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Article(id=1241116652113293678, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241116641321350143, articleNumber=null, orderNo=null, doi=null, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1724256000000, receivedDateStr=2024-08-22, revisedDate=null, revisedDateStr=null, acceptedDate=null, acceptedDateStr=null, onlineDate=1773834868696, onlineDateStr=2026-03-18, pubDate=1742400000000, pubDateStr=2025-03-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1773834868696, onlineIssueDateStr=2026-03-18, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1773834868696, creator=13701087609, updateTime=1773834868696, updator=13701087609, issue=Issue{id=1241116641321350143, tenantId=1146029695717560320, journalId=1234093305789726721, year='2025', volume='45', issue='3', pageStart='1185', pageEnd='1776', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1773834866123, creator=13701087609, updateTime=1773881366030, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1241311676130193619, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241116641321350143, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1241311676130193620, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241116641321350143, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=1568, endPage=1575, ext={EN=ArticleExt(id=1241116653967176100, articleId=1241116652113293678, tenantId=1146029695717560320, journalId=1234093305789726721, language=EN, title=Influence of carbonic anhydrase-producing bacteria on the interaction of sandstone-CO2-water, columnId=1234106388083954308, journalTitle=China Environmental Science, columnName=Environmental Ecology, runingTitle=null, highlight=null, articleAbstract=

In this study, carbonic anhydrase-producing bacteria were selected and introduced into short-term experiments involving sandstone-CO2-water interactions. The chemical properties of the solution, the dissolution-precipitation process of rock minerals, and the changes in bicarbonate ion concentration were analyzed and detected. The results showed that after 20days of reaction under conditions of 50℃ and 10MPa, the pH of the system increased, and the microbial group pH was slightly higher than that of the control group. The participation of bacteria significantly accelerated the dissolution and precipitation processes of rock minerals, reducing the core porosity from 15.02% to 13.27%. In a 1-liter solution with a solid-to-liquid ratio of 1:5, the effective CO2 sequestration amounts for the control group and the microbial group were 0.207g and 0.726g, respectively. The addition of microorganisms resulted in better carbon fixation, demonstrating that carbonic anhydrase-producing bacteria have a certain promoting effect on CO2 geological sequestration.

, correspAuthors=Chun-xiang QIAN, authorNote=null, correspAuthorsNote=null, copyrightStatement=null, copyrightOwner=null, extLink=null, articleAbsUrl=null, sourceXml=null, magXml=null, pdfUrl=null, pdf=null, pdfFileSize=null, pdfExtLink=null, richHtmlUrl=null, mobilePdfUrl=null, reviewReport=null, pdfFirstPage=null, abstractGraph=null, abstractGraphContent=null, abstractVideo=null, citation=null, cebUrl=null, magXmlContent=null, mapNumber=null, authorCompany=null, fund=null, authors=null, authorsList=Bu-kang WANG, Chun-xiang QIAN), CN=ArticleExt(id=1241116656601199311, articleId=1241116652113293678, tenantId=1146029695717560320, journalId=1234093305789726721, language=CN, title=产碳酸酐酶菌对砂岩-CO2-水相互作用的影响, columnId=1234106388268503686, journalTitle=中国环境科学, columnName=环境生态, runingTitle=null, highlight=null, articleAbstract=

选取产碳酸酐酶菌，并将其引入砂岩-CO2-水相互作用的短期试验，对溶液化学性质、岩石矿物溶解-沉淀过程以及碳酸氢根离子浓度变化进行检测分析.结果表明，在50℃、10MPa的条件下反应20d后，体系pH值提升，微生物组pH值略高于对照组，细菌的参与显著加速了岩石矿物的溶蚀沉淀过程，使岩心孔隙度从15.02%降低到13.27%.在固液比为1:5的1L溶液中，对照组和微生物组有效的CO2封存量分别为0.207，0.726g，加微生物的固碳效果更好，证明了产碳酸酐酶菌对CO2地质封存具有一定的促进作用.

