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Article(id=1149768948670972068, tenantId=1146029695717560320, journalId=1146123166801305609, issueId=1149768937925165147, articleNumber=null, orderNo=null, doi=10.12404/j.issn.1671-1815.2406035, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1723392000000, receivedDateStr=2024-08-12, revisedDate=1737648000000, revisedDateStr=2025-01-24, acceptedDate=null, acceptedDateStr=null, onlineDate=1752055879036, onlineDateStr=2025-07-09, pubDate=1748361600000, pubDateStr=2025-05-28, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1752055879036, onlineIssueDateStr=2025-07-09, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1752055879036, creator=13701087609, updateTime=1752055879036, updator=13701087609, issue=Issue{id=1149768937925165147, tenantId=1146029695717560320, journalId=1146123166801305609, year='2025', volume='25', issue='15', pageStart='6155', pageEnd='6586', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=0, createTime=1752055876475, creator=13701087609, updateTime=1768456822194, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1218559490207699090, tenantId=1146029695717560320, journalId=1146123166801305609, issueId=1149768937925165147, language=EN, specialIssueTitle=, coverIllustrator=, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1218559490211893395, tenantId=1146029695717560320, journalId=1146123166801305609, issueId=1149768937925165147, language=CN, specialIssueTitle=, coverIllustrator=, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=6297, endPage=6303, ext={EN=ArticleExt(id=1149768949056848047, articleId=1149768948670972068, tenantId=1146029695717560320, journalId=1146123166801305609, language=EN, title=Effect of Wettability on Carbon Dioxide Extraction of Crude Oil Components, columnId=1156262729003422020, journalTitle=Science Technology and Engineering, columnName=Papers·Petroleum and Natural Gas Industry, runingTitle=null, highlight=null, articleAbstract=

The silica with the highest content in sandstone was taken as the main research object. The SiO2 surfaces underwent hydroxyl (—OH) and methyl (—CH3) treatments to represent the hydrophilic and hydrophobic walls, respectively. LAMMPS software was utilized to implement molecular dynamics simulations and replicate the process of supercritical CO2 extraction of crude oil components. The results indicate that the temperature is 333.15 K and the pressure is 20 MPa. The hydroxylated silica surface extracted 5.07% more saturated hydrocarbon molecules using supercritical CO2 compared to the methylated silica surface. The interaction energy between the oil components and the two wall surfaces is mutually attractive. The interaction energy of saturated hydrocarbon molecules decreases by 77.52% for hydroxylated silica surface and 46.04% for methylated silica surface, respectively. Additionally, the interaction energy of methylated silica on saturated hydrocarbon is greater than that of the hydroxylated silica surface.It is important to note that carbon dioxide easily extracts saturated hydrocarbons with short molecular chains. The diffusion coefficients of crude oil components under two surface conditions are saturated hydrocarbons > resins > aromatic hydrocarbons > asphaltenes.

, correspAuthors=Yue-qi WANG, 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=Yin-qing LIU, Yue-qi WANG, Wen-guo MA, Rui-xin YANG, Wen-hang YUAN, Xuan LIU), CN=ArticleExt(id=1149768976932192530, articleId=1149768948670972068, tenantId=1146029695717560320, journalId=1146123166801305609, language=CN, title=润湿性对二氧化碳萃取原油组分的影响, columnId=1156262729603207500, journalTitle=科学技术与工程, columnName=论文·石油、天然气工业, runingTitle=null, highlight=null, articleAbstract=

以砂岩中含量最高的二氧化硅为主要研究对象,对二氧化硅壁面分别进行了羟基(—OH)化和甲基(—CH3)化处理代表亲水和疏水壁面,运用LAMMPS软件进行分子动力学对超临界CO2萃取原油组分的过程进行模拟研究。结果表明:温度为333.15 K、压力为20 MPa时,超临界CO2萃取出羟基化二氧化硅壁面的饱和烃分子比甲基化二氧化硅壁面的多5.07%;原油组分与两种壁面的相互作用能均为吸引关系,饱和烃分子的相互作用能下降幅度最大分别为77.52%(羟基化二氧化硅壁面)和46.04%(甲基化二氧化硅壁面)且甲基化二氧化硅对饱和烃的相互作用能大于羟基化二氧化硅壁面;CO2容易萃取出分子链较短的饱和烃分子,原油组分在两种壁面条件下的扩散系数大小为饱和烃>胶质>芳香烃>沥青质。

