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1.
CO_2向H~+和HCO_3~-的转换是一相对慢速过程。因此,其动力学可能决定碳酸盐岩的溶解速率。在灰岩和白云岩的溶解实验中,使用了自然界普遍存在的碳酸酐酶(Carbonic Anhydrase-CA)来催化这一COO_2转换反应。结果发现,对灰岩而言,加入CA后,其溶解速率在高COO_2分压时增加可达10倍,而对白云岩,其溶解速率增加主要在低COO_2分压时,可达3倍左右。这一发现表明,化学风化(包括碳酸盐岩溶  相似文献   

2.
灰岩和白云岩溶解速率控制机理的比较   总被引：14，自引：2，他引：12  
刘再华  李华举 《地球科学》2006,31(3):411-416
碳酸盐岩溶解的速率控制过程包括:(1)岩石表面上的非均相化学反应;(2)离子从岩石表面通过扩散向溶液中的传输;(3)CO2向H 和HCO-3的转换.通常是这3个过程中的最慢过程决定着碳酸盐岩的溶解速率.然而,实验和理论分析发现,在条件相似的情况下,白云岩的初始溶解速率不仅只有灰岩的1/3～1/60,而且灰岩和白云岩的溶解呈现出不同的速率控制机理.如对灰岩而言,在实验中加入能催化CO2转换反应的生物碳酸酐酶(CA)后,其溶解速率增加出现在CO2分压>100Pa的区域,最高可达10倍;而对白云岩,其溶解速率增加出现在CO2分压<10000Pa的区域,且增加仅3倍左右.此外,虽然2类岩石的溶解也均受水动力条件(旋速或流速)的控制,且主要出现在CO2分压<1000Pa的区域,但灰岩的溶解对水动力条件的变化比白云岩溶解更敏感.这些发现在解释和揭示自然界白云岩和灰岩岩溶发育及其相关资源环境问题的差异方面具有重要意义.  相似文献   

3.
珠江流域碳酸盐岩与硅酸盐岩风化对大气CO_2汇的效应   总被引：6，自引：0，他引：6  
对珠江流域11个测站的河水1个水文年4次取样进行水化学和同位素测试分析,揭示无论是碳酸盐岩区还是硅酸盐岩区,岩石风化均使河流的离子成分以HCO3-、Ca2+、Mg2+为主,碳酸盐岩风化溶蚀速率和由碳酸盐岩风化溶蚀引起的大气CO2消耗量分别为27.60 mm/ka和540.21x103mol/(km2·a-1),是硅酸盐岩风化速率和由硅酸盐岩风化引起的大气CO2消耗量的10.8倍和6.7倍,说明碳酸盐岩风化是流域碳汇过程及效应的主体。由于有利的水热条件和高的碳酸盐岩面积比例,珠江流域平均岩石风化速率和由岩石风化作用引起的大气CO2消耗量分别为30.15mm/ka和620.36×103mol/(km2·a-1),为全球60条河流平均值的2.6倍。  相似文献   

4.
硫酸参与的长江流域岩石化学风化速率与大气CO2消耗   总被引：4，自引：0，他引：4  
流域的岩石化学风化过程是全球碳循环中的重要环节。以往的流域水化学碳汇通量估算大多是基于碳酸的风化作用。而实际上,硫酸和碳酸一样,也参与了流域碳元素的地球化学循环,从而对全球碳循环过程产生影响。长江流域水体近几年出现酸化现象,大部分河段SO42-和Ca2+含量增高,其对应的岩石风化过程和大气CO2消耗速率也发生变化。文章对长江干流及主要支流2013年不同季节的离子组成进行监测,利用水化学平衡法和Galy估算模型,对长江流域岩石化学风化速率和CO2消耗通量进行了估算,对硫酸参与下的长江流域岩石风化和碳循环过程进行了分析。结果表明,长江流域水体离子主要来源于硅酸盐岩风化和碳酸盐岩风化。其中碳酸盐岩风化对河水离子贡献率为92%。在硅酸盐岩广泛分布的赣江流域,碳酸盐岩风化离子贡献也达85%。分析表明,硫酸参与了长江流域的岩石风化过程,对水体中离子产生一定影响。硫酸的参与加快了碳酸盐岩的化学风化速率,平均提高约30%,但是使流域大气CO2消耗速率降低。在不考虑蒸发岩溶蚀作用下,平均从516×103 mol/km2·a降至356×103 mol/km2·a,降低约31%。在各支流中,硫酸对乌江流域碳酸盐岩的风化和碳循环的影响最大,而对雅砻江的影响最小,这与乌江流域的含煤地层、矿床硫化物及大气酸沉降有关。  相似文献   