, correspAuthors=钱春香, authorNote=null, correspAuthorsNote=
* 责任作者，教授，
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王布康(1996-)，男，贵州遵义人，东南大学博士研究生，主要从事微生物矿化和二氧化碳地质封存研究.发表论文2篇..

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王布康(1996-)，男，贵州遵义人，东南大学博士研究生，主要从事微生物矿化和二氧化碳地质封存研究.发表论文2篇..

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王布康(1996-)，男，贵州遵义人，东南大学博士研究生，主要从事微生物矿化和二氧化碳地质封存研究.发表论文2篇..

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(a)、(b)初始岩样表面，(c)对照组反应后岩样表面，(d)微生物组反应后岩样表面

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Chemical composition analysis of sandstone

, figureFileSmall=null, figureFileBig=null, tableContent=
化学成分SiO2CaOAl2O3Na2OFe2O3MgOK2OTiO2LOIOthers
含量(%)59.2313.4111.783.092.852.701.900.733.360.95
), ArticleFig(id=1241116663710544100, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116652113293678, language=CN, label=表1, caption=

砂岩的化学成分分析

, figureFileSmall=null, figureFileBig=null, tableContent=
化学成分SiO2CaOAl2O3Na2OFe2O3MgOK2OTiO2LOIOthers
含量(%)59.2313.4111.783.092.852.701.900.733.360.95
), ArticleFig(id=1241116663840567540, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116652113293678, language=EN, label=Table 2, caption=

Changes in core porosity before and after 20days of sandstone-CO2-water interaction（%）

, figureFileSmall=null, figureFileBig=null, tableContent=
孔隙度对照组微生物组
反应前14.1515.02
反应后14.9913.27
), ArticleFig(id=1241116664037699840, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116652113293678, language=CN, label=表2, caption=

砂岩-CO2-水相互作用20d前后岩心孔隙度变化（%）

, figureFileSmall=null, figureFileBig=null, tableContent=
孔隙度对照组微生物组
反应前14.1515.02
反应后14.9913.27
), ArticleFig(id=1241116664184500494, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116652113293678, language=EN, label=Table 3, caption=

Changes in sandstone quality and corresponding carbon content in different experimental groups

, figureFileSmall=null, figureFileBig=null, tableContent=
试验组别指标碎屑薄片柱状总和
去离子水-砂岩质量(g)5.296.0854.5365.90
减少的碳物质的量(mmol)1.620.308.6510.57
CA菌-去离子水-砂岩质量(g)5.7912.3354.9973.11
减少的碳物质的量(mmol)0.441.2010.9012.54
), ArticleFig(id=1241116664293552407, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116652113293678, language=CN, label=表3, caption=

不同试验组砂岩质量与对应碳的物质的量变化

, figureFileSmall=null, figureFileBig=null, tableContent=
试验组别指标碎屑薄片柱状总和
去离子水-砂岩质量(g)5.296.0854.5365.90
减少的碳物质的量(mmol)1.620.308.6510.57
CA菌-去离子水-砂岩质量(g)5.7912.3354.9973.11
减少的碳物质的量(mmol)0.441.2010.9012.54
), ArticleFig(id=1241116664390021406, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116652113293678, language=EN, label=Table 4, caption=

CO2 sequestration after 20days of reaction in different experimental groups

, figureFileSmall=null, figureFileBig=null, tableContent=
试验组别1L反应液中砂岩碳的减少量(mmol)结束时碳酸氢根浓度(mg/L)1L溶液封存CO2量(g，固液比1:5)
去离子水-砂岩32.02238.60.207
CA菌-去离子水-砂岩34.43104.00.726
), ArticleFig(id=1241116664511656232, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116652113293678, language=CN, label=表4, caption=

不同试验组反应20d后的CO2封存量

, figureFileSmall=null, figureFileBig=null, tableContent=
试验组别1L反应液中砂岩碳的减少量(mmol)结束时碳酸氢根浓度(mg/L)1L溶液封存CO2量(g，固液比1:5)
去离子水-砂岩32.02238.60.207
CA菌-去离子水-砂岩34.43104.00.726
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产碳酸酐酶菌对砂岩-CO2-水相互作用的影响
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王布康 , 钱春香 *
中国环境科学 | 环境生态 2025,45(3): 1568-1575
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中国环境科学 | 环境生态 2025, 45(3): 1568-1575
产碳酸酐酶菌对砂岩-CO2-水相互作用的影响
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王布康 , 钱春香*
作者信息
  • 东南大学材料科学与工程学院，东南大学绿色建材与固碳利用研究中心，江苏 南京 211189

    • 王布康(1996-)，男，贵州遵义人，东南大学博士研究生，主要从事微生物矿化和二氧化碳地质封存研究.发表论文2篇..

