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Article(id=1309631420822291078, tenantId=1146029695717560320, journalId=1308397254396182630, issueId=1309631419949871909, articleNumber=null, orderNo=null, doi=10.3724/2097-213X.2025.JFCT.0034, pmid=null, cstr=32157.14.2097-213X.2025.JFCT.0191, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1761148800000, receivedDateStr=2025-10-23, revisedDate=1763827200000, revisedDateStr=2025-11-23, acceptedDate=1764777600000, acceptedDateStr=2025-12-04, onlineDate=1790170062498, onlineDateStr=2026-09-23, pubDate=1781020800000, pubDateStr=2026-06-10, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1790170062498, onlineIssueDateStr=2026-09-23, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1790170062498, creator=13701087609, updateTime=1790170062498, updator=13701087609, issue=Issue{id=1309631419949871909, tenantId=1146029695717560320, journalId=1308397254396182630, year='2026', volume='54', issue='6', pageStart='20250266-977', pageEnd='20260007-1065', issueExtLink='null', onlineDate='null', pubDate='1781020800000', pubDateStr='2026-06-10', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1790170062291, creator='13701087609', updateTime=1790212893756, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1309811068180984192, tenantId=1146029695717560320, journalId=1308397254396182630, issueId=1309631419949871909, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1309811068185178497, tenantId=1146029695717560320, journalId=1308397254396182630, issueId=1309631419949871909, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=20250304-1097, endPage=20250304-1108, ext={EN=ArticleExt(id=1309631424395838087, articleId=1309631420822291078, tenantId=1146029695717560320, journalId=1308397254396182630, language=EN, title=Effects of zeolite type and acidic properties on the catalytic cracking performance of dodecane, columnId=null, journalTitle=Journal of Fuel Chemistry and Technology, columnName=null, runingTitle=null, highlight=null, articleAbstract=

Catalytic cracking of gasoline and diesel to produce olefins is crucial for the high-value utilization of surplus fuels. This process typically employs zeolite catalysts. In order to reveal the effects of zeolite type and acidic properties on the catalytic cracking performance for the diesel model compound dodecane, SAPO-34, ZSM-5-38 (SiO2/Al2O3 ratio of 38, the same below), ZSM-5-85, ZSM-5-200 and USY were taken as research subjects. These zeolites were characterized by X-ray diffraction, scanning electron microscope, N2 physical adsorption, NH3-temperature programmed desorption and pyridine adsorption Fourier-transform infrared spectroscopy, and their catalytic cracking performance was systematically evaluated on a fixed-bed reactor. Results indicated that the zeolite type was the primary determinant of dodecane conversion and product distribution. SAPO-34, with a 0.38 nm pore size, exhibited low catalytic activity, achieving a dodecane conversion of 24.33% and nearly zero BTX aromatics yield. Although SAPO-34 showed high light olefins selectivity, severe coking occurred on its external surface. In contrast, ZSM-5-38, with a moderate pore size and acid amounts, demonstrated excellent catalytic activity, achieving nearly 100% dodecane conversion. Its liquid products were predominantly BTX aromatics, with the relatively highest light olefins yield of 18.40% and minimal coke yield of 0.18% among the three different zeolites. USY, featuring the largest pore size, also fully converted dodecane but primarily produced light alkanes and coke. Secondly, based on the identified zeolite type, adjusting the acidic properties could further refine product distribution. Experimental data indicated that the number of acid sites in ZSM-5, especially the Brønsted acid sites, decreased as the SiO2/Al2O3 ratio increased. Among ZSM-5 with different acidic properties, ZSM-5-200 showed superior catalytic cracking performance for dodecane, achieving a total gas product yield nearing 65% and a conversion of 97.79%. Additionally, the yields of ethylene, propylene and butene rose to 11.11%, 20.33% and 10.49% respectively, while maintaining a low coke yield of 0.43%. Finally, based on the above findings, the reaction pathway and regulation mechanism of dodecane catalytic cracking were proposed, including cracking, hydrogen transfer, oligomerization, aromatization and coking. The zeolite type and its acidic properties significantly influenced the conversion and product distribution by modulating the relative strength of these reactions. This study elucidates the structure-activity relationship between zeolite type, acidic properties and catalytic performance, enhances the understanding of catalytic reaction mechanisms and guides the optimization of gasoline and diesel catalytic cracking processes toward olefins production.

, authors=Wenshuo MA, Zhihao YANG, Mengxin CHEN, Jingxian WANG, Yuanyu TIAN*, Yingyun QIAO*, authorsList=Wenshuo MA, Zhihao YANG, Mengxin CHEN, Jingxian WANG, Yuanyu TIAN, Yingyun QIAO, authorCompany=null, correspAuthors=Yuanyu TIAN, Yingyun QIAO, authorNote=null, correspAuthorsNote=null, copyrightStatement=Copyright ©2026 Journal of Fuel Chemistry and Technology. All rights reserved., 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, fund=null), CN=ArticleExt(id=1309631430607602344, articleId=1309631420822291078, tenantId=1146029695717560320, journalId=1308397254396182630, language=CN, title=分子筛类型及酸性质对十二烷催化裂解性能的影响, columnId=1309584910000677174, journalTitle=燃料化学学报（中英文）, columnName=RESEARCH PAPER, runingTitle=null, highlight=null, articleAbstract=

汽柴油催化裂解制烯烃技术是实现过剩汽柴油高值化利用的重要途径，该工艺通常采用分子筛催化剂。为揭示分子筛类型及酸性质对柴油模型化合物十二烷催化裂解性能的影响，以SAPO-34、ZSM-5-38（硅铝比为38，下同）、ZSM-5-85、ZSM-5-200及USY为研究对象，通过X射线衍射、扫描电子显微镜、N2低温吸附-脱附、NH3程序升温脱附、吡啶吸附红外光谱等手段表征分析其物化性质，并利用固定床装置考察了其催化裂解性能。研究表明，分子筛类型是决定十二烷转化率及产物分布的首要因素。其中，SAPO-34催化活性较低而ZSM-5-38和USY基本实现了十二烷的完全转化；同时，在这三种不同类型的分子筛中，ZSM-5-38展现出相对最高的总低碳烯烃收率，达18.40%。其次，在明确分子筛类型的基础上，通过酸性质的调变可进一步优化产物分布。实验结果表明，在不同酸性质的ZSM-5中，低酸量的ZSM-5-200具有更优的十二烷催化裂解性能，在实现97.79%高转化率的同时，总低碳烯烃收率显著提升至41.93%。基于上述研究提出了十二烷催化裂解的反应路径及调控机制。