5.
龙门石窟碳酸盐岩体文物风化作用模拟试验研究   总被引：3，自引：1，他引：2  
张傲  方云  徐敏  陈建平  范子龙 《中国岩溶》2012,31(3):227-233
为了研究凝结水对龙门石窟碳酸盐岩表面的风化作用机理,在现场进行凝结水观测、CO2浓度监测的基础上,利用自行研制、能模拟现场温湿度环境、能提供CO2外部来源,并能对反应过程进行监控的室内模拟试验装置系统对石窟碳酸盐岩风化作用进行模拟实验。实验结果表明,凝结水会造成碳酸盐岩表面的溶解,在CO2加入的条件下风化效果加剧,岩石的质量损失和孔隙率同时增大。经过78次的模拟试验后,灰岩岩样质量损失率为0.077%~0.088%,孔隙率由实验前的0.39%~0.40%增长到0.71%~0.74%;白云岩岩样的质量损失率为0.032%~0.038%,孔隙率由实验前的0.61%~0.68%增长为0.77%~0.85%;灰岩和白云岩的平均溶蚀深度分别为89.475μm和36.865μm,溶蚀速度分别为0.0956μm/h和0.0575μm/h,风化溶蚀作用对龙门石窟文物的影响破坏较大。   相似文献   

6.
通过对四川省雅安龙苍沟峨眉山玄武岩小流域的水化学组成研究,分析了不同物质来源对小流域溪水溶解质的贡献,并对该小流域岩石风化速率和CO2消耗速率进行了估算。结果表明,龙苍沟流域溪水呈中性,PH平均值为6.82。溪水中阳离子以Ca^2+为主,约占阳离子总量的56%;阴离子以HCO3^-为主,约占阴离子总量的45%。碳酸盐岩风化、硅酸盐岩风化、大气降水和人为活动对溪水阳离子平均贡献率分别为50.2%、38.2%、10.5%和1.1%。流域硅酸盐岩风化速率为37.54±24.94 t/km^2/yr,硅酸盐岩风化对大气C02消耗速率为5.4±3.6 mol C/km^2/yr。本文首次对我国峨眉山玄武岩省化学风化大气CO2消耗量进行估算,得到其年消耗通量为1.35±0.89×10^11 mol C/yr,约为全球玄武岩CO2年消耗通量的3.31±2.18%。  相似文献   

7.
《海相油气地质》2013,(3):55-61
通过表面溶蚀和内部溶蚀两种实验方式,分别对六种类型碳酸盐岩用0.2%乙酸溶液进行溶蚀实验,对比研究了从表生环境到深埋藏环境下有机酸与不同类型碳酸盐岩的溶蚀作用机制。对比研究表明:(1)在近地表环境下(25℃,1.0 MPa),泥灰岩和含生物碎屑泥晶灰岩的溶解速率大于细晶白云岩,前两者约为后者的23倍;随着温压的增加,泥灰岩、含生物碎屑泥晶灰岩和细晶白云岩的溶解速率均相应增加,但细晶白云岩的溶解速率增加幅度更大;在深埋藏环境下(180℃,45 MPa到210℃,52.5 MPa),细晶白云岩的溶解速率逐渐与泥灰岩和含生物碎屑泥晶灰岩的溶解速率趋于一致。(2)在60℃,10 MPa时,白云质颗粒灰岩在乙酸溶液中的溶解能力大于粉细晶白云岩和亮晶鲕粒白云岩;随着温压的增加,有机酸溶液对石灰岩与白云岩的溶解能力均相应降低,且石灰岩溶蚀作用下降幅度更大,当温压达到或超过90℃、20 MPa时,粉细晶白云岩和亮晶鲕粒白云岩在乙酸溶液中的溶解能力大于白云质颗粒灰岩。根据实验结果推测:表生和相对浅埋藏的温压条件下,石灰岩的溶解速率和溶解能力大于白云岩,石灰岩的溶蚀作用较白云岩发育;但在深埋藏阶段,由于白云岩的溶解能力大于石灰岩,因此白云岩溶蚀产生的次生孔隙较石灰岩更为发育,这或许是深部的碳酸盐岩储层中多见白云岩储层的重要原因。  相似文献   