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* 责任作者，教授，
Influence of carbonic anhydrase-producing bacteria on the interaction of sandstone-CO2-water
Bu-kang WANG , Chun-xiang QIAN*
Affiliations
  • Research Center of Green Construction Materials & Carbon Utilization, School of Materials Science and Engineering, Southeast University, Nanjing 211189, China
出版时间: 2025-03-20
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摘要
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选取产碳酸酐酶菌，并将其引入砂岩-CO2-水相互作用的短期试验，对溶液化学性质、岩石矿物溶解-沉淀过程以及碳酸氢根离子浓度变化进行检测分析.结果表明，在50℃、10MPa的条件下反应20d后，体系pH值提升，微生物组pH值略高于对照组，细菌的参与显著加速了岩石矿物的溶蚀沉淀过程，使岩心孔隙度从15.02%降低到13.27%.在固液比为1:5的1L溶液中，对照组和微生物组有效的CO2封存量分别为0.207，0.726g，加微生物的固碳效果更好，证明了产碳酸酐酶菌对CO2地质封存具有一定的促进作用.

CO2  /  地质封存  /  微生物  /  水岩反应

In this study, carbonic anhydrase-producing bacteria were selected and introduced into short-term experiments involving sandstone-CO2-water interactions. The chemical properties of the solution, the dissolution-precipitation process of rock minerals, and the changes in bicarbonate ion concentration were analyzed and detected. The results showed that after 20days of reaction under conditions of 50℃ and 10MPa, the pH of the system increased, and the microbial group pH was slightly higher than that of the control group. The participation of bacteria significantly accelerated the dissolution and precipitation processes of rock minerals, reducing the core porosity from 15.02% to 13.27%. In a 1-liter solution with a solid-to-liquid ratio of 1:5, the effective CO2 sequestration amounts for the control group and the microbial group were 0.207g and 0.726g, respectively. The addition of microorganisms resulted in better carbon fixation, demonstrating that carbonic anhydrase-producing bacteria have a certain promoting effect on CO2 geological sequestration.