, authors=马文硕, 杨志濠, 陈梦鑫, 王敬贤, 田原宇*, 乔英云*, authorsList=马文硕, 杨志濠, 陈梦鑫, 王敬贤, 田原宇, 乔英云, authorCompany=null, correspAuthors=田原宇, 乔英云, authorNote=

马文硕（1999），博士研究生，研究方向为石油烃类的热裂解及催化裂解转化，

田原宇（1969），博士，教授，主要从事煤化工、生物质、重油加工、反应装置方面的研究工作，

乔英云（1979），博士，教授，主要从事碳基能源热化学转化与利用方面的研究工作，

, correspAuthorsNote=
Tel: 0532-86057766, 13792454906, E-mail:
, copyrightStatement=版权所有©燃料化学学报(中英文) 2026, copyrightOwner=null, extLink=null, articleAbsUrl=null, sourceXml=oxW3Jyoh2JvHW8mE8keKCA==, magXml=Y/wI7k5xVlinoZ8qphLMPQ==, pdfUrl=null, pdf=7mA+EdX6OXvyZX8LfS/WCQ==, pdfFileSize=4712406, pdfExtLink=null, richHtmlUrl=null, mobilePdfUrl=null, reviewReport=null, pdfFirstPage=null, abstractGraph=Sd0LitK0wdrUdayxIRMypg==, abstractGraphContent=null, abstractVideo=null, citation=null, cebUrl=null, magXmlContent=424ZnQz3MUS+byhLGBTkuA==, mapNumber=null, fund=null)}, authors=[Author(id=1309631431454851757, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, orderNo=0, firstName=null, middleName=null, lastName=null, nameCn=null, orcid=null, stid=null, country=null, authorPic=null, dead=0, email=546511068@qq.com, emailSecond=null, emailThird=null, correspondingAuthor=0, authorType=1, ext={EN=AuthorExt(id=1309631433149350577, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, authorId=1309631431454851757, language=EN, stringName=Wenshuo MA, firstName=Wenshuo, middleName=null, lastName=MA, prefix=null, suffix=null, authorComment=null, nameInitials=null, affiliation=null, department=null, xref=null, address=State Key Laboratory of Heavy Oil Processing, School of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China, bio=null, bioImg=null, bioContent=null, aboutCorrespAuthor=null), CN=AuthorExt(id=1309631433233236658, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, authorId=1309631431454851757, language=CN, stringName=马文硕, firstName=null, middleName=null, lastName=null, prefix=null, suffix=null, authorComment=null, nameInitials=null, affiliation=null, department=null, xref=null, address=中国石油大学(华东) 化学化工学院 重质油全国重点实验室, 山东 青岛 266580, bio={"img":"uNciDOniY3q0ILDLnOyuPw==","content":"

马文硕（1999），博士研究生，研究方向为石油烃类的热裂解及催化裂解转化，

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马文硕（1999），博士研究生，研究方向为石油烃类的热裂解及催化裂解转化，

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田原宇（1969），博士，教授，主要从事煤化工、生物质、重油加工、反应装置方面的研究工作，

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田原宇（1969），博士，教授，主要从事煤化工、生物质、重油加工、反应装置方面的研究工作，

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乔英云（1979），博士，教授，主要从事碳基能源热化学转化与利用方面的研究工作，

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乔英云（1979），博士，教授，主要从事碳基能源热化学转化与利用方面的研究工作，

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J Porous Mater, 2021, 28: 1059−1067., articleTitle=null, refAbstract=null)], funds=null, companyList=[AuthorCompany(id=1309631431127696041, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, xref=null, ext=[AuthorCompanyExt(id=1309631431136084650, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, companyId=1309631431127696041, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=State Key Laboratory of Heavy Oil Processing, School of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China), AuthorCompanyExt(id=1309631431148667563, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, companyId=1309631431127696041, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=中国石油大学(华东) 化学化工学院 重质油全国重点实验室, 山东 青岛 266580)])], figs=[ArticleFig(id=1309631438861992664, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=EN, label=Fig.1, caption=XRD patterns of different zeolite catalysts, figureFileSmall=MWgA69PRwXr+6o+aHnTiUA==, figureFileBig=Sd0LitK0wdrUdayxIRMypg==, tableContent=null), ArticleFig(id=1309631438950073049, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=CN, label=图1, caption=不同分子筛催化剂的XRD谱图, figureFileSmall=MWgA69PRwXr+6o+aHnTiUA==, figureFileBig=Sd0LitK0wdrUdayxIRMypg==, tableContent=null), ArticleFig(id=1309631439155593946, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=EN, label=Fig.2, caption=SEM images of different zeolite catalysts, figureFileSmall=ztj/k9UZ2K9mQIK5Q5fw/w==, figureFileBig=2sO3th5uk6NCDJACQ67PNw==, tableContent=null), ArticleFig(id=1309631439226897115, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=CN, label=图2, caption=不同分子筛催化剂的SEM图像

(a): SAPO-34; (b): ZSM-5-38; (c): ZSM-5-85;(d): ZSM-5-200; (e): USY.

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Reaction conditions: m (catalyst) = 3.6 g; p = 101.325 kPa; t = 600 ℃; WHSV = 14 h−1.

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Textural properties of different zeolite catalysts

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SampleSpecific surface area/(m2·g−1)Pore volume/(cm3·g−1)Pore diameter/nm
totalmicromesototalmicromeso
SAPO-34752735170.290.270.020.38
ZSM-5-38360300600.180.120.060.55
ZSM-5-85403353500.220.150.070.55
ZSM-5-200412360520.190.140.050.55
USY467402650.240.160.080.73
), ArticleFig(id=1309631442364236526, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=CN, label=表1, caption=

不同分子筛催化剂的织构特性

, figureFileSmall=null, figureFileBig=null, tableContent=
SampleSpecific surface area/(m2·g−1)Pore volume/(cm3·g−1)Pore diameter/nm
totalmicromesototalmicromeso
SAPO-34752735170.290.270.020.38
ZSM-5-38360300600.180.120.060.55
ZSM-5-85403353500.220.150.070.55
ZSM-5-200412360520.190.140.050.55
USY467402650.240.160.080.73
), ArticleFig(id=1309631442460705519, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=EN, label=Table2, caption=