8.
大气CO2汇:硅酸盐风化还是碳酸盐风化的贡献?   总被引：1，自引：0，他引：1  
至今人们仍普遍认为:是硅酸盐的化学风化碳汇作用在控制着长时间尺度的气候变化,而碳酸盐的化学风化作用不具有这一功能,因为碳酸盐溶解过程中消耗的所有CO<,2>又通过海洋中相对快速的碳酸盐沉积而返回大气.本研究发现,碳酸盐溶解的快速动力学特性(比硅酸盐快100倍以上)以及硅酸盐流域中少量碳酸盐矿物在控制流域溶解无机碳(DI...  相似文献   

9.
全球碳循环与气候模式中一个关键的不确定性因素就是：有机质活动、温度和大气ＣＯ２对硅酸盐风化作用的综合效应。本文首次指出辉石和钙长石的溶解速率表明，硅酸盐在富有机质溶液中的风化作用并不受土壤ＣＯ２的直接影响，但对温度却很敏感。很明显，ＣＯ２通过增加有机质的活度和产生腐蚀性有机酸而间接地加速了硅酸盐的风化。当将这种风化因素引入稳态碳循环和气候模式中的输出入时，就能加强硅酸盐风化而起到扮演全球恒温箱的作  相似文献   

10.
选取塔中地区奥陶系海相碳酸盐岩样品进行了模拟实验,以研究其在表生岩溶作用下的溶解动力学特征.实验分别在30,50℃下,用pH值为3～6的盐酸溶液,恒温水浴加热进行.结果表明:4种样品溶解速率的相对大小依次为:灰白色灰岩＞砂屑灰岩＞粗晶白云岩＞中粗-细晶白云岩,且溶解速率均随着温度的升高而增大,随着pH值的增大而减小.但随着外界环境的变化,溶解速率的变化略有差异.造成这种差异的原因可能是样品中的硅酸盐杂质、晶体颗粒的大小以及实验过程中产生的CO2的影响.由实验结果推测可知,对于塔中地区以表生岩溶作用为主形成的奥陶系海相碳酸盐岩储层,灰岩储层的储集性能可能优于白云岩储层;对于以埋藏岩溶作用为主形成的奥陶系海相碳酸盐岩储层,白云岩储层的储集性能可能优于灰岩储层.  相似文献   

11.
The conversion of CO2 into H+ and is a relatively slow reaction. Hence, its kinetics may be rate determiningin carbonate rock dissolution. Carbonic anhydrase (CA), which is widespread in nature, was used to catalyze the CO2 conversion process in dissolution experiments of limestone and dolomite. It was found that the rate of dissolution increases by a factor of about 10 after the addition of CA at a high CO2 partial pressure (Pco2) for limestone and about 3 at low Pcoj for dolomite. This shows that reappraisal is necessary for the importance of chemical weathering (including carbonate rock dissolution and silicate weathering) in the atmospheric CO2 sink and the mysterious missing sink in carbon cycling. It is doubtless that previous studies of weathering underestimated weathering rates due to the ignorance of CA as an activator in weathering, thus the contribution of weathering to the atmospheric CO2 sink is also underestimated. This finding also shows the need to examine the situ distribution and activ  相似文献   