, correspAuthors=王玥琦, authorNote=null, correspAuthorsNote=
* 王玥琦(1999—),女,汉族,黑龙江齐齐哈尔人,硕士研究生。研究方向:油气田开发,渗流理论。E-mail:。
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刘银庆(1971—),男,汉族,山东安丘人,硕士,副教授。研究方向:石油与天然气多相流动。E-mail:。

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刘银庆(1971—),男,汉族,山东安丘人,硕士,副教授。研究方向:石油与天然气多相流动。E-mail:。

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刘银庆(1971—),男,汉族,山东安丘人,硕士,副教授。研究方向:石油与天然气多相流动。E-mail:。

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Daqing: Daqing Institute of Petroleum, 2006., articleTitle=null, refAbstract=null)], funds=null, companyList=[AuthorCompany(id=1175506410734498592, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, xref=1, ext=[AuthorCompanyExt(id=1175506410742887201, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, companyId=1175506410734498592, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=1 School of Petroleum Engineering, Northeast Petroleum University, Daqing 163318, China), AuthorCompanyExt(id=1175506410747081506, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, companyId=1175506410734498592, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=1 东北石油大学石油工程学院, 大庆 163318)]), AuthorCompany(id=1175506410814190371, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, xref=2, ext=[AuthorCompanyExt(id=1175506410830967588, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, companyId=1175506410814190371, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=2 Dongsheng Petroleum Development Group Company Ltd., Shengli Oilfield, Sinopec, Dongying 257000, China), AuthorCompanyExt(id=1175506410839356197, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, companyId=1175506410814190371, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=2 中国石化胜利油田东胜精攻石油开发集团有限公司, 东营 257000)])], figs=[ArticleFig(id=1175506412525466446, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.1, caption=SiO2 surface model, figureFileSmall=DrIFogOaKIxRZzQjZm+UJA==, figureFileBig=TvYT54nRr4wcQ9vvXoZT+g==, tableContent=null), ArticleFig(id=1175506412588381007, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图1, caption=二氧化硅壁面模型

硅原子 氧原子 碳原子 氢原子

, figureFileSmall=DrIFogOaKIxRZzQjZm+UJA==, figureFileBig=TvYT54nRr4wcQ9vvXoZT+g==, tableContent=null), ArticleFig(id=1175506412642906960, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.2, caption=Molecular structures of each component in the model, figureFileSmall=M0jDwtBiAdpfYtS8JttO/Q==, figureFileBig=edz4A2d1Uzc76O6kCveaFw==, tableContent=null), ArticleFig(id=1175506412730987345, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图2, caption=原油各组分模型, figureFileSmall=M0jDwtBiAdpfYtS8JttO/Q==, figureFileBig=edz4A2d1Uzc76O6kCveaFw==, tableContent=null), ArticleFig(id=1175506412793901906, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.3, caption=Models of CO2 extraction of crude oil under different wettability conditions, figureFileSmall=oCehGj/ZLwuUXB3/NmSlqA==, figureFileBig=pigBX0Y0E3DIaCeog7OsNA==, tableContent=null), ArticleFig(id=1175506412852622163, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图3, caption=不同润湿性条件下CO2萃取原油模型

饱和烃 芳香烃 胶质 沥青质 CO2

, figureFileSmall=oCehGj/ZLwuUXB3/NmSlqA==, figureFileBig=pigBX0Y0E3DIaCeog7OsNA==, tableContent=null), ArticleFig(id=1175506412911342420, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.4, caption=CO2 extraction of hydroxylated SiO2 surfaces crude oil, figureFileSmall=AjYLlzValFgpE6pHRjy9vw==, figureFileBig=klkjF840mpVLoDClDgo0SQ==, tableContent=null), ArticleFig(id=1175506412974256981, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图4, caption=CO2萃取羟基化二氧化硅壁面原油过程