Acidic properties of different zeolite catalysts

, figureFileSmall=null, figureFileBig=null, tableContent=
SampleAcidity by NH3-TPD/(μmol·g−1)Acidity by Py-FTIR/(μmol·g−1)
total acidweak acidstrong acidS/WaBrønsted acidLewis acidB/Lb
a: S/W = Number of strong acid sites / Number of weak acid sites; b: B/L= Number of Brønsted acid sites / Number of Lewis acid sites.
SAPO-344251662591.6−−−
ZSM-5-38181115660.6140413.1
ZSM-5-8510846621.366421.6
ZSM-5-2005418362.025290.9
USY285191940.5193922.1
), ArticleFig(id=1309631442527814384, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=CN, label=表2, caption=

不同分子筛催化剂的酸性质

, figureFileSmall=null, figureFileBig=null, tableContent=
SampleAcidity by NH3-TPD/(μmol·g−1)Acidity by Py-FTIR/(μmol·g−1)
total acidweak acidstrong acidS/WaBrønsted acidLewis acidB/Lb
a: S/W = Number of strong acid sites / Number of weak acid sites; b: B/L= Number of Brønsted acid sites / Number of Lewis acid sites.
SAPO-344251662591.6−−−
ZSM-5-38181115660.6140413.1
ZSM-5-8510846621.366421.6
ZSM-5-2005418362.025290.9
USY285191940.5193922.1
), ArticleFig(id=1309631442586534641, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=EN, label=Table3, caption=

Product distribution by dodecane catalytic cracking over different zeolite catalysts

, figureFileSmall=null, figureFileBig=null, tableContent=
Samplex /%yi /%
total gasdry gasliquid gastotal liquidgasolinedieselcoke
Reaction conditions: m (catalyst) = 3.6 g; p = 101.325 kPa; t = 600 ℃; WHSV = 14 h−1; reaction cycle = 1.
Silica16.2710.934.886.055.323.921.400.03
SAPO-3424.3317.347.0610.285.103.601.501.89
ZSM-5-3899.3258.1422.6635.4841.0040.880.120.18
USY99.3163.1724.6038.5723.2422.400.8412.90
), ArticleFig(id=1309631442683003634, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=CN, label=表3, caption=

不同分子筛催化剂上十二烷催化裂解产物分布

, figureFileSmall=null, figureFileBig=null, tableContent=
Samplex /%yi /%
total gasdry gasliquid gastotal liquidgasolinedieselcoke
Reaction conditions: m (catalyst) = 3.6 g; p = 101.325 kPa; t = 600 ℃; WHSV = 14 h−1; reaction cycle = 1.
Silica16.2710.934.886.055.323.921.400.03
SAPO-3424.3317.347.0610.285.103.601.501.89
ZSM-5-3899.3258.1422.6635.4841.0040.880.120.18
USY99.3163.1724.6038.5723.2422.400.8412.90
), ArticleFig(id=1309631442766889715, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=EN, label=Table4, caption=

Product distribution by dodecane catalytic cracking over ZSM-5 with different SiO2/Al2O3 ratios

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Samplex /%yi /%
total gasdry gasliquid gastotal liquidgasolinedieselcoke
Reaction conditions: m (catalyst) = 3.6 g; p = 101.325 kPa; t = 600 ℃; WHSV = 14 h−1; reaction cycle = 1.
ZSM-5-3899.3258.1422.6635.4841.0040.880.120.18
ZSM-5-8599.8464.6420.7043.9335.0034.500.510.20
ZSM-5-20097.7964.9916.3748.6132.3731.840.540.43
), ArticleFig(id=1309631442863358708, tenantId=1146029695717560320, journalId=1308397254396182630, articleId=1309631420822291078, language=CN, label=表4, caption=

不同硅铝比ZSM-5上十二烷催化裂解产物分布

, figureFileSmall=null, figureFileBig=null, tableContent=
Samplex /%yi /%
total gasdry gasliquid gastotal liquidgasolinedieselcoke
Reaction conditions: m (catalyst) = 3.6 g; p = 101.325 kPa; t = 600 ℃; WHSV = 14 h−1; reaction cycle = 1.
ZSM-5-3899.3258.1422.6635.4841.0040.880.120.18
ZSM-5-8599.8464.6420.7043.9335.0034.500.510.20
ZSM-5-20097.7964.9916.3748.6132.3731.840.540.43
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分子筛类型及酸性质对十二烷催化裂解性能的影响
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马文硕 , 杨志濠 , 陈梦鑫 , 王敬贤 , 田原宇 * , 乔英云 *
燃料化学学报（中英文） | RESEARCH PAPER 2026,54(6): 20250304-1097-20250304-1108
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燃料化学学报（中英文） |RESEARCH PAPER 2026 , 54 (6) : 20250304-1097 -20250304-1108
分子筛类型及酸性质对十二烷催化裂解性能的影响
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马文硕 , 杨志濠, 陈梦鑫, 王敬贤, 田原宇* , 乔英云*
作者信息
  • 中国石油大学(华东) 化学化工学院 重质油全国重点实验室, 山东 青岛 266580
通讯作者:
Tel: 0532-86057766, 13792454906, E-mail:
作者简介:

马文硕（1999），博士研究生，研究方向为石油烃类的热裂解及催化裂解转化，

田原宇（1969），博士，教授，主要从事煤化工、生物质、重油加工、反应装置方面的研究工作，

乔英云（1979），博士，教授，主要从事碳基能源热化学转化与利用方面的研究工作，

Effects of zeolite type and acidic properties on the catalytic cracking performance of dodecane
Wenshuo MA , Zhihao YANG, Mengxin CHEN, Jingxian WANG, Yuanyu TIAN* , Yingyun QIAO*
Affiliations
  • State Key Laboratory of Heavy Oil Processing, School of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
出版时间: 2026-06-10 doi: 10.3724/2097-213X.2025.JFCT.0034
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摘要
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汽柴油催化裂解制烯烃技术是实现过剩汽柴油高值化利用的重要途径，该工艺通常采用分子筛催化剂。为揭示分子筛类型及酸性质对柴油模型化合物十二烷催化裂解性能的影响，以SAPO-34、ZSM-5-38（硅铝比为38，下同）、ZSM-5-85、ZSM-5-200及USY为研究对象，通过X射线衍射、扫描电子显微镜、N2低温吸附-脱附、NH3程序升温脱附、吡啶吸附红外光谱等手段表征分析其物化性质，并利用固定床装置考察了其催化裂解性能。研究表明，分子筛类型是决定十二烷转化率及产物分布的首要因素。其中，SAPO-34催化活性较低而ZSM-5-38和USY基本实现了十二烷的完全转化；同时，在这三种不同类型的分子筛中，ZSM-5-38展现出相对最高的总低碳烯烃收率，达18.40%。其次，在明确分子筛类型的基础上，通过酸性质的调变可进一步优化产物分布。实验结果表明，在不同酸性质的ZSM-5中，低酸量的ZSM-5-200具有更优的十二烷催化裂解性能，在实现97.79%高转化率的同时，总低碳烯烃收率显著提升至41.93%。基于上述研究提出了十二烷催化裂解的反应路径及调控机制。