12.
碳酸盐岩的H2CO3溶蚀产生岩溶碳汇,占整个岩石风化碳汇的 94%。西南岩溶区硫酸型酸雨严重,硫酸型酸雨广泛参与碳酸盐岩的溶蚀。H2SO4参与的碳酸盐岩风化是一个大气CO2净释放过程,具有减汇作用巨大。另一方面,岩溶区石灰土壤和地下水具有较高的pH值及盐基饱和度,对H+有巨大的缓冲作用,大气酸沉降在碳酸盐岩地区可能并不会造成地下水的HCO3-和pH降低;相反,较高浓度的SO42-所产生的盐效应和SO2-4与各种阳离子形成的离子对会增大方解石、白云石溶解度,可增强H2CO3对碳酸盐的溶蚀,这可能会使岩溶作用产生更大的碳汇效应。因此,硫酸型酸雨参与碳酸盐岩风化的减汇效应不仅可能被高估,硫酸型酸雨还可能增强碳酸盐岩的H2CO3溶蚀,具有增加岩溶碳汇效应的作用。应结合石灰土壤对大气酸沉降的缓冲容量和阈值及大气酸沉降的H+与土壤中盐基离子的交换量,并综合考虑盐效应、离子对作用、同离子效应,客观评价硫酸型酸雨流经石灰土壤层后对碳酸盐岩溶蚀吸收大气/土壤CO2的影响   相似文献   

13.
The dissolution rate-determining processes of carbonate rocks include: (1) heterogeneous reactions on rock surfaces; (2) mass transport of ions into solution from rock surfaces via diffusion; and (3) the conversion reaction of CO2 into H+ and HCO 3 − . Generally, it is the slowest of these three processes that limits the dissolution rate of carbonate rock. However, from experiment and theoretical analysis under similar conditions not only were the initial dissolution rates of dolomite lower by a factor of 3–60 than those of limestone, but also there are different dissolution rate-determining mechanisms between limestone and dolomite. For example, for limestone under the condition of CO2 partial pressures dissolution rates increased significantly by a factor of about ten after addition of carbonic anhydrase (CA) into solution, which catalysed the conversation reaction of CO2, whereas CA had little influence on dolomite dissolution. For dolomite, the increase of dissolution rate after addition of CA into solution appeared at Moreover, the enhancement factor of CA on dolomite dissolution rate was much lower (by a factor of about 3). In addition, when dissolution of both limestone and dolomite was determined by hydrodynamics (rotation speed or flow speed), especially under the dissolution of limestone was more sensitive to hydrodynamic change than that of dolomite. These findings are of significance in understanding the differences in karstification and relevant problems of resource and environment in dolomite and limestone areas.  相似文献   

14.
我国南方岩溶区和北方黄土区的大气CO2效应   总被引：10，自引：1，他引：9  
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  相似文献   

15.
Fertilization and aglime (agricultural lime) application, as important agricultural activities in acid soil, exert an influence on the fluxes of carbon both between and within ecosystems. Animal manure added to soil can elevate the soil CO2 and release organic acid due to microbial decomposition of the high organic matter content of animal manure. Additionally, the elevated CO2 can accelerate carbonate weathering in alkaline soil, such as lime soil. However, in acidic soil, it is unclear whether the chemical weathering of additive aglime can be quickened by the elevated CO2 due to animal manure addition. Thus, to ascertain the impact of animal manure addition on aglime weathering in acidic soil and to understand the weathering agent of aglime or underlying carbonate in the acidic soil profile, we established two contrasting profiles (control profile and manurial profile) in a cabbage-corn or capsicum-corn rotation in a field experiment site located in the HuaXi district of Guiyang, China, and buried carbonate rock tablets at different depths of soil profiles to calculate the dissolution rate of carbonate rock by monitoring the weights of the tablets. The results indicated that soil CO2 increased due to animal manure addition, but the rate of dissolution of the carbonate rock tablets was reduced, which was attributed to the increase in the pH in acidic soil after animal manure addition because the relationship between the dissolution rate of carbonate rock and soil pH indicated that the weathering rate of carbonate rock was controlled by pH and not by CO2 in acidic soil. Thus, the contribution of H+ ions (mainly exchangeable acid) in acid soil as a weathering agent to the weathering of underlying carbonate (and/or aglime) may lead to the overestimation of the CO2 consumption through chemical weathering at the regional/global scale using hydro-chemical methods.  相似文献   

