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Article(id=1325516960468972203, tenantId=1146029695717560320, journalId=1205116786560364546, issueId=1325516904667951420, articleNumber=null, orderNo=null, doi=10.16236/j.cnki.nrjxb.202504037, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1734192000000, receivedDateStr=2024-12-15, revisedDate=1740758400000, revisedDateStr=2025-03-01, acceptedDate=null, acceptedDateStr=null, onlineDate=1793957470290, onlineDateStr=2026-11-06, pubDate=1753372800000, pubDateStr=2025-07-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1793957470290, onlineIssueDateStr=2026-11-06, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1793957470290, creator=13701087609, updateTime=1793957470290, updator=13701087609, issue=Issue{id=1325516904667951420, tenantId=1146029695717560320, journalId=1205116786560364546, year='2025', volume='43', issue='4', pageStart='289', pageEnd='383', issueExtLink='null', onlineDate='null', pubDate='1753372800000', pubDateStr='2025-07-25', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1793957456986, creator='13701087609', updateTime=1793959854445, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1325526961023640114, tenantId=1146029695717560320, journalId=1205116786560364546, issueId=1325516904667951420, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1325526961023640115, tenantId=1146029695717560320, journalId=1205116786560364546, issueId=1325516904667951420, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=322, endPage=332, ext={EN=ArticleExt(id=1325516960829682348, articleId=1325516960468972203, tenantId=1146029695717560320, journalId=1205116786560364546, language=EN, title=Effect of anisole/toluene blending on soot characteristics of n-heptane diffusion flames, columnId=null, journalTitle=Transactions of CSICE, columnName=null, runingTitle=null, highlight=null, articleAbstract=

Anisole, a second-generation biomass fuel, has a similar molecular structure to toluene in diesel. Blending of biomass fuels with diesel is seen as a viable solution to the energy crisis. Using a liquid fuel combustion system and selecting n-heptane as the base fuel, the flame morphology, incipient soot size distribution, nanostructure, microcrystalline parameters, orderliness, functional groups and oxidation activity of the soot in the flame of n-heptane, n-heptane blended with volume fraction of 10% toluene, 10% anisole, and 5% toluene/5% anisole were analyzed at an evaporation temperature of 160 ℃. Results show that, for the size and nanostructure of soot particles, the average size of soot in the flame becomes larger under the anisole/toluene blending. For the nanostructure of soot, the blend of anisole and toluene changes the morphology of soot particles and accelerates the soot formation. From microcrystalline parameters, the overall soot structure is more organized after anisole/toluene blending, and the effect of anisole in n-heptane flame on the nanostructure of soot is less than that of toluene. For soot ordering, the intensity ratio of the D1 peak to the G1 peak(ID1/IG1) increases by 17.3% from T10 to A05 and by 11.5% from A05 to A10, respectively, and the degree of graphitization of soot decreases with the increase of anisole blending. The graphitization of soot in the n-heptane flame is minimized when only anisole is blended.

, authors=Wei Li1, Junlong Liu1, Yujuan Li1, Wenlong Dong2, Huaqiang Chu2, authorsList=Wei Li, Junlong Liu, Yujuan Li, Wenlong Dong, Huaqiang Chu, authorCompany=null, correspAuthors=Huaqiang Chu, 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, fund=null), CN=ArticleExt(id=1325516969637720778, articleId=1325516960468972203, tenantId=1146029695717560320, journalId=1205116786560364546, language=CN, title=苯甲醚/甲苯掺混对正庚烷扩散火焰碳烟特性的影响, columnId=null, journalTitle=内燃机学报, columnName=, runingTitle=null, highlight=null, articleAbstract=

