preparation steps and may be subject to differential preservation that can limit production of a continuous time series. The potential for pyrolysis gas-chromatography-mass-spectrometry (Py-GC-MS) to be applied to bulk peat samples is investigated here. The only preparatory step required was freeze drying. Analysis of a range of important peat-forming plants demonstrates that Sphagnum moss species are unique in containing the pyrolysis product of sphagnum acid, 4-isopropenylphenol. In contrast, non-Sphagnum species are rich in lignin pyrolysis products, which are absent from Sphagnum. The presence of these pyrolysis markers is reflected in bulk peat composition and tested here using archives from Bolton Fell Moss and Butterburn Flow (UK), Kontolanrahka (Finland) and Bissendorfer Moor (Germany). A ratio between 4-isopropenylphenol and two lignin pyrolysis products is proposed as a proxy for total Sphagnum input to peat archives and shows potential for use as a rapid screening tool for characterising bulk peat composition before more intensive analysis.  相似文献   

18.
Analysis of the C, N, and Xe release kinetics of intermediate-sized nanodiamond fraction from the Orgueil CI meteorite during isothermal pyrolysis conducted for the first time and subsequent oxidation indicates that (a) the rate of C, N, and Xe release at pyrolysis at a constant temperature decreases with time; (b) the relative amount of released Xe, which mostly has a normal isotopic composition (Xe-P3) at various pyrolysis time up to 800°C, is controlled, first of all, by the heating temperature, whereas the amount of N is controlled by both the temperature and heating time; and (c) prolonged pyrolysis notably modifies the distribution of nitrogen of normal (δ15N = 0) and anomalous (δ15N= ?350‰) isotopic composition in diamond grains. The identified features of the C and N release kinetics are explained by differences in the binding energy of chemically adsorbed O with C atoms and the accommodation of the main amounts of N in extended defects of the crystal structure of nanodiamond. The major factors of the decrease in the Xe-P3 release rate during the isothermal pyrolysis of nanodiamond are either the differences between the Xe desorption parameters of the traps in graphite-like phases containing Xe-P3 or the differences between the radiation-induced defectiveness of grains of the population containing implanted Xe-P3. Our results led us to conclude that (1) meteoritic nanodiamond contains relatively low amounts of a phases carrying the P3 component of noble gases, regardless of the nature of this component, and (2) the population of nanodiamond grains containing most of isotopically anomalous nitrogen was produced at a high rate to preserve this nitrogen, first of all, at extended defects in the diamond crystal structure.  相似文献   

19.
The terpenoid composition of fossil resin from the Cape York Peninsula, Australia has been analysed by pyrolysis-gas chromatography-mass spectrometry (Py-GC-MS) to determine its origin. The pyrolysis products were dominated by cadalene-based C15 bicyclic sesquiterpenoids including some C30–C31 bicadinanes and bicadinenes typical of Class II resin derived from angiosperm plants of Dipterocarpaceae. This observation contrasts with the Araucariaceae (Agathis sp.) source previously suggested for the resin based on Fourier transform infrared (FTIR) analyses. Dipterocarpaceae are not known in Australian vegetation but grow abundantly in Southeast Asia including New Guinea, indicating that the geological origin of the amber is not the Australian mainland but could be traced to Southeast Asia.  相似文献   

20.
This study has characterised the oxidation products of a fine-grained single domain magnetite which was made synthetically by a colloidal method. Changes in the intrinsic magnetic properties (saturation magnetisation, saturation remanence, and coercive force) during progressive oxidation are correlated with lattice parameter changes and an oxidation mechanism. It is proposed that magnetite oxidises to hematite via at least two metastable maghemites. The first of these, formed on low temperature oxidation by the formation of a magnetite/maghemite solid solution, is a face centered maghemite with lattice parameter a= 8.3419±0.0006 Å. A second maghemite, produced on oxidation at higher temperatures, has a primitive cubic structure and a lattice parameter a = 8.3505±0.0005 Å. Maghemite cation distributions are derived to explain the reduced saturation magnetisations of between 56 and 74 Am2 kg-1 observed, and a maghemite structure containing an increase in tetrahedral Fe3+ ions and up to 3 octahedral vacancies per 32 oxygen unit cell is proposed.  相似文献   

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