饱和烃 芳香烃 胶质 沥青质 CO2

, figureFileSmall=AjYLlzValFgpE6pHRjy9vw==, figureFileBig=klkjF840mpVLoDClDgo0SQ==, tableContent=null), ArticleFig(id=1175506413028782934, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.5, caption=CO2 extraction of methylated SiO2 surface crude oil, figureFileSmall=Ak0Zm6WTsOKKqkXHS0Jwnw==, figureFileBig=FaDqZj0NMv1ibYgZc7sTjw==, tableContent=null), ArticleFig(id=1175506413108474711, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图5, caption=CO2萃取甲基化二氧化硅壁面原油过程

饱和烃 芳香烃 胶质 沥青质 CO2

, figureFileSmall=Ak0Zm6WTsOKKqkXHS0Jwnw==, figureFileBig=FaDqZj0NMv1ibYgZc7sTjw==, tableContent=null), ArticleFig(id=1175506413179777880, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.6, caption=Number density distribution of each component of hydroxylated SiO2 surface model crude oil in the Z direction, figureFileSmall=5VUEMj8mIybMfcUSNXbckg==, figureFileBig=EFqKmAC9b/SLj8+PMxSPwQ==, tableContent=null), ArticleFig(id=1175506413234303833, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图6, caption=羟基化二氧化硅壁面模型原油各组分在Z方向上的数密度分布, figureFileSmall=5VUEMj8mIybMfcUSNXbckg==, figureFileBig=EFqKmAC9b/SLj8+PMxSPwQ==, tableContent=null), ArticleFig(id=1175506413293024090, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.7, caption=Number density distribution of each component of methylated SiO2 surface model crude oil in the Z direction, figureFileSmall=2XifslQNRTzPzM+snePfjQ==, figureFileBig=FRERbaB3fzapLX+qcU0ecA==, tableContent=null), ArticleFig(id=1175506413347550043, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图7, caption=甲基化二氧化硅壁面模型原油各组分在Z方向上的数密度分布, figureFileSmall=2XifslQNRTzPzM+snePfjQ==, figureFileBig=FRERbaB3fzapLX+qcU0ecA==, tableContent=null), ArticleFig(id=1175506413406270300, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.8, caption=Interaction energy between each component of crude oil and SiO2 surface varies with time, figureFileSmall=Z06S7rz2RQlZ0vlrcEEVSA==, figureFileBig=3C5k/Lm+bOl0a3MO1t3v6Q==, tableContent=null), ArticleFig(id=1175506413448213341, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图8, caption=原油各组分与二氧化硅壁面相互作用能随时间变化趋势, figureFileSmall=Z06S7rz2RQlZ0vlrcEEVSA==, figureFileBig=3C5k/Lm+bOl0a3MO1t3v6Q==, tableContent=null), ArticleFig(id=1175506413511127902, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Fig.9, caption=Mean square displacement of each component of crude oil in two surface models, figureFileSmall=/x+OJ5IG0AgMp5mBY7jLFA==, figureFileBig=v/6acBQHVD75oHG+5QJIZQ==, tableContent=null), ArticleFig(id=1175506413569848159, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=图9, caption=不同壁面模型中原油各组分均方位移, figureFileSmall=/x+OJ5IG0AgMp5mBY7jLFA==, figureFileBig=v/6acBQHVD75oHG+5QJIZQ==, tableContent=null), ArticleFig(id=1175506413620179808, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Table 1, caption=

Saturated hydrocarbon variation in two surface models

, figureFileSmall=null, figureFileBig=null, tableContent=
壁面
模型		 数密度/Å-3 下降/%
0 ns 1 ns 2 ns
—OH 4.049 935 3.387 399 2.950 623 27.14
—CH3 3.653 488 2.972 781 2.847 291 22.07
), ArticleFig(id=1175506413674705761, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=表1, caption=

