张晓月,刘娜,张松旭,许建福

• 1:吉林大学地球科学学院

摘要(Abstract)：

矿物封存是CO_2地质埋存技术中最安全、泄漏风险最低的封存手段。近年来，玄武岩体系的CO_2矿化封存受到广泛关注，其核心在于利用火山岩中的Ca、Mg的硅酸盐矿物与CO_2发生水-岩反应，转化为稳定碳酸盐矿物。本研究围绕玄武岩中重要的造岩矿物——透辉石（CaMgSi_2O_6），设计并开展不同温度条件下的CO_2-透辉石单矿物相互作用实验，并结合数值模拟约束反应路径与固碳潜力。通过对反应后溶液总矿化度（TDS）与主要离子的变化、固体质量的损失、扫描电镜（SEM）形貌与矿物识别综合分析，表明：CO_2流体对透辉石的溶解强度与温度正相关；反应产物中可识别出方解石、菱镁矿和白云石等碳酸盐矿物，指示Mg、Ca的有效迁移与固碳；数值模拟与实验结果相互印证，明确了透辉石具有可观的固碳潜力。本研究为玄武岩固碳潜力的定量和预测提供了实验与模拟的双重证据，对完善玄武岩-CO_2-水地球化学模型与工程选址具有启示意义。

关键词(KeyWords)： CO_2矿化封存;透辉石;水-岩相互作用;TOUGHREACT;碳酸盐矿物沉淀

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金面上项目（42272146）,国家自然科学基金青年科学基金项目（41202073）

