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1.
An integration of methods to quantify the surface area of porous solid materials with a broad span of spatial resolution is presented. The application of it is to detect and quantify the rock surface area modifications caused by fluid-rock interactions on different scales from several nanometres to metres. The new approach is to study the fluid-accessible surface area of rock fragments during dissolution processes.In this paper, diverse methods for surface quantification at different levels of surface detail were adapted for the application of rock surface quantification and porosimetry measurements. The geometric external surface area of rock fragments can be determined by paraffin wax coating and, in special cases, by parallelepiped surface estimations. This geometrical surface area of rock polyhedrons is equal to the macroscopic bounding surface area of a rock volume. Representative surface details on the scale of micrometres to millimetres on geometrical surface area can be quantified by mechanical roughness analyses. The resultant roughness factors are compared to optical roughness quantifications by confocal laser scanning microscopy and white light interferometry and can indicate modifications of the pore space up to several hundred nanometres. The comparison of rock pore space data, measured by both mercury intrusion porosimetry and nitrogen adsorption, quantifies the surface area of pores with a diameter of approximately 2 nm.These various surface data at different levels of detail were integrated to get an estimation of this surface area, which affects fluid-rock interactions. The proposed concept has the potential to trace the multi-scale rock surface area evolution in response to fluid-rock interaction processes.The importance of this concept is its application beyond the laboratory survey. For example, additionally to their specific surface area, the reactive surface area of rock particles in a mining dump is controlled by geometrical size and surface roughness of particles.  相似文献   

2.
Different from previous studies on effect of weathering upon geochemical variation along a single weathered profile, this paper provides a new methodology validated by comparing a weathered outcrop samples and their stratigraphic counterpart un-weathered core samples in a nearby shallow borehole. This outcrop and borehole penetrated the Ordovician-Silurian Wufeng–Longmaxi shales, located in the same anticline structure in the northern part of Guizhou Province, Southern China. The mineral composition, major, trace and rare earth elements (REEs) composition and Rock-Eval parameters of outcrop and core samples were analyzed and compared. Organic matter (OM) was observed in the microscope and extracted for elements analysis. The results show that short-term weathering still has significant influence on OM, mineral and elemental composition of black shales. The elements composition shows the outcrop profile was moderately weathered. The REEs compositions do not alter much during weathering process and the REEs composition and their relative ratios still are valid for rock origin determination. The OM, mainly composed by graptolite and bitumen, even entering the highly-over thermal maturity, is still sensitive to the weathering with a systematic loss 30–50% of TOC along the outcrop profile, which suggests that the OM consumption is predominantly controlled by weathering duration and the distance from the weathering surface. In turn, OM has significant influence on the trace elements transportation behavior during weathering. Some trace elements associated with the OM such as V, Cr, Th, U, Ni and Co, change significantly in their absolute concentration during weathering, but their relative ratios do not necessarily change too much and might be still reliable proxies for paleo-environmental determination. The mobility of shale minerals during weathering is in the following order: plagioclase?>?potassium feldspar and dolomite >pyrite and OM. Short-term weathering can also result in considerable transportation of elements and significant variation of minerals content in black shale, which may pose potentially high environmental and engineering risk in the regions rich in black shale.  相似文献   