两种壁面模型饱和烃变化情况

, figureFileSmall=null, figureFileBig=null, tableContent=
壁面
模型		 数密度/Å-3 下降/%
0 ns 1 ns 2 ns
—OH 4.049 935 3.387 399 2.950 623 27.14
—CH3 3.653 488 2.972 781 2.847 291 22.07
), ArticleFig(id=1175506413741814626, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=EN, label=Table 2, caption=

Diffusivity of each component of crude oil extracted by CO2 on two surfaces

, figureFileSmall=null, figureFileBig=null, tableContent=
壁面模型 饱和烃/(cm2·s-1) 芳香烃/(cm2·s-1) 胶质/(cm2·s-1) 沥青质/(cm2·s-1)
—OH 9.267 370×10-5 3.740 131×10-7 9.420 361×10-7 5.981 430×10-8
—CH3 7.255 657×10-5 1.672 625×10-6 4.211 183×10-6 2.959 136×10-7
), ArticleFig(id=1175506413825700707, tenantId=1146029695717560320, journalId=1146123166801305609, articleId=1149768948670972068, language=CN, label=表2, caption=

不同矿物壁面条件下CO2萃取原油各组分扩散系数

, figureFileSmall=null, figureFileBig=null, tableContent=
壁面模型 饱和烃/(cm2·s-1) 芳香烃/(cm2·s-1) 胶质/(cm2·s-1) 沥青质/(cm2·s-1)
—OH 9.267 370×10-5 3.740 131×10-7 9.420 361×10-7 5.981 430×10-8
—CH3 7.255 657×10-5 1.672 625×10-6 4.211 183×10-6 2.959 136×10-7
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润湿性对二氧化碳萃取原油组分的影响
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刘银庆 1 , 王玥琦 1, * , 马文国 1 , 杨瑞鑫 2 , 袁文航 1 , 刘璇 1
科学技术与工程 | 论文·石油、天然气工业 2025,25(15): 6297-6303
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科学技术与工程 | 论文·石油、天然气工业 2025, 25(15): 6297-6303
润湿性对二氧化碳萃取原油组分的影响
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刘银庆1 , 王玥琦1, * , 马文国1, 杨瑞鑫2, 袁文航1, 刘璇1
作者信息
  • 1 东北石油大学石油工程学院, 大庆 163318
  • 2 中国石化胜利油田东胜精攻石油开发集团有限公司, 东营 257000

    • 刘银庆(1971—),男,汉族,山东安丘人,硕士,副教授。研究方向:石油与天然气多相流动。E-mail:。

通讯作者:

* 王玥琦(1999—),女,汉族,黑龙江齐齐哈尔人,硕士研究生。研究方向:油气田开发,渗流理论。E-mail:。
Effect of Wettability on Carbon Dioxide Extraction of Crude Oil Components
Yin-qing LIU1 , Yue-qi WANG1, * , Wen-guo MA1, Rui-xin YANG2, Wen-hang YUAN1, Xuan LIU1
Affiliations
  • 1 School of Petroleum Engineering, Northeast Petroleum University, Daqing 163318, China
  • 2 Dongsheng Petroleum Development Group Company Ltd., Shengli Oilfield, Sinopec, Dongying 257000, China
出版时间: 2025-05-28 doi: 10.12404/j.issn.1671-1815.2406035
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摘要
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以砂岩中含量最高的二氧化硅为主要研究对象,对二氧化硅壁面分别进行了羟基(—OH)化和甲基(—CH3)化处理代表亲水和疏水壁面,运用LAMMPS软件进行分子动力学对超临界CO2萃取原油组分的过程进行模拟研究。结果表明:温度为333.15 K、压力为20 MPa时,超临界CO2萃取出羟基化二氧化硅壁面的饱和烃分子比甲基化二氧化硅壁面的多5.07%;原油组分与两种壁面的相互作用能均为吸引关系,饱和烃分子的相互作用能下降幅度最大分别为77.52%(羟基化二氧化硅壁面)和46.04%(甲基化二氧化硅壁面)且甲基化二氧化硅对饱和烃的相互作用能大于羟基化二氧化硅壁面;CO2容易萃取出分子链较短的饱和烃分子,原油组分在两种壁面条件下的扩散系数大小为饱和烃>胶质>芳香烃>沥青质。