十二烷  /  催化裂解  /  分子筛类型  /  酸性质  /  低碳烯烃

Catalytic cracking of gasoline and diesel to produce olefins is crucial for the high-value utilization of surplus fuels. This process typically employs zeolite catalysts. In order to reveal the effects of zeolite type and acidic properties on the catalytic cracking performance for the diesel model compound dodecane, SAPO-34, ZSM-5-38 (SiO2/Al2O3 ratio of 38, the same below), ZSM-5-85, ZSM-5-200 and USY were taken as research subjects. These zeolites were characterized by X-ray diffraction, scanning electron microscope, N2 physical adsorption, NH3-temperature programmed desorption and pyridine adsorption Fourier-transform infrared spectroscopy, and their catalytic cracking performance was systematically evaluated on a fixed-bed reactor. Results indicated that the zeolite type was the primary determinant of dodecane conversion and product distribution. SAPO-34, with a 0.38 nm pore size, exhibited low catalytic activity, achieving a dodecane conversion of 24.33% and nearly zero BTX aromatics yield. Although SAPO-34 showed high light olefins selectivity, severe coking occurred on its external surface. In contrast, ZSM-5-38, with a moderate pore size and acid amounts, demonstrated excellent catalytic activity, achieving nearly 100% dodecane conversion. Its liquid products were predominantly BTX aromatics, with the relatively highest light olefins yield of 18.40% and minimal coke yield of 0.18% among the three different zeolites. USY, featuring the largest pore size, also fully converted dodecane but primarily produced light alkanes and coke. Secondly, based on the identified zeolite type, adjusting the acidic properties could further refine product distribution. Experimental data indicated that the number of acid sites in ZSM-5, especially the Brønsted acid sites, decreased as the SiO2/Al2O3 ratio increased. Among ZSM-5 with different acidic properties, ZSM-5-200 showed superior catalytic cracking performance for dodecane, achieving a total gas product yield nearing 65% and a conversion of 97.79%. Additionally, the yields of ethylene, propylene and butene rose to 11.11%, 20.33% and 10.49% respectively, while maintaining a low coke yield of 0.43%. Finally, based on the above findings, the reaction pathway and regulation mechanism of dodecane catalytic cracking were proposed, including cracking, hydrogen transfer, oligomerization, aromatization and coking. The zeolite type and its acidic properties significantly influenced the conversion and product distribution by modulating the relative strength of these reactions. This study elucidates the structure-activity relationship between zeolite type, acidic properties and catalytic performance, enhances the understanding of catalytic reaction mechanisms and guides the optimization of gasoline and diesel catalytic cracking processes toward olefins production.