3.
We explored changes in the relative importance of carbonate vs. silicate weathering as a function of landscape surface age by examining the Ca/Sr and Sr isotope systematics of a glacial soil chronosequence located in the Raikhot watershed within the Himalaya of northern Pakistan. Bedrock in the Raikhot watershed primarily consists of silicate rock (Ca/Sr ≈ 0.20 μmol/nmol, 87Sr/86Sr ≈ 0.77 to 1.2) with minor amounts of disseminated calcite (Ca/Sr ≈ 0.98 to 5.3 μmol/nmol, 87Sr/86Sr ≈ 0.79 to 0.93) and metasedimentary carbonate (Ca/Sr ≈ 1.0 to 2.8 μmol/nmol, 87Sr/86Sr ≈ 0.72 to 0.82). Analysis of the exchangeable, carbonate, and silicate fractions of seven soil profiles ranging in age from ∼0.5 to ∼55 kyr revealed that carbonate dissolution provides more than ∼90% of the weathering-derived Ca and Sr for at least 55 kyr after the exposure of rock surfaces, even though carbonate represents only ∼1.0 wt% of fresh glacial till. The accumulation of carbonate-bearing dust deposited on the surfaces of older landforms partly sustains the longevity of the carbonate weathering flux. As the average landscape surface age in the Raikhot watershed increases, the Ca/Sr and 87Sr/86Sr ratios released by carbonate weathering decrease from ∼3.6 to ∼0.20 μmol/nmol and ∼0.84 to ∼0.72, respectively. The transition from high to low Ca/Sr ratios during weathering appears to reflect the greater solubility of high Ca/Sr ratio carbonate relative to low Ca/Sr ratio carbonate. These findings suggest that carbonate weathering controls the dissolved flux of Sr emanating from stable Himalayan landforms comprising mixed silicate and carbonate rock for tens of thousands of years after the mechanical exposure of rock surfaces to the weathering environment.  相似文献   

4.
Re-Os analyses were performed on five soil profiles developed on silicate lithologies in the Narayani drainage basin of the Himalayas, as well as on several altered black shales and associated alteration phases. The results indicate that all of these samples have lost large amounts of Re. This Re loss approached 100% in the black shale-derived soils, which also most probably lost substantial quantities of Os. The near constancy of Os and Re concentrations with depth indicates that this loss occurred quite early in the alteration process, rather than progressively during the course of soil development. A slight decrease in 187Os/188Os was observed toward the surface of the two black shale soil profiles, possibly indicating a minor preferential mobility of radiogenic 187Os for this lithology. In the black shale-derived saprolite and soils, the loss of Re and Os was related to the loss of organic carbon. The importance of this phase is underscored by the fact that organic material separated from a black shale sample accounted for nearly all of the Os contained in the whole rock. Analysis of alteration phases from the surface of a weathered black shale showed that Os liberated during alteration was partially reprecipitated in Fe oxides, with Os isotopic compositions very similar to that of the original rock, whereas Re was removed with the fluid phase.These results demonstrate the disproportionately large role that black shale weathering may play in determining the Re and Os contents of continental runoff and, thus, ultimately of seawater, but they also emphasize the possible complexity of this process. The data suggest that a large fraction of the Os contained in black shales is released during chemical alteration, which is apparently not the case for most other silicate rocks. Therefore, the potential contribution of black shales to the dissolved Os budget of runoff and river water may be even greater than that expected from the high Os concentrations of these rocks. The extent to which this Os will affect the seawater Os composition depends on how efficiently it is recaptured by secondary phases such as Fe-Mn oxides in situ or during transport. These results also underscore the high mobility of Re with respect to Os at every stage in the erosional process, thus explaining the order of magnitude increase in Re/Os ratio from the black shale source rocks to seawater.  相似文献   

5.
Reactive surface area is one of the key parameters for studying the kinetics of mineral dissolution. The common practice in experimental kinetics is to normalize the dissolution rate to the surface area measured by the BET method. The relationship between BET surface area and the reactive surface area is not trivial in minerals such as smectites, which possess both internal and external surface areas, and in which the dissolution is controlled by the chemical attack on the edge surface. The present study examines two proxies for the reactive surface area of the Clay Mineral Society reference smectite SAz-1: BET surface area and the edge surface area measured using AFM.Since smectites are very microporous, their BET surface area is strongly influenced by the degassing procedure. It is demonstrated that outgassing the smectite powder at 135°C in a 15 mL min−1 N2 gas flow for at least 24 hours minimizes contribution from micropores to less than 11% of the BET surface area.Following dissolution experiments in solutions with a low electrolyte concentration, the BET surface area increased from 34 ± 2 m2 g−1 in raw SAz-1 to 127 ± 13 m2 g−1 in SAz-1 sample recovered from dissolution experiments. This increase in BET surface area is explained by a decrease in the average size of the smectite aggregates, and by an increase in microporosity due to the depletion in the major interlayer cation, i.e., Ca2+. As the BET surface area of the raw smectite sample includes considerably less microporosity compared to the BET surface area of the smectite recovered from dissolution experiments, the former is a better approximation of the external surface area of the dried sample powder.AFM measurements show that there is no correlation between the specific external surface area of the sample and its specific edge surface area. This observation is explained by the platy morphology of the smectite particle in which the specific external surface area depends linearly on the height reciprocal, whereas the specific edge surface area is independent of the particles height and depends linearly on the sum of the reciprocals of the length of the axes. Therefore, there is no reason to expect a correlation between the BET and the edge surface area. Our results show that the edge surface area (4.9 ± 0.7 m2 g−1) of the smectite particles cannot be predicted based on its external surface area (136 ± 20 m2 g−1). Therefore, the BET surface area cannot serve as a proxy for the reactive surface area. We suggest using AFM measurements of the specific edge surface area as an alternative proxy for the reactive surface area of smectite.  相似文献   