超临界CO2  /  萃取  /  原油组分  /  分子动力学

The silica with the highest content in sandstone was taken as the main research object. The SiO2 surfaces underwent hydroxyl (—OH) and methyl (—CH3) treatments to represent the hydrophilic and hydrophobic walls, respectively. LAMMPS software was utilized to implement molecular dynamics simulations and replicate the process of supercritical CO2 extraction of crude oil components. The results indicate that the temperature is 333.15 K and the pressure is 20 MPa. The hydroxylated silica surface extracted 5.07% more saturated hydrocarbon molecules using supercritical CO2 compared to the methylated silica surface. The interaction energy between the oil components and the two wall surfaces is mutually attractive. The interaction energy of saturated hydrocarbon molecules decreases by 77.52% for hydroxylated silica surface and 46.04% for methylated silica surface, respectively. Additionally, the interaction energy of methylated silica on saturated hydrocarbon is greater than that of the hydroxylated silica surface.It is important to note that carbon dioxide easily extracts saturated hydrocarbons with short molecular chains. The diffusion coefficients of crude oil components under two surface conditions are saturated hydrocarbons > resins > aromatic hydrocarbons > asphaltenes.

supercritical CO2  /  extraction  /  crude oil components  /  molecular dynamics
刘银庆, 王玥琦, 马文国, 杨瑞鑫, 袁文航, 刘璇. 润湿性对二氧化碳萃取原油组分的影响. 科学技术与工程, 2025 , 25 (15) : 6297 -6303 . DOI: 10.12404/j.issn.1671-1815.2406035
Yin-qing LIU, Yue-qi WANG, Wen-guo MA, Rui-xin YANG, Wen-hang YUAN, Xuan LIU. Effect of Wettability on Carbon Dioxide Extraction of Crude Oil Components[J]. Science Technology and Engineering, 2025 , 25 (15) : 6297 -6303 . DOI: 10.12404/j.issn.1671-1815.2406035
正文
