东濮凹陷文留地区深层强超压环境下有机质热演化

东濮凹陷文留地区的地层普遍发育超压甚至强超压系统.超压与地层有机质热演化反应过程存在复杂的相关性.深层盐下、盐间地层有机质的热演化受强超压的影响,不同热演化反应过程不同程度地受到抑制作用:镜质体反射率演化正常;烃类裂解以及烃类结构演化在深层强超压作用下受到抑制作用.有机质热演化过程中的超压抑制为深层源岩成烃提供了更为有利的条件,是文留地区深层天然气成藏的主要因素.     

Smectite-Zeolite Envelope Surrounding the Tsukiyoshi Uranium Deposit, Central Japan: A Natural Analogue Study

Abstract. The Tsukiyoshi uranium deposit in Gifu Prefecture is the largest one in Japan. It is embedded in lower part of the Mizunami Group of Miocene age. Relating to the existence of this uranium deposit, the constituent minerals in sediments were studied by XRD and SEM, using many drilling cores. The most abundant authigenic mineral is smectite. The amount of smectite increases generally from upper to lower horizons, and a highly smectitized zone is situated around the uranium deposit. Smectitization predominated in mafic glassy grains of sediments, which was probably formed in early burial diagenesis. Zeolites including clinoptilolite-heulandite, mordenite, analcime, chabazite and philipsite are secondly abundant authigenic minerals. They seem to have been formed at early to late diagenetic stages. Opaline silica is rather rare. Carbonate minerals, including cal-cite, dolomite, siderite and rhodochrosite are common. They may be formed by diagenesis as well. Gypsum and pyrite occur in upper horizons and lower horizons, respectively. In particular, a highly smectitized zone including pyrite probably played an important role for retarding the migration of uranium and as a result keeping the uranium deposit for past one million years. This smectite-zeolite envelope surrounding the Tsukiyoshi uranium deposit is regarded as a natural analogue of the buffer materials surrounding the high-level radioactive waste repository.     

未熟烃源岩中矿物低温催化脂肪酸脱羟生烃动力学模拟实验研究

在１５０～１６０℃和未熟烃源岩矿物的催化下,使十八烷酸脱羟生烃,用测定反应放出的ＣＯ２量随时间的变化关系直接研究了我国７个油田未熟烃源岩对脂肪酸催化脱羟生烃的动力学。由所得到的动力学参数与未熟烃源岩中碳酸盐含量的关联中发现,在低温、常压、无水条件下或低温、高压、碱性盐水条件下未熟烃源岩对脂肪酸催化脱羟生烃的动力学参数与其碳酸盐的含量有关,一般碳酸盐含量反应速率常数大,而反应活化能低。     

381溶浸场地地下水环境的复元研究

讨论了水环境复元的水一岩作用及其对水环境整治的正负影响。展示水文地球化学在水环境评价和整治工作中的不可忽略的作用和意义。在介绍溶浸场地水环境复原研究过程中，提出反映环境整治程度的参数，如清洗比、清除比和清洗程度等概念和求测计算方法。在地浸场地复原研究中，提出了采用冲洗清洗法与自然恢复相结合的方法，预计可以获得较佳效果。     

Numerical evaluation of multicomponent cation exchange reactive transport in physically and geochemically heterogeneous porous media

Experimental evidence and stochastic studies strongly show that the transport of reactive solutes in porous media is significantly influenced by heterogeneities in hydraulic conductivity, porosity, and sorption parameters. In this paper, we present Monte Carlo numerical simulations of multicomponent reactive transport involving competitive cation exchange reactions in a two-dimensional vertical physically and geochemically heterogeneous medium. Log hydraulic conductivity, log K, and log cation exchange capacity (log CEC) are assumed to be random Gaussian functions with spherical semivariograms. Random realizations of log K and log CEC are used as input data for the numerical simulation of multicomponent reactive transport with CORE^2D, a general purpose reactive transport code. Longitudinal features of the fronts of reactive and conservative species are computed from the temporal and spatial moments of depth-averaged concentrations. Monte Carlo simulations show that: (1) the displacement of reactive fronts increases with increasing variance of log K, while it decreases with the variance of log CEC; (2) second-order spatial moments increase with increasing variances of log K and log CEC; (3) uncertainties in the mean arrival time are largest (smallest) for negatively (positively) correlated log K and Log CEC; (4) cations undergoing competitive cation exchange exhibit different apparent velocities and retardation factors due to both physical and geochemical heterogeneities; and (5) the correlation between log K and log CEC affects significantly apparent cation retardation factors in heterogeneous aquifers.     