6.
Subaerial exposure and oxidation of organic carbon (Corg)-rich rocks is believed to be a key mechanism for the recycling of buried C and S back to Earth's surface. Importantly, processes coupled to microbial Corg oxidation are expected to shift new biomass δ13Corg composition towards more negative values relative to source. However, there is scarcity of information directly relating rock chemistry to oxidative weathering and shifting δ13Corg at the rock-atmosphere interface. This is particularly pertinent to the sulfidic, Corg-rich alum shale units of the Baltoscandian Basin believed to constitute a strong source of metal contaminants to the natural environment, following subaerial exposure and weathering. Consistent with independent support, we show that atmospheric oxidation of the sulfidic, Corg-rich alum shale sequence of the Cambrian-Devonian Baltoscandian Basin induces intense acid rock drainage at the expense of progressive oxidation of Fe sulfides. Sulfide oxidation takes priority over microbial organic matter decomposition, enabling quantitative massive erosion of Corg without producing a δ13C shift between acid rock drainage precipitates and shale. Moreover, 13C enrichment in inorganic carbon of precipitates does not support microbial Corg oxidation as the predominant mechanism of rock weathering upon exposure. Instead, a Δ34S = δ34Sshale − δ34Sprecipitates ≈ 0, accompanied by elevated S levels and the ubiquitous deposition of acid rock drainage sulfate minerals in deposited efflorescent precipitates relative to shales, provide strong evidence for quantitative mass oxidation of shale sulfide minerals as the source of acidity for chemical weathering. Slight δ15N depletion in the new surface precipitates relative to shale, coincides with dramatic loss of N from shales. Collectively, the results point to pyrite oxidation as a major driver of alum black shale weathering at the rock-atmosphere interface, indicating that quantitative mass release of Corg, N, S, and key metals to the environment is a response to intense sulfide oxidation. Consequently, large-scale acidic weathering of the sulfide-rich alum shale units is suggested to influence the fate and redistribution of the isotopes of C, N, and S from shale to the immediate environment.  相似文献   

7.
近年来的研究证明,中新生代未熟—低熟海相富有机质泥质烃源岩中有机质是通过溶解在水中的分子规模的碳有机质以化学吸附的形式被吸附到矿物表面上和蒙脱石结构层内。然而,对于高熟海相泥质烃源岩中有机质的赋存状态却少有报道。通过对塔里木盆地下寒统底部高熟海相泥质烃源岩的有机碳含量、矿物表面积、扫描电镜和透射电镜的综合分析,得到了其有机质以细小的颗粒状保存于沉积物颗粒之间的结论。同时,通过高熟海相烃源岩与现代未熟海相烃源岩有机质赋存状态的对比,提出了值得进一步研究的有关科学问题。  相似文献   