CO2  /  geological sequestration  /  microbes  /  water-rock reaction
王布康, 钱春香. 产碳酸酐酶菌对砂岩-CO2-水相互作用的影响. 中国环境科学, 2025 , 45 (3) : 1568 -1575 .
Bu-kang WANG, Chun-xiang QIAN. Influence of carbonic anhydrase-producing bacteria on the interaction of sandstone-CO2-water[J]. China Environmental Science, 2025 , 45 (3) : 1568 -1575 .
正文
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大量化石燃料的使用导致大气中二氧化碳(CO2)浓度急剧增加，使得全球气温上升，由此所引发的全球气候变化问题已经成为威胁人类生存的重要问题[1-5].减少CO2对生存环境的影响要从源头控制CO2的排放以及对现有CO2进行捕集、利用和封存.地质封存是CO2封存的主要方式，被认为是迅速减少温室气体排放量最有效最有前景的技术之一，具有封存时间长、安全性高、封存量大等优点[6-8].CO2地质封存场所应该满足以下条件：区域内地质构造稳定，封存地有足够大的容积，具有良好密封性的盖层，封存场所温度和压力要超过CO2的临界点，常见的封存区域包括深部咸水层、枯竭油气藏和深部不可开采的煤层等[9-11].在CO2封存过程中，超临界的CO2(scCO2，临界温度和压力为31.1℃和7.4MPa)被注入地下深部多孔地质构造中，导致局部地层的环境压力升高和地下的地球化学变化，扰乱储层流体和岩石的原有平衡[12-13].因此，有必要研究CO2注入储层后的地球化学变化，以明晰CO2的封存机理和效果，同时也防止CO2发生泄漏.
地质封存的方式有物理封存和化学封存，物理封存主要依靠地质结构将CO2圈闭，有泄漏的风险，需要长期监测；化学封存是指将CO2转化为离子态或者固体碳酸盐的形式固定，泄漏风险小且相对更加安全，但自然过程十分缓慢[14-15].地层中含有大量的微生物，在维持地球化学平衡中扮演着不同的角色，例如产酸、产碱、影响氧化还原反应、结成生物膜封堵裂缝孔隙等，随着CO2地质封存的研究越来越多，人们开始注意到微生物在其中的积极作用[12,16-17].以往对CO2注入后的地球化学变化研究主要集中在地层流体运移[18-19]、岩体微孔隙变化[20-21]和CO2对地层原位微生物群落的影响[22-23]，起初主要将微生物群落变化作为监测CO2泄露的一个因子，而微生物对水岩反应的具体影响和机理研究较少.前期研究表明，在常温常压下微生物代谢作用产生的碳酸酐酶能有效促进CO2与HCO3−之间的转化，因此研究产碳酸酐酶菌对高温高压下CO2地质封存的实际影响具有重要意义[24-25].为了探究微生物与CO2、水、岩石之间的复杂相互作用，本文模拟地下1000m左右的地层压力和温度开展了20d微生物介导的砂岩-scCO2-去离子水试验，以探明产碳酸酐酶菌介导的短期水岩反应机理，及其对CO2地质封存的影响.
1　材料与方法
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1.1　试验材料
1.1.1　水和微生物
试验用水为扬州某公司生产的去离子水，试验所用微生物为东南大学绿色建材与固碳利用研究中心筛选培养的产碳酸酐酶菌，培养基成分包括葡萄糖(5g/L)和酵母浸粉(2.5g/L)，反应前在温度为50℃的培养箱中振荡培养30h，OD600值达到1.4左右.
1.1.2　岩石样品
试验所用岩心样品为砂岩，表面呈砖红色，购买自山东某公司，根据X射线衍射(XRD)和X射线荧光(XRF)检测结果表明，主要成分为石英、钠长石、钙长石、方解石、白云石和微斜长石，砂岩的化学成分如表1所示，试验时，将一部分岩石切割成直径25mm、高5mm的岩石薄片和直径25mm、高50mm的圆柱样品，另一部分处理成直径小于3mm均匀破碎的石块碎屑.