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随着中国对能源需求日益增加,石油作为重要能源之一,提高原油采收率技术在中国受到了重视。注气提高采收率技术发展迅速,其中又以注CO2技术的发展速度最快。注CO2提高原油采收率的效果非常明显而且利用CO2可以减轻温室效应[1],在驱油过程中还可以实现CO2的地质埋存,将温室气体CO2注入油藏用于驱油形成了碳循环利用模式,使温室气体变成了一种可利用的资源同时也符合可持续发展的理念[2]。
分子动力学(molecular dynamics,MD)是以牛顿经典力学为基础,再通过积分算法求解牛顿运动方程,最终可以得到随模拟时间变化的构型[3]。可以用于分析实验中难以研究的纳米尺度问题的数值模拟方法。根据所有粒子之间的相互作用势对体系内每个分子的运动进行计算,进一步分析系统内各个物质的微观行为。
CO2的现场应用最早开始于1956年,在美国Permain(二叠)盆地首先进行了注CO2混相驱替试验[4]。王朝[5]以分子动力学模拟方法研究了超临界二氧化碳驱在微观过程中,证实二氧化碳能够与岩石表面的羟基形成氢键而吸附在岩石表面,因此岩石壁面的原油分子会被剥离,与壁面分离。而二氧化碳能够萃取原油中的庚烷和甲苯,降低沥青质在原油中的溶解能力从而吸附壁面形成沉淀。杨琛[6]从微观角度采用分子动力学计算分析了吸附能的大小,得到了极性越强的原油组分与石英表面的吸附能也越大且其原油组分的极性越强更易于吸附于石英表面。
研究学者们多运用分子动力学对CO2驱替过程进行了多方面的研究,但针对不同基团对CO2萃取原油其组分的影响方面研究较少。基于此,运用LAMMPS软件通过分子动力学模拟方法,从微观角度基于同种矿物分别加亲水、疏水基团对CO2驱油机理开展研究,以期从微观角度揭示CO2驱替原油组分的影响。
1 分子动力学模拟
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从分子层面分析CO2分子与原油中各种烃类分子之间的相互作用力,在一定温压条件下通过模拟计算精确分析润湿性对萃取过程的影响这是传统实验难以细致观察到的。利用分子动力学模拟捕捉CO2萃取原油的瞬态行为,观察如何快速渗透到原油分子间隙并开始萃取原油组分,从模拟中得到的分子扩散系数可以预测油藏尺度的萃取效率是实现从分子特性到宏观采收率的关联预测。
1.1 研究思路
通过文献调研了解到砂岩油藏矿物组成,选择其中含量最多SiO2作为研究对象。LAMMPS软件是一款大规模原子分子并行模拟器,侧重于模拟分子和原子的运动。采用在SiO2壁面上进行完全羟基化与完全甲基化建立亲水和疏水的SiO2壁面模型以模拟不同润湿性。
先确定模拟所需模型的建立,选择合适的力场,根据牛顿第二定律计算分子的位置。随着模拟时间的推进,CO2分子与原油分子不断的碰撞和相互作用,由于CO2分子有一定的溶解性和扩散性,它能逐渐渗透到原油分子之间从而置换出原油分子。最终CO2萃取原油的程度可以从数密度、均方位移和扩散系数中得出原油组分分子在超临界CO2环境中是如何运动的。
1.2 模拟分子与模拟立场
选取SiO2分子作为致密砂岩储层壁面,并沿着(1 0 0)剖面进行切割,对SiO2壁面进行了羟基化[7]和甲基化[8]处理如图1所示,模拟亲水、疏水基团对CO2萃取原油的影响。拟体系的力场文件选择PCFF-INTERFACE[9]力场,系综采用正则系综(canonical ensemble,NVT),模拟单位为real,截断半径为12 Å,时间步长为1.0 fs。
X和Y方向(平行于壁面方向)采用周期性边界,Z方向(垂直于壁面方向)为非周期性边界,对油以及CO2组分采用Berendsen控温方式控制温度为333.15 K。模拟油分子式及组分参考SARA(Saturate,Aromatic,Resin,Asphaltene)原油模型[10-13]如图2所示,原油中各组分质量分数比例[14]按照原油组成进行模拟构建:饱和烃40.80%、芳香烃32.20%、胶质15.00%、沥青质11.90%。
先分别建立SiO2壁面模型(60 Å×60 Å×12 Å)、原油模型、CO2模型并导出模型文件。然后利用LAMMPS软件进行能量最小化后将模型组合到一起,将原油分子放置到壁面上,通过前期尝试准备工作发现模拟进行1.0 ns后原油与壁面系统可以达到稳定,之后将CO2分子与油壁模型组合到一起,进行0.4 ns的NVT模拟后,发现系统压力稳定在目标压力20 MPa,此时的CO2为超临界状态,所以将NVT模拟0.4 ns后的系统构型作为最终的初始构型,如图3所示,盒子大小60 Å×60 Å×173 Å,原子数约16 000个。