dodecane  /  catalytic cracking  /  zeolite type  /  acidic properties  /  light olefins
马文硕, 杨志濠, 陈梦鑫, 王敬贤, 田原宇, 乔英云. 分子筛类型及酸性质对十二烷催化裂解性能的影响. 燃料化学学报（中英文）, 2026 , 54 (6) : 20250304-1097 -20250304-1108 . DOI: 10.3724/2097-213X.2025.JFCT.0034
Wenshuo MA, Zhihao YANG, Mengxin CHEN, Jingxian WANG, Yuanyu TIAN, Yingyun QIAO. Effects of zeolite type and acidic properties on the catalytic cracking performance of dodecane[J]. Journal of Fuel Chemistry and Technology, 2026 , 54 (6) : 20250304-1097 -20250304-1108 . DOI: 10.3724/2097-213X.2025.JFCT.0034
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伴随“双碳”目标的提出，汽车电动化进程显著加速，势必会带来汽柴油等传统燃料油品消费量的大幅下降[1−3]，如何实现过剩汽柴油资源的高附加值转化，已成为亟待解决的行业痛点。同时，2023年中国炼油总产能已达9.32亿吨，结构性产能过剩矛盾持续加剧[4−5]，致使部分石化企业面临汽柴油出厂压力不断加大的局面。在此背景下，乙烯、丙烯及丁烯等低碳烯烃作为关键性基础化工原料[6−7]，在高分子聚合物、合成纤维、塑料、橡胶等诸多领域应用广泛，市场需求呈逐年增长态势[8−12]。因此，开发汽柴油等富余燃料油品高效转化制低碳烯烃技术，不仅契合迫切的现实需求，更对优化石化产业结构、提升资源利用价值、驱动行业转型升级具有重大的战略意义。
当前，汽柴油制烯烃领域的研究主要聚焦于催化裂解技术，其核心在于高效催化剂的设计与开发[13−14]。分子筛基催化剂凭借优异的裂解活性、择形的孔道结构与可调的酸性中心备受关注[15−17]。研究表明，分子筛拓扑结构类型对催化裂解产物分布具有特定的导向作用[18]。李凤岭等[19]考察了FER、FAU、AFI、MFI、AEL、TON、BEA等不同构型分子筛对加氢裂化尾油的催化裂解性能，发现反应转化率受分子筛孔径尺寸与孔道结构的双重调控。其中，SAPO-11分子筛因自身独特的一维孔道结构（孔径尺寸为0.40 nm × 0.65 nm）展现出最优催化裂解性能。魏晓丽等[20]在固定流化床上探究了分子筛类型对正庚烷裂解的影响，结果表明，ZRP分子筛较Y型与Beta分子筛更利于裂解反应的进行，原料转化率显著增加。此外，分子筛酸性质亦对催化裂解性能有显著影响[21]。韩蕾等[22]以硅铝比为24的ZSM-5为母体，通过酸处理脱铝的方式制得了系列不同酸量的ZSM-5分子筛，用于正辛烷和乙基环己烷的催化裂解研究。结果表明，两种模型化合物的转化率均与ZSM-5总酸量呈正相关，但过高的酸量会导致低碳烯烃收率及选择性的降低。Ramesh等[23]在固定床反应器上研究发现，十二烷催化裂解转化率随Beta分子筛Brønsted酸量的增加单调递减，当以高硅铝比的Beta分子筛作为催化剂时，轻质烯烃收率达到较高水平。
综上所述，分子筛类型与酸性质是影响催化裂解反应路径、反应活性及产物分布的关键因素，然而其内在作用机制尚缺乏系统认知。因此，为深入揭示分子筛类型与酸性质在催化裂解过程中的内在作用机制，本研究选取了三种代表性的工业常用分子筛，即CHA构型的SAPO-34、MFI构型的ZSM-5和FAU构型的USY，构建了在孔道结构与酸性质方面具有显著差异的对比研究体系。三种分子筛的孔径依次增大，覆盖了反应物分子从扩散严重受限到高度可及的传质区间；在酸性质方面，SAPO-34通常富含强酸位点，USY以弱酸为主，而ZSM-5的酸性质可通过硅铝比实现灵活调节，从而在酸性质上形成有效系统的对比。基于此，本研究以直链十二烷为典型柴油模型化合物，探究了SAPO-34、ZSM-5、USY三种分子筛的催化裂解行为，进而考察了ZSM-5酸性质对其反应性能的影响规律，最终通过产物分布分析构建了十二烷催化裂解的反应路径及其调控机制。研究阐明了分子筛类型及酸性质与催化性能间的构效关系，为汽柴油高效转化制烯烃技术路线提供了重要的理论依据与实验基础。
1　实验部分
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1.1　原料与试剂
H型SAPO-34（硅铝比为0.5）、ZSM-5-38、ZSM-5-85、ZSM-5-200及USY（硅铝比为6）分子筛，均购自天津南化催化剂有限公司，使用前，各分子筛在800 ℃马弗炉中焙烧处理4 h；十二烷（C12H26，纯度为98%），购自上海阿拉丁生化科技股份有限公司。
1.2　分析表征
采用德国Bruker公司的D8 Advance X射线衍射仪分析样品的物相组成，以Cu Kα射线为辐射源（波长为0.1542 nm），工作电流40 mA，工作电压40 kV，5°−45°扫描。采用日本电子株式会社的JSM-7900F型热场发射扫描电子显微镜观测样品的表观形貌及颗粒尺寸。采用美国Micromeritics公司的ASAP 2460全自动比表面积和孔隙度分析仪表征样品的孔结构，样品经300 ℃真空脱气4 h后在77 K下以氮气为吸附质检测吸附-脱附等温线，并根据BET法计算总比表面积，通过t-plot法得到微孔比表面积及微孔孔容。采用天津先权工贸发展有限公司的TP-5080-D全自动多用吸附仪（配备TCD检测器）测定样品的酸量及酸强度，取0.1 g样品置于石英管中部，首先在氦气流中300 ℃预处理2 h，降温至110 ℃并切换通入10%的氨氦混合气吸附40 min，切换回氦气吹扫，同时程序升温（110−700 ℃）脱附氨气，记录得到样品的NH3-TPD谱图。使用德国Bruker公司的VERTEX70V红外光谱仪分析样品的酸类型，使用专用模具将10−15 mg待测样品压成自支撑片后置于真空红外原位池的中部恒温区，在真空下500 ℃预处理1 h，冷却至150 ℃采集谱图背景，采集完成后继续冷至室温进行40 min的吸附吡啶处理，升温至150 ℃脱附吡啶分子并记录谱图。使用日本岛津公司的SHIMADZU DTG-60H差热-热重同步分析仪测定反应后催化剂的热失重曲线及微分热失重曲线。使用中国雷尼绍公司的inVia Qontor原位激光共聚焦拉曼光谱仪（配备325 nm紫外激光器）表征反应后催化剂上积炭的有序程度。