8.
锑属亲铜元素,易与硫结合。锑在地核(0. 14×10~(-6))、地幔(0. 006×10~(-6))和地壳(0. 02×10~(-6))中的丰度均很低,而在黑色页岩(5. 0×10~(-6))中明显富集。锑是一种典型的低温成矿元素。我国华南地区低温成矿域拥有世界60%的锑探明储量。研究结果显示锑的成矿主要经历两阶段富集过程:一是与风化和沉积作用有关的表生过程;二是地球内部热驱动过程。寒武纪时华南位于赤道附近,受冈瓦纳大陆的造山带的影响,是全球地表风化最强烈的地区之一。在新元古代氧化事件的驱动下,锑在表生风化过程中被氧化为更易迁移的水溶性的SbO_3~-。因埃迪卡拉生物群所产生的有机质,有利于萃取水体中的锑并沉淀在还原性沉积物(黑色页岩)中。华南中生代岩浆活动烘烤表层富锑的寒武纪黑色页岩,产生的成矿流体向上迁移,淋滤黑色页岩中的Sb或与黑色页岩变质脱水或熔融产生成矿流体混合;而后搬运至远离岩体的有利位置沉淀,最终形成大规模的华南锑矿带。  相似文献   

9.
Hydraulic fracturing is an important technological advance in the extraction of natural gas and petroleum from black shales, but water injected into shale formations in the fracturing process returns with extraordinarily high total-dissolved-solids (TDS) and high concentrations of barium, Ba. It is generally assumed that high TDS comes from the mixing of surface water (injected fluid) with Na–Ca–Cl formation brines containing elevated Ba, but the mechanisms by which such mixing might occur are disputed. Here we show that Ba in water co-produced with gas could originate from water-rock reactions, with Ba levels observed in produced waters reached on a time scale relevant to hydraulic fracturing operations. We examined samples from three drill cores from the Marcellus Shale in Pennsylvania and New York to determine the possible water-rock reactions that release barium during hydraulic fracturing. Two samples, one containing microcrystalline barite (BaSO4) and one without barite, contain elevated concentrations of Ba relative to the crustal average for shale rocks. A third sample is slightly depleted in Ba relative to the crustal average. Micro-XRF measurements and SEM/EDS analysis combined with chemical sequential extraction methods reveal that a majority of the Ba in all samples (55–77 wt.%) is present in clays and can only be leached from the rock by dissolution in hydrofluoric acid. Thus, a majority of barium in our samples is relatively inaccessible to leaching under hydraulic fracturing conditions. However, the balance of Ba in the rocks is contained in phases that are potentially leachable during hydraulic fracturing (e.g., soluble salts, exchangeable sites on clays, carbonates, barite, organics).We next studied how shale reacts with water at elevated temperatures (80 °C), low Eh (−100 to −200 mV), and a range of ionic strengths (IS = 0.85–6.4) that emulate conditions prevalent at depth during hydraulic fracturing. Our experimental results indicate that the amount of Ba released from the bulk rock has a positive correlation with the ionic strength of the reacting fluid. Between 5 and 25% of the total Ba in the rock can be leached from shale under ionic strength conditions and leachate compositions typical of produced waters over a contact time of just 7 days. We suggest that reductive weathering of black shale occurs during hydraulic fracturing due to: 1) Ba2+ in clays exchanging with Na+ and Ca2+ ions that are present in high concentrations in produced water, and 2) increased solubility and dissolution kinetics of barite under high ionic strength conditions. At the low Eh conditions prevalent during hydraulic fracturing the sulfate deficient water allows Ba to be dissolved into the produced water. Based on Ba yields determined from laboratory leaching experiments of Marcellus Shale and a reasonable estimate of the water/rock mass ratio during hydraulic fracturing, we suggest that all of the Ba in produced water can be reconciled with leaching directly from the fractured rock.  相似文献   