选取了羟基化二氧化硅、甲基化二氧化硅两种壁面条件下进行二氧化碳萃取原油模拟的0、1、2 ns 3个时间点原油各组分以及二氧化碳的位置分布情况如图4和图5所示。可以明显看到,原油组分中饱和烃组分得到了有效动用,被CO2萃取出并溶解到CO2相中,而原油组分中的芳香烃、胶质、沥青质并没有明显的变化。
2 模拟结果分析
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2.1 萃取过程模型数密度分布分析
如图6和图7所示分别为羟基化二氧化硅与甲基化二氧化硅壁面模型原油各组分沿Z方向的密度分布曲线,该曲线表示了分子沿垂直于壁面方向的位置变化情况。可以看到,各壁面模型中初始时刻大量的饱和烃分子位于壁面表面形成吸附层,随着模拟的进行,远离壁面的CO2相中饱和烃的数密度值升高,这说明位于壁面的饱和烃分子被逐渐萃取到CO2相中;模型中芳香烃分子在壁面到与壁面距离12 Å的位置之间数密度值升高幅度大于胶质和沥青质分子,羟基化二氧化硅壁面中芳香烃数密度增加24.94%,甲基化二氧化硅壁面中芳香烃数密度增加17.70%。
这是由于随着CO2分别萃取两种壁面原油组分模拟的进行,原本大量吸附在壁面附近的饱和烃分子被二氧化碳萃取出,附近的芳香烃分子“顶替”了饱和烃的位置,胶质和沥青质分子数密度值变化不大;在距离壁面12 Å乃至更远的位置时更多的胶质、沥青质组分则“顶替”了芳香烃的位置,使得数密度峰值略有升高。
为了更具体的比较两种壁面条件下CO2萃取饱和烃的差异,分别统计了各模型不同的模拟时间饱和烃数密度的变化,如表1所示。用初始时刻原油模型Z方向高度作为计算数密度的范围,取60 Å;拟采用积分法(面积)求下降情况,由于距离都是60 Å,求萃取率时约分后可抵消,则最终用数密度和来进行分析。
由此可以得到在羟基化二氧化硅壁面下饱和烃减少了27.14%,甲基化二氧化硅壁面下饱和烃减少了22.07%,CO2萃取羟基化二氧化硅壁面下原油时较萃取甲基化二氧化硅壁面时的萃取率高出18.68%;这是由于甲基是疏水基团,羟基是亲水基团,将二氧化硅壁面甲基化后与原油形成的油壁模型,吸附性比羟基化二氧化硅壁面更好,使得饱和烃在CO2萃取时不易被萃取出,数密度差值较小,萃取率低。
2.2 萃取过程模型相互作用能分析
用数密度分布分析得到CO2萃取羟基化二氧化硅壁面效果比甲基化二氧化硅壁面效果好,统计了两种壁面模型中原油各组分与壁面的相互作用能随时间变化的趋势,由相互作用能的变化可以反映出原油各组分被动用的情况,以及两种壁面下二氧化碳萃取效果的差异,如图8所示。
造成这种现象的原因是由于二氧化碳将大部分的饱和烃分子由壁面处萃取到二氧化碳体相中,导致饱和烃组分距离壁面更远,相互作用能减小,而大量的饱和烃分子被萃取出后,壁面附近出现了更多的空间,导致芳香烃、胶质、沥青质等大分子更贴近壁面,从而使得与两种壁面的相互作用能略微升高。
造成这种现象的原因是由于二氧化碳将大部分的饱和烃分子由壁面处萃取到二氧化碳体相中,导致饱和烃组分距离壁面更远,相互作用能减小,而大量的饱和烃分子被萃取出后,壁面附近出现了更多的空间,导致芳香烃、胶质、沥青质等大分子更贴近壁面,从而使得与两种壁面的相互作用能略微升高。
2.3 萃取过程模型均方位移(MSD)分析
在分子动力学模拟中,原子的热运动过程是无规则的,而且从模拟过程开始后便不会再静止。均方位移(mean square displacement, MSD)的物理意义就是对原子在一定时间内的平均运动状态进行统计,其定义式为
MSD=<|r(t)- r ( 0 ) 2>
式(1)中:r(t)为在t时刻的位置;r(0)为初始时刻位置。
通过对原油中各组分在不同矿物组分壁面条件下的均方位移曲线进行分析,进而我们可以明确两种壁面模型中原油各组分扩散能力的差异,如图9所示。
由图9可见,在两种壁面条件下,饱和烃组分的均方位移皆显著高于原油中的其他组分,胶质组分的均方位移略高于芳香烃和沥青质组分,这是由于饱和烃分子链较短,运动能力明显强于其他组分,并且大量的饱和烃分子被二氧化碳萃取到二氧化碳体相中,运动空间相比于其他组分要大得多,而原油中的其他组分由于与壁面的相互吸引,吸附在壁面表面并没有发生大面积的运移。