1.1.3　试验装置
本研究的水岩反应试验装置由CO2气瓶、空压机、气体增压系统和高温高压反应釜组成，如图1所示.
1.2　试验方法
1.2.1　砂岩-CO2-水静态反应试验
不同形状的砂岩样品与微生物介导的CO2-去离子水在无菌的高温高压不锈钢反应釜中反应，以不添加微生物为对照组.首先放入岩样，再加入反应溶液(去离子水或者去离子水与菌液的混合)，然后对密封的反应釜抽真空以排除其他气体的干扰，将反应温度设置为50℃，待温度达到目标值后再通入CO2气体，直至釜内压力达到10MPa时停止通入CO2.设置釜内运行转速为500r/min，运行时间20d，初始固液质量比为1：5，当添加微生物时细菌培养液与去离子水的质量比为3：5.待运行时间结束后，取出岩样用蒸馏水冲洗3次，在60℃下干燥48h后称重，然后再进行岩石样品测试分析.
1.2.2　反应溶液地球化学分析
为了在试验过程中维持反应釜内的压力和固液比，不得不减少采样次数和样品量，每间隔5d取一次反应溶液进行分析，每次取样约5mL.液体样品中溶解的Ca2+，Mg2+，Na+和K+采用电感耦合等离子体发射光谱法测定(ICP-OES，精度0.1×10-6)，在测试前用盐酸进行酸化处理.溶液pH值采用精密pH计(雷磁PHS-3C，精度0.01)测定，测定时间为取出样品后立即进行，待读数稳定后读取数值.测定pH值后再用酶标仪检测溶液中OD600值.溶液中的碳酸氢根和碳酸根采用滴定法检测，分别用甲基橙和酚酞作指示剂，用盐酸标准溶液滴定稀释后的反应液，根据滴定消耗盐酸标准溶液的体积，计算出碳酸氢根和碳酸根的含量.
1.2.3　岩样变化分析
反应前后岩石的表面形貌通过扫描电子显微镜(SEM)观察，测试前需用高分辨率溅射镀膜仪喷金镀膜.岩石矿物物相变化用X射线衍射(XRD)检测，分析前将反应前后碎屑岩石样品烘干并研磨过200目筛，扫描速度为0.15°/min，步长为0.02°，扫描范围为5~70℃.岩石碳物质的量的变化用烧失法检测，具体操作为将样品放入马弗炉中从30℃升温到500℃持续煅烧30min，然后将样品取出冷却、称重，接着放回样品继续升温到900℃持续煅烧120min，再次将样品取出冷却称重，两次质量相减得到损失的CO2质量，再除以CO2的相对分子质量即为碳物质的量变化；岩石样品的质量变化用精密天平称量.岩石孔隙率和内部孔径变化采用低场核磁检测，所用设备为MesoMR12-060V-I型纳米孔隙结构分析系统-低场核磁(孔径测试范围为4~1400nm).
2　结果与讨论
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2.1　注射scCO2后溶液pH值和OD600值变化
scCO2注入反应体系会对溶液的酸碱性产生影响，同时微生物的代谢活动也会影响pH值的变化，对不同时间的反应液进行pH值和OD600值检测，能更好地判断CO2和岩石矿物的溶解情况以及细菌的浓度变化.测量结果如图2所示，当scCO2溶于水后形成H2CO3导致初始pH值较低，溶液pH值随着反应时间增加逐渐升高，OD600值的变化趋势呈先减小再增加.随着反应的进行，pH值从0d的5.4左右增加到20d的6.4左右，增长速率由大变小，但还未达到稳定的状态，同时微生物组的pH值比对照组稍高，pH值的增加说明矿物溶蚀过程消耗了氢离子使pH值得到缓冲[26].另外，由于pH值测量是在反应釜外进行，温度和压力与釜内实际情况有差别，导致所测pH值比釜内实时值略高.微生物生长需要一定的条件，反应釜内养分不足、条件苛刻，不利于微生物的生长繁殖，反应到第10d时OD600值降到最低，后面开始逐渐升高可能是因为细菌适应环境后的生长或者是部分黏土矿物溶解脱离以及可能的碳酸盐沉淀生成共同导致，推测营养物质消耗完后，微生物将不再繁殖生长，进一步的原因分析还有待增加反应时间和测试方法验证.
2.2　砂岩-CO2-水相互作用中的矿物溶蚀与沉淀
2.2.1　岩石物相变化和质量变化