作者(Author): 张晓月,刘娜,张松旭,许建福

参考文献(References)：

• [1]JING Z. Legal regulation of CCS technique[J]. Applied Mechanics and Materials, 2013, 361-363:1028-1031.
• [2]苗健，牟鸿涛，龙陆军，等.不同相态下CO2封存技术研究进展[J].中国煤炭地质，2025,37(6):66-71.
• [3]任韶然，张莉，张亮.CO2地质埋存：国外示范工程及其对中国的启示[J].中国石油大学学报（自然科学版），2010,34(1):93-98.
• [4]GUNTER W D,PERKINS E H,MCCANN T J.Aquifer disposal of CO2-rich gases:Reaction design for added capacity[J]. Energy Conversion and Management, 1993, 34(9-11):941-948.
• [5]METZ B, DAVIDSON O, DE CONINCK H C, et al. IPCC special report on carbon dioxide capture and storage[M]. Cambridge:Cambridge University Press, 2005.
• [6]张亮，温荣华，耿松鹤，等.CO2在玄武岩中矿物封存研究进展及关键问题[J].高校化学工程学报，2022,36(4):473-480.
• [7]高志豪，夏菖佑，廖松林，等.玄武岩CO2矿化封存潜力评估方法研究现状及展望[J].高校地质学报，2023,29(1):66-75.
• [8]XU T, APPS J A, PRUESS K. Mineral sequestration of carbon dioxide in a sandstone-shale system[J]. Chemical Geology, 2005, 217(3-4):295-318.
• [9]XU T, SONNENTHAL E, SPYCHER N, et al. TOUGHREACT—a simulation program for non-isothermal multiphase reactive geochemical transport in variably saturated geologic media:Applications to geothermal injectivity and CO2 geological sequestration[J].Computers&Geosciences, 2006, 32(2):145-165.
• [10]杨睿芝.枯竭气藏CO2注入和埋存中与地层水岩石相互作用研究[D].四川成都：西南石油大学，2017.
• [11]GYSI A P, STEF??NSSON A. Mineralogical aspects of CO2 sequestration during hydrothermal basalt alteration—An experimental study at 75 to 250°C and elevated pCO 2[J]. Chemical Geology, 2012, 306-307:146-159.
• [12]赵爽.幔源CO2-岩屑砂岩相互作用的地质记录[D].吉林长春：吉林大学，2013.
• [13]朱焕来，曲希玉，刘立，等.CO2流体-长石相互作用实验研究[J].吉林大学学报（地球科学版），2011,41(3):697-706.
• [14]MUNZ I A, BRANDVOLL??，HAUG T A, et al. Mechanisms and rates of plagioclase carbonation reactions[J]. Geochimica et Cosmochimica Acta, 2012, 77:27-51.
• [15]DE OBESO J C, AWOLAYO A N, NIGHTINGALE M J, et al.Experimental study on plagioclase dissolution rates at conditions relevant to mineral carbonation of seafloor basalts[J]. Chemical Geology, 2023, 620.
• [16]KASHIM M Z, TSEGAB H, RAHMANI O, et al. Reaction mechanism of wollastonite in situ mineral carbonation for CO2 sequestration:Effects of saline conditions, temperature, and pressure[J]. ACS Omega, 2020, 5(45):28942-28954.
• [17]曲希玉.CO2流体-砂岩相互作用的实验研究及其在CO2气储层中的应用[D].吉林长春：吉林大学，2007.
• [18]贾祎轲.二氧化碳地质封存过程中水—气—岩反应实验及模拟研究[D].北京：中国地质大学（北京），2013.
• [19]莫绍星，龙星皎，李瀛，等.基于TOUGHREACT-MP的苏北盆地盐城组咸水层CO2矿物封存数值模拟[J].吉林大学学报（地球科学版），2014,44(5):1647-1658.
• [20]董林森.CO2-火山碎屑岩相互作用的特征与机理[D].吉林长春：吉林大学，2011.
• [21]谢爽.不同相态CO2-水-页岩相互作用实验研究[D].重庆：重庆大学，2021.
• [22]王晓，文凯星，石祥超，等.扩散作用控制下CO2矿化封存实验及模拟研究[J].煤炭学报，2024,49(10):4235-4251.
• [23]刘云乾，廖志伟，丁海，等.玄武岩矿化封存CO2机理及储层演化特征研究进展[J].成都理工大学学报（自然科学版），2024,51(6):975-988.
• [24]李万伦，陈晶，贾凌霄，等.玄武岩CO2地质封存研究进展[J].地质论评，2022, 68(2):648-657.
• [25]邱添，曾令森，申婷婷.基性–超基性岩碳酸盐化固碳效应研究进展[J].中国地质调查，2021,8(4):20-32.
• [26]SN??BJ??RNSD??TTIR S??，SIGF??SSON B, MARIENI C, et al.Author correction:Carbon dioxide storage through mineral carbonation[J]. Nature Reviews Earth&Environment, 2020, 1(12):695.
• [27]CAO X, LI Q, XU L, et al. A review of in-situ carbon mineralization in basalt[J]. Journal of Rock Mechanics and Geotechnical Engineering,2023,15(5):1201-1215.
• [28]LU P, APPS J, ZHANG G, et al. Knowledge gaps and research needs for modeling CO2 mineralization in the basalt-CO2-water system:A review of laboratory experiments[J]. Earth-Science Reviews, 2024,250.
• [29]赵文.玄武岩分布特征及工程性状[J].铁道勘察，2009, 35(5):60-64.
• [30]KOSCHEL D, COXAM J Y, RODIER L, et al. Enthalpy and solubility data of CO2 in water and NaCl(aq)at conditions of interest for geological sequestration[J]. Fluid Phase Equilibria, 2006, 247(1-2):107-120.
• [31]WAPLES D W, WAPLES J S. A review and evaluation of specific heat capacities of rocks, minerals, and subsurface fluids. Part 1:Minerals and nonporous rocks[J]. Natural Resources Research, 2004,13(2):97-121.
• [32]BRANTLEY S L, MELLICHAMP D A. Surface area and porosity of primary silicate minerals[J]. American Mineralogist, 2000, 85(11-12):1767-1783.
• [33]WOLERY T J, DAVELER S A. EQ6:A computer program for reaction path modeling of aqueous geochemical systems—Theoretical manual, user’s guide, and related documentation(Version 7.0)[R].Livermore:Lawrence Livermore National Laboratory, 1992.
• [34]PALANDRI J L, KHARAKA Y K. A compilation of rate parameters of water-mineral interaction kinetics for application to geochemical modeling[R]. Reston:U.S. Geological Survey, 2004.
• [35]DAVAL D, HELLMANN R, CORVISIER J, et al. Dissolution kinetics of diopside as a function of solution saturation state:Macroscopic measurements and implications for modeling of geological storage of CO2[J]. Geochimica et Cosmochimica Acta, 2010, 74(9):2615-2633.
• [36]SN??BJ??RNSD??TTIR S??，SIGF??SSON B, MARIENI C, et al.Carbon dioxide storage through mineral carbonation[J]. Nature Reviews Earth&Environment, 2020, 1(2):90-102.
• [37]SALDI G D, JORDAN G, SCHOTT J, et al. Magnesite growth rates as a function of temperature and saturation state[J]. Geochimica et Cosmochimica Acta, 2009, 73(18):5646-5657.
• [38]TURVEY C C, WILSON S A, HAMILTON J L, et al.Hydrotalcites and hydrated Mg-carbonates as carbon sinks in serpentinite mineral wastes from the Woodsreef chrysotile mine, New South Wales, Australia:Controls on carbonate mineralogy and efficiency of CO2 air capture in mine tailings[J]. International Journal of Greenhouse Gas Control, 2018, 79:38-60.
• [39]GYSI A P, STEF??NSSON A. CO2-water-basalt interaction. Low temperature experiments and implications for CO2 sequestration into basalts[J]. Geochimica et Cosmochimica Acta, 2012, 81:129-152.
• [40]SN??BJ??RNSD??TTIR S??，GISLASON S R. CO2 storage potential of basaltic rocks offshore Iceland[J]. Energy Procedia, 2016,86:371-380.
• [41]MCGRail B P, SCHAEF H T, HO A M, et al. Potential for carbon dioxide sequestration in flood basalts[J]. Journal of Geophysical Research:Solid Earth, 2006, 111(B12).
• [42]WHITE S K, SPANE F A, SCHAEF H T, et al. Quantification of CO2 mineralization at the Wallula Basalt Pilot Project[J].Environmental Science&Technology, 2020, 54(22):14609-14616.
• [43]赵欣豪，刘会虎，丁海，等.二氧化碳地质封存工程实例及技术分析[J].中国煤炭地质，2024,36(10):66-69.
• [44]STEWART E M, AGUE J J, FERRY J M, et al. Carbonation and decarbonation reactions:Implications for planetary habitability[J].American Mineralogist, 2019, 104(10):1369-1380.
• [45]FERREIRA A, COSTA I S L, ALMEIDA F F M, et al.Unraveling the rapid CO2 mineralization experiment using the Paranáflood basalts of South America[J]. Scientific Reports, 2024, 14.
• [46]吾尔娜，吴昌志，季峻峰，等.松辽盆地徐家围子断陷玄武岩气藏储层的CO2封存潜力研究[J].高校地质学报，2012,18(2):239-247.