定义扩散系数D为
D= l i m t → ∞ 1 6 t<|r(t)- r ( 0 ) 2>
通过均方位移(MSD)与扩散系数D之间的关系,可求出原油中各组分在不同壁面模型CO2萃取条件下的扩散系数D,两种壁面下饱和烃的扩散系数如表2所示。在模拟CO2萃取原油过程中,CO2有效作用在饱和烃分子上,饱和烃分子的扩散系数最大,被动用情况最好。萃取过程的扩散系数大小为饱和烃>胶质>芳香烃>沥青质。
3 结论
收起
用LAMMPS软件进行分子动力学模拟,使用正则系综(canonical ensemble,NVT)在温度为333.15 K、压力20 MPa,弛豫0.4 ns,模拟时间2 ns条件下进行CO2萃取二氧化硅壁面原油组分的研究,得出以下结论。
(1)根据数密度曲线得出,在羟基化二氧化硅壁面下饱和烃减少了27.14%,甲基化二氧化硅壁面下饱和烃减少了22.07%,CO2萃取羟基化二氧化硅壁面下原油时较萃取甲基化二氧化硅壁面时的萃取率高出5.07%。由于甲基(—CH3)为疏水基团对原油的吸附性更好,使得饱和烃分子更不易被萃取出,由于大量的饱和烃分子被芳香烃分子CO2萃取到CO2相中,芳香烃优先“顶替”了饱和烃的位置,使得芳香烃的数密度在距离壁面12 Å附近处有所增加且羟基化二氧化硅壁面的芳香烃数密度比甲基化二氧化硅壁面下芳香烃数密度高7.24%。
(2)原油组分分别与两种壁面的相互作用能均为吸引关系,其中饱和烃的相互作用能下降幅度最大,分别为77.52%(羟基二氧化硅壁面)和46.04%(甲基化二氧化硅壁面),出于相互作用能与距离成反比,饱和烃分子被CO2萃取的多,距离壁面距离远,所以饱和烃分子的相互作用能下降最大。由于饱和烃分子质量相对较小、分子结构简单、自身体积小易被CO2萃取到二氧化碳相中,而芳香烃的相互用能升高的原因是大量的饱和烃被萃取后远离壁面芳香烃“顶替”了饱和烃的位置导致芳香烃的相互作用能升高。
(3)原油组分在两种壁面条件下的扩散系数大小均为饱和烃>胶质>芳香烃>沥青质,芳香烃“顶替”了最初时刻油膜中吸附在壁面周围的饱和烃的位置而原本芳香烃所在位置有所“空余”胶质运动的空间加大导致芳香烃扩散系数小于胶质,而沥青质扩散系数最小被动用情况最差。
综上所述,超临界二氧化碳对羟基化二氧化硅壁面条件下的原油动用情况优于甲基化二氧化硅壁面,说明在矿物壁面亲水环境的萃取效果优于亲油环境,在实践中超临界二氧化碳萃取原油技术应优先用于亲水矿物壁面环境中,也就是水驱结束后。
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doi: 10.12404/j.issn.1671-1815.2406035
  • 接收时间：2024-08-12
  • 首发时间：2025-07-09
  • 出版时间：2025-05-28
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  • 收稿日期：2024-08-12
  • 修回日期：2025-01-24
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    1 东北石油大学石油工程学院, 大庆 163318
    2 中国石化胜利油田东胜精攻石油开发集团有限公司, 东营 257000

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* 王玥琦(1999—),女,汉族,黑龙江齐齐哈尔人,硕士研究生。研究方向:油气田开发,渗流理论。E-mail:。
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2种不同金属材料的力学参数
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species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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