陈义林, 秦勇. 无机成因二氧化碳气-水界面交换反应表征与机制[J]. 煤炭学报, 2017, (7). DOI: 10.13225/j.cnki.jccs.2016.1424
引用本文: 陈义林, 秦勇. 无机成因二氧化碳气-水界面交换反应表征与机制[J]. 煤炭学报, 2017, (7). DOI: 10.13225/j.cnki.jccs.2016.1424
CHEN Yi-lin, QIN Yong. Characterization and mechanism of exchange reaction through gas-water interface of gaseous inorganic CO2[J]. Journal of China Coal Society, 2017, (7). DOI: 10.13225/j.cnki.jccs.2016.1424
Citation: CHEN Yi-lin, QIN Yong. Characterization and mechanism of exchange reaction through gas-water interface of gaseous inorganic CO2[J]. Journal of China Coal Society, 2017, (7). DOI: 10.13225/j.cnki.jccs.2016.1424

无机成因二氧化碳气-水界面交换反应表征与机制

Characterization and mechanism of exchange reaction through gas-water interface of gaseous inorganic CO2

  • 摘要: 天然气中二氧化碳组分和水体中溶解无机碳构成碳酸平衡体系及碳同位素分馏平衡体系。通过开展无机成因二氧化碳气体的气-水交换实验,揭示了二氧化碳气体在溶解过程中组分体积分数和碳同位素的精细变化。研究发现:在101 325 Pa和30℃条件下,二氧化碳气体经13 h与瓶中水体达到组分体积分数和碳同位素的分馏平衡;初始二氧化碳体积分数为2.0%,平衡后为1.1%;初始δ13CCO2值为-2.5‰,平衡后为-14.6‰,碳同位素分馏幅度高达12.1‰。经气-水界面交换反应,无机成因二氧化碳气体体积分数和碳同位素值随时间变化均可表征为负指数函数。黄河水样δ13CDIC值为-8.2‰,表明水体中大部分DIC来源于土壤有机质分解释放的CO2;富重碳同位素二氧化碳气体与水体DIC反应平衡后,二氧化碳气体由无机成因经混染改造为有机成因。

     

    Abstract: Gaseous carbon dioxide (CO2 ) in natural gas and dissolved inorganic carbon (DIC) in aqueous system are in chemical and isotopic equilibrium. A gas-water exchange experiment with inorganic gaseous CO2 in a closed glass bottle was performed to elucidate the meticulous dynamic change in the chemical composition when gaseous CO2 dis- solves in the water. The results indicate that the CO2 gas achieved compositional and carbon isotopic equilibrium through the gas-water interface within 13 h at 101 325 Pa and 30 ℃ . The initial concentration and δ13 CCO2 values of gaseous CO2 were 2. 0% and -2. 5‰,respectively,and the equilibrium values were 1. 1% and -14. 6‰,respective- ly,with a strong isotopic fractionation (i. e. ,12. 1‰). During the gas-water exchange and dissolution of CO2 ,the CO2 concentration and δ13 CCO2 values could be expressed as an exponential function of time. The δ13 CDIC value,which was approximately -8. 2‰,indicated that a larger proportion of DIC came from organic origin. Gaseous inorganic CO2 was mixed by organic CO2 in water through the gas-water interface,which ultimately presented the characteristic of organic gas. Therefore,carbon isotopic geochemistry of groundwater must be investigated prior to determining the origin and source of gaseous CO2 in natural gas.

     

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