1.3　催化剂反应性能评价及产物分析
在固定床反应器上评价催化剂的十二烷催化裂解性能。将3.6 g催化剂颗粒（20−40目）装填于反应器恒温段，在压力101.325 kPa、温度600 ℃及质量空速（Weight hour space velocity，WHSV）14 h−1的条件下进行反应。生成的油气经两级冷凝冷却后分离为气相和液相产物。气相产物采用SCION 8500 GC型气相色谱仪分析，液相产物的馏程和化学组成则分别通过SCION 436 GC型模拟蒸馏仪和SCION 8500GC-8700SQ型气质联用仪表征。反应后催化剂的积炭含量利用南京华欣分析仪器公司的HX-HW8型高频红外碳硫分析仪准确测定。
催化裂解反应以十二烷转化率（x，%）和各产物收率（yi，%）为评价指标，计算公式如下所示：
$ x=\dfrac{{{m}}_{{0}}-{{m}}_{{1}}}{{{m}}_{{0}}}{\times }{100}{ }{\%} $
$ {{y}}_{{i}}=\dfrac{{{m}}_{{i}}}{{{m}}_{\text{0}}}{\times}{100}{\%} $
式中：m0为原料总质量，g；m1为产物中十二烷质量，g；mi为产物i质量，g。
2　结果与讨论
收起
2.1　分子筛催化剂物化性质表征
2.1.1　分子筛催化剂的物相分析
图1为不同分子筛催化剂的X射线衍射（XRD）谱图。其中，SAPO-34分子筛呈现出典型的CHA拓扑结构特征衍射峰；而不同硅铝比的ZSM-5分子筛均观察到明显的MFI结构特征衍射峰；此外，USY分子筛的特征衍射峰归属于FAU八面沸石构型。值得注意的是，所有样品的XRD谱图中均无杂晶相存在，说明样品的物相组成单一，纯度较高。
2.1.2　分子筛催化剂的表观形貌分析
图2为不同分子筛催化剂的扫描电子显微镜（SEM）图像。结果显示，各分子筛在表观形貌上存在显著差异。具体而言，SAPO-34分子筛呈现尺寸为6−10 μm的立方体形貌；ZSM-5系列分子筛形貌较为一致，均由棺状的颗粒堆积组成，其粒径分布在1−5 μm；USY分子筛则由1 μm左右的类八面体颗粒团聚构成。
2.1.3　分子筛催化剂的孔道结构分析
利用N2低温吸附-脱附技术表征不同分子筛催化剂的孔道结构，结果如图3所示。SAPO-34呈现I型等温线特征，为典型的微孔材料；而ZSM-5-38、ZSM-5-85、ZSM-5-200和USY兼具I型与IV型等温线特征，并在相对压力（p/p0）为0.45−0.95出现明显的H4型滞后回环，表明其具有微孔-介孔复合结构。DFT孔径分布进一步显示，八元环孔道的SAPO-34孔径最小（0.38 nm），十元环孔道的ZSM-5-38、ZSM-5-85和ZSM-5-200孔径居中（0.55 nm），而十二元环孔道的USY孔径最大（0.73 nm）。表1汇总了上述样品的织构特性。结果显示，五种分子筛均以微孔为主，其中，SAPO-34的总比表面积（752 m2/g）和微孔比表面积（735 m2/g）最大，USY次之，而ZSM-5系列相对较低。孔容分布规律类似，总孔容和微孔孔容由大到小依次为：SAPO-34 > USY > ZSM-5-85 > ZSM-5-200 > ZSM-5-38。此外，SAPO-34几乎不含介孔结构，而其余四种分子筛的介孔比表面积（50−65 m2/g）和介孔孔容（0.05−0.08 cm3/g）相近。
2.1.4　分子筛催化剂的酸性质分析
采用NH3程序升温脱附（NH3-TPD）技术对不同分子筛催化剂的酸量及酸强度进行了表征，结果详见图4（a）及表2。分析表明，五种分子筛的NH3-TPD谱图均在低温区和高温区呈现两个脱附峰，分别对应于弱酸位和强酸位，对其分别进行积分得到对应的弱酸量与强酸量，进而计算得到两者的比值。其中，SAPO-34的总酸量最高（425 μmol/g）且以强酸为主；USY的总酸量次之（285 μmol/g）但其弱酸位占主导；ZSM-5-38的总酸量仅为181 μmol/g，且随着硅铝比的升高，该系列样品的总酸量持续下降。这是因为ZSM-5的酸性位主要源自分子筛骨架的铝氧四面体[24]，高硅铝比降低了样品的铝含量，最终造成总酸量的减少。同时，ZSM-5的弱酸量降幅更大，导致强酸量与弱酸量之比（S/W）由ZSM-5-38的0.6升至ZSM-5-200的2.0。
为进一步探究不同分子筛的酸类型，采用吡啶吸附红外光谱（Py-FTIR）对其进行了表征，见图4（b）。需要说明的是，由于吡啶分子的动力学直径大于SAPO-34的孔径，故SAPO-34的酸类型无法通过Py-FTIR测定。谱图中位于1550和1450 cm−1处的吸收峰分别归属于吡啶在Brønsted酸（B酸）与Lewis酸（L酸）位点上的吸附。结果表明，所有样品表面均同时存在B酸与L酸中心。其中，USY分子筛以B酸为主，其B酸量与L酸量之比（B/L）为2.1。对于ZSM-5系列样品，随着硅铝比升高，B酸与L酸数量均呈下降趋势且B酸量减少更为显著。ZSM-5-38与ZSM-5-85的B/L比分别为3.1和1.6；而ZSM-5-200的B/L比小于1，说明L酸在该样品中占主导地位。
2.2　分子筛催化剂十二烷催化裂解性能
2.2.1　分子筛类型对十二烷催化裂解性能的影响
以石英砂为空白对照，系统评价了SAPO-34、ZSM-5-38和USY三种分子筛催化剂的十二烷催化裂解性能，结果如表3和图5所示。根据表3可知，石英砂上十二烷的转化率仅为16.27%，说明在该反应条件下热裂解程度较低。与之相比，SAPO-34催化下的转化率增至24.33%，而ZSM-5-38与USY则展现出更高的催化活性，转化率接近100%。上述显著差异主要源于分子筛孔径尺寸的不同：SAPO-34的孔径尺寸较小（0.38 nm），严重限制了十二烷的传质与扩散，裂解活性较低；相反，ZSM-5-38与USY较大的孔径有效降低了反应物的传质阻力，使其更易进入分子筛孔道内部与酸性位接触，从而极大促进了催化裂解的进行。总气相产物收率由高到低依次为：USY > ZSM-5-38 > SAPO-34 > 石英砂，体现出原料裂解深度的差异。其中，在USY上十二烷裂解程度最深，产物主要由气相组分构成，ZSM-5-38次之，而SAPO-34与石英砂的裂解深度较低。干气与液化气的变化趋势与总气相产物一致。根据图5（a）干气收率分布可知，石英砂、SAPO-34与ZSM-5-38的干气中乙烯收率最高，与之相对地，在USY催化下甲烷和乙烷的收率均高于乙烯。图5（b）液化气收率分布显示，石英砂和SAPO-34的液化气主要为丙烯和丁烯，在ZSM-5-38和USY上丙烷和丁烷居多。这是因为ZSM-5-38与USY较大的孔径和可及性良好的酸性位能促进丙烯和丁烯发生双分子氢转移反应，使之饱和生成相应的烷烃。此外，相较于ZSM-5-38，USY凭借更大的孔径和更丰富的酸性位点，具有更强的氢转移反应活性，丙烷、丁烷的收率更高。