10.
Apatite dissolution experiments were conducted using both a fluidized bed and stirred tank reactor over a range of pH, temperature, solution saturation state, and on non-carbonated and carbonated apatite compositions: igneous fluorapatite (FAP) and sedimentary carbonate fluorapatite (CFA), respectively. From 2 <pH <6, the rate of release from dissolution of all apatite components [calcium (Ca), phosphorus (P), and fluoride (F)] increased with decreasing pH for FAP. From 6 < pH < 8.5, the FAP dissolution rate is pH independent. Measuring apatite dissolution rates at pH > 8.5 were not possible due to detection limits of the analytical techniques used in this study and the high insolubility of FAP. For the CFA compositions studied, the dissolution rate decreased with increasing pH from 4 < pH < 7. During early stages of the dissolution reaction for both FAP and CFA, mineral components were released in non-stoichiometric ratios with reacted solution ratios of dissolved Ca:P and Ca:F being greater than mineral stoichiometric ratios, suggesting that Ca was preferentially released compared to P and F from the mineral structure during the early stages of dissolution. An increase in reacted solution pH accompanies this early elevated release of Ca. As the dissolution reaction proceeded to steady state, dissolution became congruent. When normalized to BET measured surface area, FAP dissolved faster from 4 < pH < 7 compared to CFA. The apparent Arrhenius activation energy (Ea) of FAP dissolution over the temperature range of 25-55°C at pH = 3.0, I = 0.1, and pCO2 = 0 is 8.3 ± 0.2 kcal mol−1. Both the apparent exchange of solution H+ for solid-bound Ca at low pH in the early stage of dissolution and the Ea of dissolution suggest a surface and not a diffusion controlled dissolution reaction for FAP and CFA. The degree of undersaturation of the solution, ΔGR, with respect to FAP was important in determining the dissolution rate. At pH = 3.0, I = 0.1, and pCO2 = 0, the dissolution rate of FAP was ∼ 5× greater in the far-from-equilibrium region compared to the near-equilibrium slope region.A simple apatite weathering model incorporating the experimental results from this study was constructed, and numerical calculations suggest that during the Phanerozoic both the surface area of igneous rock available for weathering and the average global temperature were important factors in determining the P weathering flux from apatite dissolution. It is possible that elevated global temperatures coupled with relatively high surface area of igneous rock during the early- to mid-Paleozoic resulted in elevated P weathering fluxes, which along with climatic evolutionary pressures of the Neoproterozoic, facilitated the radiation of multicellular organisms, large-scale phosphorite deposition, and abundance of calcium phosphate shelled organisms during the early Cambrian.  相似文献   

11.
Four porous, glass-dominated rhyolites from Kozushima Island, different in age and extent of weathering, were studied. Because the four rhyolites are homogeneously weathered to considerable depth, and because their initial chemical compositions were equal, the different rock characteristics can provide information about rates of rhyolite dissolution and clay mineral formation over ∼52,000 yr. Because glass surfaces retreat without surface roughening, surface area (measured by Brunauer-Emmett-Teller method; BET) was assumed to be approximately constant over time. The field dissolution rate, as inferred from the rate of loss of Si, was ∼6 × 10−19 mol cm−2 s−1. The estimated clay mineral formation rate was ∼1 × 10−19 mol cm−2 s−1. About 20% of dissolved Si precipitated as clays. In order to investigate the factors affecting the field dissolution rate, dissolution experiments that used powdered and block rhyolite samples were conducted. Under relevant field conditions (20°C and pH 6∼7), the rates were ∼5 × 10−17 and ∼5 × 10−18 mol cm−2 s−1 for powdered rhyolite and blocks, respectively. The dissolution rates obtained in this study decrease in the order powder > block > field. Because all surface areas were directly measured by BET, the differences are not attributable to the errors in surface area. The most plausible explanations of the slower rates are the lower degree of flushing and resultant high-solution saturation states in the pores (both in the field and in the rhyolite blocks used in experiments) plus the formation of alteration/hydrated layers at the glass surface.  相似文献   