XRD物相分析结果如图3(a)所示，反应前后岩石物相种类没有变化，没有新的矿物衍射峰生成，但峰的强度发生了改变.20d后，岩石薄片和圆柱的质量损失如图3(b)所示，对于同样的砂岩，体积越大质量损失率越低，同时微生物组的质量损失也比对照组大，对照组岩石薄片和岩石圆柱的质量损失率分别为1.81%和0.88%，微生物组质量损失率分别为2.20%和1.40%，说明微生物组发生的溶蚀作用更加强烈，这主要与微生物的生长代谢有关.
2.2.2　主要阳离子浓度变化
CO2注入地层后，短时间内会引起注入点附近的地层溶液pH值降低，导致部分可溶性岩石矿物的溶解，为研究反应釜内砂岩的地球化学变化，对反应过程溶液主要阳离子浓度(K+、Na+、Ca2+、Mg2+)进行检测.检测结果如图4所示，在岩石-CO2-水的相互作用过程中，相比于对照组，微生物组能够明显促进岩石的阳离子溶出.
由图4(a)可知，对照组K+浓度变化幅度较小，数值基本在10~15mg/L之间，掺入细菌反应后，溶液中K+浓度能够增加4~5倍，具有很好地释放钾的作用，变化规律与前人研究一致[27].在前5d内，对照组Na+浓度减少，微生物组增多，在5d后，对照组中检测不到Na+的存在，微生物组中Na+浓度也降低至6mg/L左右(图4(b))，根据钠的浓度变化推测反应釜中可能生成了片钠铝石[20]，但因为量太少或者非晶的缘故，XRD物相检测中未观察到片钠铝石的峰强.Ca2+浓度随着反应时间增加而不断增多，这主要与方解石和白云石的溶解有关，在第15d时略有下降，可能是因为局部过饱和产生了少量的碳酸盐沉淀，反应结束对照组和微生物组最高分别达到593.4和859.67mg/L左右(图4(c)).与Ca2+变化趋势相似，溶液中Mg2+浓度变化也与反应时间成正比，前5d对照组Mg2+增加较少，而微生物组则迅速升高(图4(d)).对比两组试验阳离子溶出结果，与质量损失变化对应，皆显示出微生物组的溶蚀作用更强.主要原因是碳酸酐酶对CO2的催化水合作用产生的H+能够置换部分硅酸盐和碳酸盐矿物中的阳离子，造成矿物溶蚀破坏[28]；同时，当微生物与矿物复合时，微生物代谢作用产生的有机酸能够在局部促进矿物溶解，但由于有机酸的酸性不是很强，起到的作用有限[29]；除此之外，通过前人对微生物胞外聚合物的研究，发现其具有pH值较低、黏度较高的特殊性质，能为细菌矿物复合体的形成和矿物溶解提供有利的条件[30-31].
2.2.3　岩石微区形貌变化
岩石表面微区形貌变化与岩石发生的地球化学反应剧烈程度有关，为探求微生物介导的砂岩-CO2-水相互作用对岩样表面溶蚀的影响，对反应前后岩样表面进行扫描电镜观察.结果如图5所示，反应前初始岩样表面相对完整致密，没有明显深坑，等到水岩反应试验开展20d后，对照组和微生物组岩石表面皆可看到明显的溶蚀深坑，同时部分区域也露出光滑且菱角分明的矿物形态，由表面反映内部，说明砂岩发生了剧烈的溶蚀作用，但加菌与不加菌在表面形貌上的变化较小.由于石英具有较强的稳定性，根据2.2.2节主要阳离子浓度变化和赵静等[32]的研究结果，推测本试验中钠长石、钙长石、方解石、白云石和微斜长石都有不同程度的溶解，但因为试验时间较短，在XRD物相检测中未能检出岩石物相变化.
2.2.4　岩石内部孔隙结构变化
岩心孔隙结构变化对CO2地质封存有直接的影响，为更好地表征岩石在通入CO2后发生的溶蚀与沉淀，对反应前后的岩样进行低场核磁检测，以展现岩心内部孔隙结构变化.由表2和图6可知，经过砂岩-CO2-水相互作用20d后，对照组岩心孔隙度从14.15%增加到14.99%，小孔径比例增加，大孔径比例基本未变；微生物组岩心孔隙度从15.02%降低到13.27%，小孔径比例增加但大孔径比例相对减少更多，说明水岩反应过程中发生了改变岩石内部孔隙结构的溶解-沉淀作用，且微生物组产生的次生矿物沉淀更多导致孔隙度下降.由图7岩心孔喉尺寸变化可知，反应后0.25µm以下的小尺寸孔喉比例增多，其他尺寸孔喉比例减少，说明内部新产生的次生矿物对较大孔喉产生了一定的填充作用，同时岩样内部的溶蚀作用使部分未连通的微小孔隙溶解贯通.
2.3　砂岩-CO2-水相互作用的固碳效果