值得注意的是，尽管石英砂和SAPO-34的烯烃选择性较高，但受转化率限制，其低碳烯烃的收率低于ZSM-5-38和USY。最终，ZSM-5-38展现出相对最高的总低碳烯烃收率，达18.40%。
总液相产物收率按降序排列为：ZSM-5-38 > USY > 石英砂 ≈ SAPO-34，且各样品的液相产物均以汽油馏分为主。分析图5（c）BTX芳烃收率分布可得，石英砂与SAPO-34的BTX芳烃收率趋近于0，而ZSM-5-38与USY展现出显著更高的BTX芳烃收率，分别为39.44%和21.34%，且该值与其各自的汽油馏分收率相近，表明ZSM-5-38与USY催化产生的汽油馏分主要为BTX芳烃。根据文献报道，催化裂解中的BTX芳烃产物主要源于烯烃中间体在催化剂孔道内酸性位上的齐聚、环化和芳构化反应[25−26]。据此推测产生上述现象的原因是，石英砂和SAPO-34的孔道限制了BTX芳烃的生成与扩散，相反，ZSM-5-38和USY的孔道结构提供了BTX芳烃生成所必需的几何空间，使部分烯烃中间体吸附于孔道内的酸性位点得以芳构化，最终生成并释放出BTX芳烃。
不同分子筛催化剂的积炭收率存在显著差异。其中，USY催化下体系中积炭收率最高（12.90%），这表明，USY在促进BTX芳烃生成的同时，其更大的孔径和丰富的酸性位也加速了轻质芳烃的稠环化或深度脱氢缩合等反应的进行，使积炭收率大幅增加。SAPO-34的积炭收率次之，这主要归因于其较小的孔径限制了分子扩散，导致反应物易堵塞于催化剂外表面过度缩合为积炭。相比之下，ZSM-5-38的积炭收率极低，仅为0.18%，说明ZSM-5-38固有的孔道结构和适中的酸性质可有效抑制十二烷催化裂解中积炭的生成。
计算得到各分子筛催化剂的氢转移指数（Hydrogen transfer index，HTI）呈现如下递减趋势：USY > ZSM-5-38 > SAPO-34 > 石英砂。该趋势表明，USY分子筛在该过程中促进氢转移反应的能力最强，其孔道结构和酸性质更有利于氢物种的迁移与再分配；ZSM-5-38同样具有较高的氢转移活性，但低于USY；SAPO-34和石英砂发生氢转移反应的频率最低，这一结果与前述各产物收率分布特征一致，进一步验证了分析结论的准确性。
2.2.2　ZSM-5酸性质对十二烷催化裂解性能的影响
图4和表2显示，ZSM-5-38、ZSM-5-85及ZSM-5-200的酸性位数量、强度和类型差异显著。据此，本小节在明确ZSM-5为最优分子筛类型的基础上，进一步探究了其酸性质对十二烷催化裂解性能的影响，结果见表4与图6。根据表4可知，在ZSM-5-38与ZSM-5-85催化下十二烷的转化率均超过99%，且ZSM-5-200的转化率亦高达97.79%。推测产生该现象的原因是，尽管ZSM-5-200的总酸量较少（54 μmol/g），但其S/W值为2.0，表明其酸中心以强酸为主，强酸位对C−C键裂解具有更高的本征活性，因而在有限的酸性位上仍可实现高效裂解；同时，ZSM-5-200固有的孔道结构有利于十二烷的扩散与传质，可确保反应物与酸性位点的充分接触，从而支撑了较高的反应转化率。此外，气相产物收率随ZSM-5硅铝比的升高逐渐增加。这主要归因于高硅铝比ZSM-5中酸性位数量少，从而限制了气体分子发生齐聚、环化等二次反应。进一步分析发现，伴随硅铝比的升高，产物中干气收率单调递减，而液化气收率相应增加。这是因为液化气可在酸性位的作用下进一步深度裂解为干气，提高硅铝比可显著减缓该反应的进行，导致干气和液化气收率出现此消彼长的现象。
图6（a）与（b）分别展示了干气和液化气的收率分布。结果显示，当ZSM-5硅铝比升高时，氢气、甲烷、乙烷、丙烷的收率持续降低，且乙烯、丙烯、丁烯的收率不断增加，该趋势说明较低的总酸量有效抑制了氢转移反应的进行，从而减少烷烃生成并提高烯烃选择性。进而结合酸类型分析可知，B酸位点通常被认为是催化裂解、氢转移及芳构化等反应的关键活性中心，而L酸位点则更倾向于促进脱氢反应。Py-FTIR表征结果显示，随着ZSM-5硅铝比升高，催化剂的B/L比由ZSM-5-38的3.1降至ZSM-5-200的0.9，表明ZSM-5-200具备以L酸为主导的酸性特征，这是其低碳烯烃选择性提高的另一关键因素。最终，ZSM-5-200展现出最高的总低碳烯烃收率，具体地，乙烯、丙烯和丁烯的收率分别增至11.11%、20.33%和10.49%。
总液相产物收率由高到低依次排列为：ZSM-5-38 > ZSM-5-85 > ZSM-5-200。结合模拟蒸馏结果及图6（c）BTX芳烃收率分布可知，各样品的液相产物均以汽油馏分中的BTX芳烃为主。因此，液相产物收率的降低主要源于BTX芳烃的减少。分析该现象产生的原因是ZSM-5硅铝比升高导致其总酸量，尤其是B酸量的显著下降，这在一定程度上阻止了烯烃中间体发生后续的齐聚、环化和芳构化反应，从而在提高烯烃收率的同时抑制了BTX芳烃的生成。
不同硅铝比ZSM-5的积炭收率数据显示，随着硅铝比的升高，产物中积炭收率呈现逐渐增加的趋势。该现象可归因于两方面因素：一方面，硅铝比升高抑制了氢转移反应，促使烯烃收率增加，而烯烃作为积炭前驱体，更容易形成积炭；另一方面，硅铝比提高使ZSM-5中强酸位比例上升，有利于烯烃中间体在局部强酸位点上发生积炭反应，导致积炭收率增加。但值得注意的是，即使硅铝比最高的ZSM-5-200，其积炭收率也仅小幅上升至0.43%，整体上积炭生成量仍维持在较低水平，凸显出ZSM-5良好的抗积炭性能。
不同硅铝比ZSM-5的氢转移指数按降序排列为：ZSM-5-38 > ZSM-5-85 > ZSM-5-200。该结果表明，在硅铝比升高的情况下，体系中氢转移反应逐渐被抑制，符合上述各产物收率分布情况，进一步证实了氢转移反应活性与ZSM-5酸性质间的内在关联。
2.2.3　反应后分子筛催化剂的积炭表征