12.
The paucity of weathering rates for quartz in the natural environment stems both from the slow rate at which quartz dissolves and the difficulty in differentiating solute Si contributed by quartz from that derived from other silicate minerals. This study, a first effort in quantifying natural rates of quartz dissolution, takes advantage of extremely rapid tropical weathering, simple regolith mineralogy, and detailed information on hydrologic and chemical transport. Quartz abundances and grain sizes are relatively constant with depth in a thick saprolite. Limited quartz dissolution is indicated by solution rounding of primary angularity and by the formation of etch pits. A low correlation of surface area (0.14 and 0.42 m2 g−1) with grain size indicates that internal microfractures and pitting are the principal contributors to total surface area.Pore water silica concentration increases linearly with depth. On a molar basis, between one and three quarters of pore water silica is derived from quartz with the remainder contributed from biotite weathering. Average solute Si remains thermodynamically undersaturated with respect to recently revised estimates of quartz solubility (<180 μM) but exceeds estimated critical saturation concentrations controlling the initiation of etch pit formation (>17–81 μM). Etch pitting is more abundant on grains in the upper saprolite and is associated with pore waters lower in dissolved silica. Rate constants describing quartz dissolution increase with decreasing depth (from 10−14.5–10−15.1 mol m−2 s−1), which correlate with both greater thermodynamic undersaturation and increasing etch pit densities. Unlike for many aluminosilicates, the calculated natural weathering rates of quartz fall slightly below the rate constants previously reported for experimental studies (10−12.4–10−14.2 mol m−2 s−1). This agreement reflects the structural simplicity of quartz, dilute solutes, and near-hydrologic saturation.  相似文献   

13.
我国南方岩溶区和北方黄土区的大气CO2效应   总被引：18，自引：0，他引：18       下载免费PDF全文
我国南方岩溶区与北方黄土区都是巨大的碳库。碳酸盐的溶蚀及再结晶是两个碳库与大气ＣＯ２交换的重要过程。碳的区域平衡是评价化学风化消耗或逸散ＣＯ２的基础。岩溶区与黄土区在地球化学风化的环境背景、溶蚀过程、产物运移和归宿等差异很大。黄土区化学风化消耗大气ＣＯ２通量较岩溶区小。目前评价两类地区土壤与大气ＣＯ２的源汇关系尚不成熟,需要定量认识土壤ＣＯ２与下伏碳酸盐岩溶蚀或与下伏黄土次生碳酸盐化作用。岩溶区湖泊沉积物中有机质分解产生的ＨＣＯ３－制约外源及内生碳酸盐溶解和自生碳酸盐形成。  相似文献   

14.
It has commonly been assumed that the weathering rates of feldspars are proportional to their exposed surface areas. However, weathering does not affect the whole surface of a grain uniformily; preferential dissolution occurs at highly localized sites, which are determined by the location of crystalline defects. To examine the importance of reactions at these sites relative to those occurring on bulk surfaces, we compared the rates of dissolution of 5 different size fractions of an alkali feldspar, whose specific surface areas (m2/g) spanned a range of a factor of twenty.At any given pH value, the bulk dissolution rates (moles/g/h) for the five fractions varied by less than a factor of two. The results suggest that reactions at crystalline defects dominate weathering processes during the early stages of dissolution. Furthermore, the exposure of these defects is not simply or easily related to total surface area. These findings strongly suggest that care must be taken to distinguish between the surface reaction controlled mechanism and a surface area controlled model which is frequently—and incorrectly—assumed to be equivalent. The data presented here are consistent with the former mechanism but strongly dispute the latter.  相似文献   

15.
铀的地球化学性质与成矿——以华南铀成矿省为例   总被引：1，自引：1，他引：1  
铀是强不相容元素,随着岩浆演化而不断富集,在岩浆演化末期受结构氧增加影响进入独居石、磷钇矿等副矿物中。岩浆演化通常无法直接形成达到工业品位的铀矿床。铀是对氧逸度敏感的变价元素。在表生风化过程中岩体(层)中的铀被氧化为UO_2~(2+)而极易溶解进入水体中,并可在还原环境沉淀而富集成矿,氧化还原界面是找矿的理想选区。大气水可通过断裂构造系统进入一定深度,并受热源作用形成高氧逸度的热液而萃取出岩体(层)中的铀在还原位置沉淀富集形成矿床。新元古代氧化事件以及Marinoan冰期结束使得表生风化过程中更多的U进入水体;而寒武纪生命大爆发,易在沉积盆地底部形成还原环境,有利于U的沉淀富集。受上述三方面因素控制,在华南形成了广泛分布的富铀黑色页岩层,并被之后的沉积物覆盖,成为华南各型铀矿床的铀源层。印支期构造运动使部分富铀黑色页岩层发生部分熔融形成了富铀的S型花岗岩,该类岩石亦是之后铀成矿作用的铀源岩。燕山运动后期华南发生伸展构造背景下的岩浆热事件为以大气水为主的高氧逸度热液的形成并作用于铀源岩(层)提供了有利条件,促使华南各类型铀矿床开始在白垩纪集中形成。  相似文献   