16.
To investigate the impacts of mineral composition on physical and mechanical properties of carbonate rocks, limestone specimens containing different contents in calcite and dolomite are selected to perform CO2-water-rock reaction experiments. The X-ray Diffraction (XRD) and Nuclear Magnetic Resonance (NMR) are carried out to examine the change characteristics of mineral dissolution and pore structure after reaction. The core flooding experiments with Fiber Bragg gratings are implemented to examine the stress sensitivity of carbonate rocks. The results show that the limestones containing pure calcite are more susceptible to acid dissolution compared to limestone containing impure dolomite. The calcite content in pure limestone decreases as the reaction undergoes. The dissolution of dolomite leads to the formation of calcite in impure limestone. Calcite dissolution leads to the formation of macropore and flow channels in pure limestone, while the effects of impure dolomite in impure limestone results in mesopore formation. When confining pressure is lower than 12 MPa, pure limestones demonstrate higher strain sensitivity coefficients compared to impure limestone containing dolomite after reaction. When confining pressure exceeds 12 MPa, the strain sensitivity coefficients of both pure and impure limestones become almost equal.  相似文献   

17.

A much improved understanding of how farmyard manure application may affect carbonate rock dissolution is needed in order to predict possible feedbacks between the rock carbon cycle and the global climate system. Two carbonate mineral rock tablets; dolomite and limestone were buried at six depths between 0 and 110 cm in a soil typical of the subtropical karst area in Guiyang City, Guizhou Province. The extent of tablet dissolution, soil CO2, soil pH, soil water content, soil mineral and chemical composition, and chemical composition of soil water were tested in order to assess the degree of dissolution under manure application over the course of one year. The results show that manure addition decreases the dissolution rate of carbonate rocks; limestone and dolomite by between 11.7%-116.9% and 25.0%-65.69% respectively, with the dissolution rate of limestone consistently exceeding that of dolomite under the same conditions. Our data indicates that the rate of pedogenesis of the dolomite and limestone rocks is decreased as much as 35.77% and 59.41% respectively, as a result of manure application. Moreover, the results suggest that manure application accelerated the generation of soil CO2, with soil CO2 concentration increasing on average by 93.94%, and the CO2 flux increasing by 67.64% compared with the control profile. Finally, the data also indicates that manure decreases CO2 uptake by dissolution of carbonate rocks by 25.50%-39.45% on a Guiyang city scale. The counteraction of the CO2 sink contributed by karst water due to farmyard manure utilization in general karst area (both dolomite and limestone) however was 59.41%-62.72%, indicating the application of manure successfully reduces both dissolution and CO2 release to the atmosphere.

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18.
The chemical weathering can consume atmosphere/soil CO2. Human activities such as pollution, fertilization and acid precipitation have exerted a large impact on CO2 intake by carbonate weathering. Thus, based on the analysis on chemical component change of the karst groundwater in the karst ridge watershed of Conglin Village, Fuling District of Chongqing City, the influence of human activities such as fertilization, sewage discharges from mustard tuber processing, breeding industry and acid rain precipitation on carbonate weathering and CO2 intake in 1980, 2003 and 2006 was studied. The results showed that CO2 intake by carbonate rock declined with year. Because H+ derived from acid sewage discharge, fertilization and acid precipitation reacted with carbonate rock when mustard tuber production and swine breeding were developed fleetly after 2000 as well as the burning amount of high-sulfur coal augmented persistently, which led to the increase of (Ca2++Mg2+)/HCO3-. The difference on charge between Ca2++Mg2+ and HCO3- was balanced by NO3-+SO42-. The control on pollution and acid rain, especially the pre-neutralization of acid waste water, would rejuvenate the atmospheric CO2 intake strength of carbonate weathering besides the protection of water and soil environment  相似文献   

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