采用差热-热重同步分析仪对反应后分子筛催化剂的积炭进行了表征。如图7（a）所示，各催化剂的热失重（TG）曲线在高温区（> 450 ℃）表现出明显的失重现象，这主要源于积炭物种的烧除。失重量按以下顺序依次递减：USY > SAPO-34 > ZSM-5-200 > ZSM-5-85 ≈ ZSM-5-38，反映出不同催化剂在反应过程中的积炭倾向逐渐减弱。从图7（b）微分热失重（DTG）曲线可以看出，ZSM-5系列分子筛在300−900 ℃呈现持续缓慢的失重趋势，未观察到明显的失重速率峰值。与之不同的是，SAPO-34的积炭失重速率峰值出现在542 ℃，而USY的峰值温度则位于568 ℃，表明在USY上形成的积炭更难以脱除。
为进一步揭示反应后SAPO-34与USY上积炭物种的化学结构特性，对其进行了拉曼（Raman）光谱表征。图8（a）显示，反应后催化剂在约1400和1625 cm−1处出现两个特征峰，分别对应于积炭物种的D带和G带。其中，D带通常归属于无定形或缺陷碳物种，而G带则反映了有序石墨化碳的存在。通过计算D带和G带的强度比（ID/IG）可得到催化剂表面无定形碳与石墨化碳的相对含量，进而分析积炭物种的有序程度。
图8（b）结果表明，USY的ID/IG比为0.32，低于SAPO-34的ID/IG比（0.43），说明USY上积炭物种的石墨化程度更高，结构更为有序，因而具有更好的热稳定性，这与热重分析结果一致。对上述差异归因如下：SAPO-34较小的孔径严重限制了反应物的扩散，导致其更易于催化剂外表面积聚，进而在高温下缩合生成无序碳；相比之下，USY具有较大的孔径，有利于反应物分子接近孔道内的活性位点，促进其在酸性位的作用下发生稠环化或深度脱氢缩合等反应，从而逐步转化为结构更稳定的石墨化积炭物种。
2.2.4　分子筛催化剂的反应稳定性分析
为评估不同分子筛催化剂在十二烷催化裂解反应中的稳定性，本小节考察了十二烷转化率与低碳烯烃收率随反应时间的变化。如图9（a）所示，USY表现出最显著的失活行为，反应5 h后转化率由初始的99.31%降至89.69%，这主要归因于其表面剧烈的积炭反应，导致活性位点被迅速覆盖，催化活性减弱；SAPO-34的失活程度次之，5 h后转化率降至20.03%；相比之下，ZSM-5-38和ZSM-5-85随着反应的进行始终维持98%以上的高转化率，展现出优异的反应稳定性，这与两者良好的抗积炭能力密切相关。ZSM-5-200的稳定性略低于ZSM-5-38与ZSM-5-85，反应5 h后的转化率为95.05%，与其升高的积炭收率相符。此外，从图9（b）可见，低碳烯烃收率随时间的变化与转化率基本一致。在整个反应过程中，USY与SAPO-34的低碳烯烃收率降幅较大；ZSM-5-38与ZSM-5-85的稳定性良好；而ZSM-5-200的相应收率于5 h后降至40.68%。
2.3　十二烷催化裂解的反应路径及其调控机制
依据上述的研究和讨论，提出并系统阐明了十二烷催化裂解的反应路径及其调控机制（如图10所示），涵盖裂解、氢转移、齐聚、芳构化及积炭等关键步骤。分子筛类型是决定十二烷转化率和产物分布的首要因素，不同类型的分子筛展现出显著的催化性能差异。当以CHA构型的SAPO-34为催化剂时，其较小的孔径尺寸（0.38 nm）严重制约了反应物分子的扩散及孔内催化过程，导致十二烷转化率较低，同时，受限的孔道结构降低了双分子氢转移和芳构化反应活性，产物中低碳烯烃选择性较高而BTX芳烃收率趋近于0。
此外，反应物易堵塞于SAPO-34外表面过度缩合生成无序积炭；相比之下，MFI构型的ZSM-5孔径尺寸适宜（0.55 nm），可促进反应物的高效扩散与转化，十二烷转化率高，相应的产物分布以低碳烷烃、烯烃和BTX芳烃为主，积炭收率极低；对于FAU构型的USY，其较大的孔径（0.73 nm）同样有利于十二烷的催化转化，相较于ZSM-5，其凭借更大的孔径和更丰富的酸性中心呈现出更强的双分子氢转移反应活性，使低碳烷烃收率增加，该特性也加速了轻质芳烃的稠环化或深度脱氢缩合反应，导致大量石墨化积炭的生成。其次，在明确分子筛类型影响的基础上，通过酸性质的调控可进一步优化产物分布。一方面，随着ZSM-5硅铝比的升高，其酸性位数量降低，抑制了体系中深度裂解、氢转移、齐聚与芳构化反应的发生，进而表现出干气和液化气收率此消彼长、烯烃收率升高且低碳烷烃和BTX芳烃收率相应下降的趋势。另一方面，当ZSM-5硅铝比升高时，其B酸量大幅减少而L酸比例相应增加，同样可抑制氢转移与芳构化反应的进行，最终提高了低碳烯烃收率并减少了BTX芳烃的生成。
3　结　论
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采用固定床装置考察了SAPO-34、ZSM-5-38、ZSM-5-85、ZSM-5-200及USY对十二烷催化裂解性能的影响。结果表明，分子筛类型是影响十二烷转化率及产物分布的首要因素。其中，在孔径最小的SAPO-34上十二烷转化率仅为24.33%，BTX芳烃收率趋近于0，烯烃选择性高但催化剂外表面积炭严重；与之相比，ZSM-5-38和USY凭借较大孔径均实现了十二烷的近完全转化，两者酸性质的差异导致产物分布明显不同。具备适中酸量的ZSM-5-38表现出相对最高的总低碳烯烃收率（18.40%）和极低的积炭收率（0.18%）；而酸量更高的USY则过度促进了氢转移和积炭反应，产物以低碳烷烃为主且积炭收率高达12.90%。
其次，在明确分子筛类型的基础上，通过酸性质的调变可进一步优化产物分布。研究表明，低酸量的ZSM-5-200表现出最佳的十二烷催化裂解性能：在实现97.79%高转化率的同时总气相产物收率接近65%，此外，乙烯、丙烯和丁烯的收率分别增至11.11%、20.33%和10.49%且积炭收率仍维持在较低水平（0.43%）。
阐明了十二烷催化裂解的反应路径及其调控机制。该过程主要涉及裂解、氢转移、齐聚、芳构化和积炭等关键反应，分子筛类型及酸性质通过调控上述反应的相对强弱，直接影响原料转化率与产物分布。该反应路径与调控机制揭示了分子筛类型及酸性质与催化性能间的构效关系，不仅深化了对催化反应机理的理解，也为优化汽柴油催化裂解制烯烃工艺指明了方向。

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doi: 10.3724/2097-213X.2025.JFCT.0034
  • 接收时间：2025-10-23
  • 首发时间：2026-09-23
  • 出版时间：2026-06-10
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  • 收稿日期：2025-10-23
  • 修回日期：2025-11-23
  • 录用日期：2025-12-04
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