16.
近年来发现黔南地区下石炭统打屋坝组发育厚度较大的黑色页岩层,该地层已经成为黔南地区重要的页岩气目标地层。为进一步了解该地层的页岩气参数,评价其页岩气勘探潜力,对代页1井打屋坝组黑色页岩进行观察和取样分析,显示该井打屋坝组黑色页岩钻厚为80 m,总体为一套深水陆棚相沉积; 干酪根显微组分以腐泥组、壳质组和镜质组为主,Ⅰ型-Ⅲ型干酪根均有发育,有机碳(TOC)含量主要分布在1.5%3.3%之间,镜质体反射率(Ro)为2.15%2.66%; 矿物组成以石英、黏土矿物为主,脆性矿物(不含方解石)含量在35%64%之间; 含气量在0.494.97 m3/t之间,平均为2.20 m3/t。通过露头剖面观察,显示黔南下石炭统打屋坝组黑色页岩厚度均较大,代页1井含气量较高,有机地化、储集物性参数较好,反映打屋坝组具有良好的勘探前景,可进一步加强该地层的基础地质、页岩储层改造和页岩气富集规律研究工作。  相似文献   

17.
The effect of lattice disorder and mineral surface area on the reactivity of finely ground fluorite was studied on ball-milled powders. Structural information was provided by X-ray whole powder pattern modeling (WPPM). The mean size of coherent scattering domains decreases with milling time from 70 nm to ∼20 nm, whereas the density of lattice defects increases with both time and intensity of milling treatment, from 4 × 1015 m-2 to 24 × 1015 m-2. High resolution transmission electron microscopy (HRTEM) of ground fluorite grains shows several line defects and a general tendency of nanometric crystalline domains to agglomerate in larger grains.Solution chemistry was investigated using batch reactors with free drift of solution saturation state with respect to fluorite. Total surface area was measured by the Brunaver, Emmet and Teller (BET) method, and dissolution rates were measured at pH = 2 (HCl) and T = 295 K. In far from equilibrium conditions, dissolution rates normalized by BET area do not increase with the dislocation density. In near-equilibrium condition, however, measured stationary ionic product clearly increases with both time and intensity of milling treatment. Thermodynamic predictions of the solubility constant indicate negligible or little effect of total surface area. Consequently, the observed increase in the stationary ionic product can be related to the increasing lattice defect content. This confirms the significant role of dislocation outcrops on mineral dissolution in close to equilibrium conditions.  相似文献   

18.
《Applied Geochemistry》1994,9(5):583-595
A steady-state geochemical model has been developed to study water-rock interactions controlling metal release from waste rock heaps at the Aitik Cu mine in northern Sweden. The Cu release in drainage waters from the site is of environmental concern. The waste rock heaps are treated as single completely mixed flow-through reactors. The geochemical model includes kinetices of sulphide and primary silicate mineral weathering, heterogeneous equilibrium with secondary mineral phases and speciation equilibrium. Field monitoring of drainage water composition provides a basis for evaluation of model performance.The relative rate of oxidative weathering of sulphides and dissolution of primary silicate minerals, using published kinetic data, are consistent with net proton and base cation fluxes at the site. The overall rate of Fe2+ oxidation within the heap is three orders of magnitude faster than that which could be explained by surface-catalysed reaction kinetics. This suggests significant activity of iron-oxidizing bacteria. The absolute weathering rates of sulphides and silicate minerals, normalized to a measured BET surface area, are approximately two orders of magnitude lower at field scale than published rates from laboratory experiments. Because of the relative absence of carbonate minerals, the weathering of biotite and plagioclase feldspar are important sources of alkalinity.  相似文献   