Degradation of phenol of high concentration by FeAIOx/MMT catalyzed Fenton reaction

以蒙脱土为载体制备负载型Fe/Al复合氧化物（FeAlOx/MMT）用于催化Fenton反应降解高浓度苯酚废水。实验结果表明,活性相FeAlOx中Fe/Al摩尔比为0.22时制备所得催化剂对Fenton反应具有最佳活性,且Fe/Al复合氧化物并未嵌入蒙脱土层间。在低温和高pH条件下催化体系存在诱导期,诱导期内FeAlOx/MMT缓释出Fe离子并进而由Fe离子催化溶液中的Fenton反应。通过对非均相催化降解苯酚废水的动力学研究发现,H2O2初始浓度、溶液的pH和反应温度对COD降解效率具有显著影响。调节降解过程中的温度序列和氧化剂引入程序能够缓解高温和高双氧水浓度双重因素耦合导致的HO.自消耗。在优化的降解条件下使用理论用量的H2O2可使得1 g/L的苯酚废水中苯酚降解率达到100%,而COD的降解率则达到97%。     

Geochemical characteristics and origin of light hydrocarbons in biogenic gas

The light hydrocarbon geochemical characteristics of biogenic gases from Sebei 1 gas field in the Qaidam Basin, Baoshan gas field in the Baoshan Basin and Alaxin gas field, Puqian gas pool, Aonan gas pool in the Songliao Basin are studied and the origin is discussed based on the composition and isotope data of gases. The isoalkane contents among light hydrocarbons in natural gas show a negative relationship with δ13C1 values. The isoalkane contents of the gases with δ13C1 values of less than ?60‰ are also h...     

Irreversible sorption of benzene in sandy aquifer materials

Hydrocarbon compounds in aquifers are generally known to show a retardation effect due to sorption onto the surfaces of solid particles. In this study, we investigated the effect of sorption on the transport of benzene in sandy aquifer materials by conducting batch and column tests for both sandy aquifer materials and sandy materials to which had been added 0·5% powdered activated carbon. The batch test was conducted by equilibrating dry materials with benzene solutions of various initial concentrations, and by analysing the concentrations of benzene in the initial and equilibrated solutions using high‐performance liquid chromatography (HPLC). The column test was performed to monitor the concentrations of effluent versus time, known as a breakthrough curve (BTC). We injected KCl and benzene solutions as tracers into the inlet boundary as two different types of square pulse and step, and monitored the effluent concentrations at the exit boundary under a steady‐state condition using an electrical conductivity meter and HPLC. Simulation of benzene transport was performed using the convective–dispersive equation model with the distribution coefficients obtained from the batch test and the transport parameters of the conservative solute KCl from the column test. The observed BTCs of KCl and benzene for pulse injection showed that the arrival times of the peaks of both tracers coincided well, but the relative peak concentration of benzene was much lower than that of KCl. Comparison of the simulated and observed BTCs showed a great discrepancy for all cases of injection mode and material texture, indicating the absence of retardation effect. These results reveal that the predominant process affecting the benzene transport in the sandy aquifer materials is an irreversible sorption rather than retardation. This tentative conclusion was verified by simulation of benzene transport using an irreversible sorption parameter that led to a good agreement between the simulated and observed BTCs. Copyright © 2002 John Wiley & Sons, Ltd.     

The role of Fischer-Tropsch catalysis in the origin of methane-rich Titan

Fischer-Tropsch catalysis, which converts CO and H₂ into CH₄ on the surface of iron catalyst, has been proposed to produce the CH₄ on Titan during its formation process in a circum-planetary subnebula. However, Fischer-Tropsch reaction rate under the conditions of subnebula have not been measured quantitatively yet. In this study, we conduct laboratory experiments to determine CH₄ formation rate and also conduct theoretical calculation of clathrate formation to clarify the significance of Fischer-Tropsch catalysis in a subnebula. Our experimental result indicates that the range of conditions where Fischer-Tropsch catalysis proceeds efficiently is narrow (T∼500-600 K) in a subnebula because the catalysts are poisoned at temperatures above 600 K under the condition of subnebula (i.e., H₂/CO = 1000). This suggests that an entire subnebula may not become rich in CH₄ but rather that only limited region of a subnebula may enriched in CH₄ (i.e., CH₄-rich band formation). Our experimental result also suggests that both CO and CO₂ are converted into CH₄ within time significantly shorter than the lifetime of the solar nebula at the optimal temperatures around 550 K. The calculation result of clathration shows that CO₂-rich satellitesimals are formed in the catalytically inactive outer region of subnebula. In the catalytically active inner region, CH₄-rich satellitesimals are formed. The resulting CH₄-rich satellitesimals formed in this region play an important role in the origin of CH₄ on Titan. When our experimental data are applied to a high-pressure model for subnebula evolution, it would predict that there should be CO₂ underneath the Iapetus subsurface and no thick CO₂ ice layer on Titan's icy crust. Such surface and subsurface composition, which may be observed by Cassini-Huygens mission, would provide crucial information on the origin of icy satellites.     

矿物类Fenton反应降解有机污染物的研究进展

作为高级氧化工艺之一,Fenton技术能高效地氧化降解有机污染物,矿物催化类Fenton体系的建立则是对Fenton技术的发展和提升。本文在简要介绍传统Fenton技术的基础上,重点阐述了负载型非均相催化类Fenton反应和天然含铁矿物催化类Fenton反应的产生及发展现状。最后结合笔者的科研工作结果展望了天然黑（铁）电气石在矿物催化类Fenton体系中的应用前景。