CO2通入反应釜后，在高温高压作用下有一部分会转化为HCO3−或者CO32−的形式存在，尤其在微生物的碳酸酐酶参与下，会加速CO2的水合作用，因此对反应过程中溶液的HCO3−和CO32−进行滴定检测，可以反映CO2在溶液中的溶解量，但因为砂岩中的碳酸盐也会发生部分溶解，所以在计算CO2溶解封存量时要考虑矿物溶解的因素.通过烧失法检测反应前后砂岩的碳含量变化，如反应体系碳物质的量减少则表示溶解作用大于沉淀作用，反之则表示溶解作用小于沉淀作用.综上，有效的CO2溶解封存量等于溶液中总的碳增加量减去固体砂岩中碳的减少量.
本次试验中滴定法未检测出碳酸根离子，溶液中CO2的溶解量通过碳酸氢根离子表示，如图8所示，随着反应时间的进行，碳酸氢根离子浓度持续升高，具体表现为前期增长较快，中后期增长较慢，且微生物组的碳酸氢根离子浓度明显高于对照组，这主要是因为碳酸酐酶的水合与矿物溶解的共同作用.在反应前5d HCO3−的增长速率最大，对照组和微生物组分别达到242.7，484.1mg/ (L·d)，反应到20d时，总的浓度分别增长到2038.6和3104mg/L.根据第2.2.2节主要阳离子浓度变化结果，假设K+、Na+、Ca2+、Mg2+全部由HCO3−平衡，则在1L溶液中对照组与微生物组分别需要33.0和48.5mmol碳酸氢根离子来平衡，比反应结束实际测量的结果低，主要原因是一部分碳酸氢根离子由氢离子平衡.
由2.2.1砂岩质量损失结果可知，不同形态的砂岩在体系中参与反应的程度不同，所以对反应前后的砂岩碎屑、薄片和圆柱分别进行烧失，计算出不同形态砂岩碳的物质的量变化总和即为固体砂岩中碳的变化量.
烧失法测砂岩中碳的物质的量计算公式为[33]：
式中：n为碳的物质的量变化；M500是煅烧到500℃的质量；M900是煅烧到900℃的质量.
测量计算结果如表3、表4所示，反应后对照组和添加微生物组砂岩中碳的物质的量变化分别为10.57，12.54mmol，根据结束时碳酸氢根离子浓度和反应前后砂岩中碳的物质的量变化，可计算出1L反应液中(固液比为1：5)有效的CO2封存量分别为0.207和0.726g，微生物组固碳效果明显比对照组更优.
3　结论
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3.1　CO2通入反应容器后，由于其溶解于水生成碳酸，会引起体系pH值下降，之后随着反应时间增加pH值逐渐增高，到后期趋于平缓.细菌与培养液的加入能缓冲一定的pH值，反应前期微生物组的pH值略高，试验到20d时，两者的pH值接近，从长期来看，微生物对CO2地质封存体系pH值的影响较小.
3.2　微生物加速了岩石矿物溶蚀.试验开始会有部分细菌附着在矿物表面，在新陈代谢过程中，细菌产生有机酸使局部pH值降低，加上碳酸酐酶的催化水合与胞外聚合物的协同作用，加速了砂岩矿物的离子溶出，使更多可溶性矿物被溶解；反应之后岩样表面增加了溶蚀坑洞，且微生物加速了此溶蚀过程，岩样的质量损失增大.
3.3　岩心的孔隙结构变化对流体在岩石内部的运移和封存起着至关重要的作用，砂岩-CO2-水反应后20d后，岩心内部的小尺寸孔喉增加，中大尺寸孔喉减少，对照组岩心孔隙度增加，微生物组孔隙度减少，表明岩心内部不仅有溶蚀作用，也有沉淀填充了大直径孔喉.
3.4　溶液中碳酸氢根离子浓度随着反应时间的增加而增加，细菌产生的碳酸酐酶能促进CO2的水合反应，同时细菌的代谢产物有机酸和胞外聚合物有利于岩石矿物的溶解，使微生物组的碳酸氢根离子浓度高于对照组.试样反应20d后，固液比为1：5的1L溶液在加菌和不加菌条件下，能分别封存CO2 0.726和0.207g，微生物组是对照组的3.5倍.
基金
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  • 国家自然科学基金资助项目(U22B20146)
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2025年第45卷第3期
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    东南大学材料科学与工程学院，东南大学绿色建材与固碳利用研究中心，江苏 南京 211189

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