19.
Building stones manufactured from contact metamorphic slates (Fruchtschiefer slate) from Theuma (Sachsen, Germany) were investigated for mineralogical alterations as well as for changes in porosity and surface roughness due to weathering. After weathering periods of several years to decades, the originally dark gray-colored slates show pale spots of several centimeters in size at the surface of building stones. The dark-colored and light-colored sections of the slate show no differences in mineralogy. Surface weathering did not result in newly precipitated minerals. It was also found that the observed differences in color are not caused by variations in sedimentary organic carbon concentration or in sulfide/sulfate concentrations. Obtained results instead indicate that dark surface sections may show a thin cover of recent organic matter (OM), e.g., living OM, soot, dirt, etc. Microscopic investigations suggested that this cover was exfoliated at light-colored surface sections. The observed disaggregation of the upper 2 mm of the building block material results in an increase in porosity. Porosity of black (unweathered) slate is <2 vol.%. Due to weathering, the slate’s pores with diameters >1 μm show a significant increase in frequency compared to the original pore size distribution. Porosity of weathered rock volumes increased to approx. 8 vol.%. Discolored surface sections show a higher surface roughness (root-mean-square roughness, Rq ~ 1 μm) compared to dark-colored slate surfaces (Rq ~ 200 nm), both data are for cleavage planes. Preferentially, the discolored surface sections are located close to the edges of cut stones. This and the alteration in porosity, pore size, and surface roughness indicate that color changes of the slate are largely influenced by rock disaggregation proceeding from the edges into the center rather than by mineral dissolution/precipitation processes.  相似文献   

20.
Volcanic areas play a key role in the input of elements into the ocean and in the regulation of the geological carbon cycle. The aim of this study is to investigate the budget of silicate weathering in an active volcanic area. We compared the fluxes of the two major weathering regimes occurring at low temperature in soils and at high temperature in the active volcanic arc of Kamchatka, respectively. The volcanic activity, by inducing geothermal circulation and releasing gases to the surface, produces extreme conditions in which intense water-rock interactions occur and may have a strong impact on the weathering budgets. Our results show that the chemical composition of the Kamchatka river water is controlled by surface low-temperature weathering, atmospheric input and, in some limited cases, strongly imprinted by high-temperature water-rock reactions. We have determined the contribution of each source and calculated the rates of CO2 consumption and chemical weathering resulting from low and high-temperature water/rock interactions. The weathering rates (between 7 and 13.7 t/km2/yr for cations only) and atmospheric CO2 consumption rates (∼0.33-0.46 × 106 mol/km2/yr for Kamchatka River) due to rock weathering in soils (low-temperature) are entirely consistent with the previously published global weathering laws relating weathering rates of basalts with runoff and temperature. In the Kamchatka River, CO2 consumption derived from hydrothermal activity represents about 11% of the total HCO3 flux exported by the river. The high-temperature weathering process explains 25% of the total cationic weathering rate in the Kamchatka River. Although in the rivers non-affected by hydrothermal activity, the main weathering agent is carbonic acid (reflected in the abundance of in rivers), in the region most impacted by hydrothermalism, the protons responsible for minerals dissolution are provided not only by carbonic acid, but also by sulphuric and hydrochloric acid. A clear increase of weathering rates in rivers impacted by sulphuric acid can be observed. In the Kamchatka River, 19% of cations are released by hydrothermal acids or the oxidative weathering of sulphur minerals.Our results emphasise the important impact of both low and high-temperature weathering of volcanic rocks on global weathering fluxes to the ocean. Our results also show that besides carbonic acid derived from atmospheric CO2, hydrochloric acid and especially sulphuric acid are important weathering agents. Clearly, sulphuric acid, with hydrothermal activity, are key parameters that cause first-order increases of the chemical weathering rates in volcanic areas. In these areas, accurate determination of weathering budgets in volcanic area will require to better quantify sulphuric acid impact.  相似文献   

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