苯甲醚作为一种第二代生物质燃料，与柴油中甲苯具有相似的分子结构．生物质燃料与柴油掺混燃烧被视为解决能源危机的可行方案．基于此，采用液体燃料燃烧系统，选取正庚烷作为基础燃料，在蒸发温度为160℃下对正庚烷、正庚烷掺混10%(体积分数)甲苯(T10)、10%苯甲醚(A10)和5%甲苯/5%苯甲醚(A05)燃料的火焰形态、碳烟粒径分布、纳观结构、微晶参数、有序度、官能团和氧化活性进行了分析．结果表明：在碳烟颗粒的尺寸及纳观结构方面，随着苯甲醚/甲苯掺混，火焰中碳烟平均粒径变大．在碳烟纳观结构方面，苯甲醚和甲苯的加入改变了火焰中碳烟颗粒形态，加速了碳烟生成．在微晶参数方面，掺混苯甲醚/甲苯后，碳烟整体结构更为有序，苯甲醚对正庚烷火焰中碳烟纳观结构的影响小于甲苯．在碳烟有序度方面，D1峰与G1峰强度比(ID1/IG1)从T10到A05的增加幅度为17.3%，从A05到A10的增加幅度为11.5%，碳烟石墨化程度随苯甲醚掺混增大而降低．在只有苯甲醚掺混的工况下，正庚烷火焰中碳烟的石墨化程度提升最小．

, authors=李卫1, 刘俊龙1, 李玉娟1, 董文龙2, 楚化强2, authorsList=李卫, 刘俊龙, 李玉娟, 董文龙, 楚化强, authorCompany=null, correspAuthors=楚化强, authorNote=

李卫，博士，高级工程师，.

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楚化强，博士，教授，.
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李卫，博士，高级工程师，.

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李卫，博士，高级工程师，.

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Carbon，2005，43(8)：1731-1742., articleTitle=Raman microspectroscopy of soot and related carbonaceous materials：Spectral analysis and structural information, refAbstract=null), Reference(id=1325516991636845367, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325516960468972203, doi=null, pmid=null, pmcid=null, year=2021, volume=225, issue=null, pageStart=120, pageEnd=135, url=null, language=null, rfNumber=［28］, rfOrder=27, authorNames=Chu H, Ya Y, Nie X, journalName=Combustion and Flame, refType=null, unstructuredReference=Chu H，Ya Y，Nie X，et al. Effects of adding cyclohexane，n-hexane，ethanol，and 2，5-dimethylfuran to fuel on soot formation in laminar coflow n-heptane/iso-octane diffusion flame[J]. Combustion and Flame，2021，225：120-135., articleTitle=Effects of adding cyclohexane，n-hexane，ethanol，and 2，5-dimethylfuran to fuel on soot formation in laminar coflow n-heptane/iso-octane diffusion flame, refAbstract=null), Reference(id=1325516991724925752, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325516960468972203, doi=null, pmid=null, pmcid=null, year=2022, volume=null, issue=null, pageStart=null, pageEnd=null, url=null, language=null, rfNumber=［29］, rfOrder=28, authorNames=牙宇晨, journalName=null, refType=null, unstructuredReference=牙宇晨. 不同含氧燃料对正庚烷/异辛烷雾化燃烧火焰中碳烟生成的影响[D]. 马鞍山：安徽工业大学能源与环境学院，2022., articleTitle=不同含氧燃料对正庚烷/异辛烷雾化燃烧火焰中碳烟生成的影响, refAbstract=null)], funds=[Fund(id=1325516987765502746, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325516960468972203, awardId=52306125, language=CN, fundingSource=国家自然科学基金资助项目(52306125), fundOrder=null, country=null), Fund(id=1325516987828417307, tenantId=1146029695717560320, 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Fuel ratios and mass flow rate settings for four fuel conditions

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燃料工况正庚烷(体积分数)/%甲苯(体积分数)/%苯甲醚(体积分数)/%燃料质量流量/(g·h-1)碳氢比
N001000010.800.43750
T109010010.700.48125
A05905510.730.48125
A109001010.880.48125
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4种燃料工况的燃料配比及质量流量设置

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燃料工况正庚烷(体积分数)/%甲苯(体积分数)/%苯甲醚(体积分数)/%燃料质量流量/(g·h-1)碳氢比
N001000010.800.43750
T109010010.700.48125
A05905510.730.48125
A109001010.880.48125
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Split-peak data of ID1、IG1 and ID1/IG1 from Raman spectra of soot in center of HAB=30mm and HAB=40mm

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工况HAB/mmID1IG1ID1/IG1
N0030939.31501157.6540.811
40447.3980460.3740.972
T10302041.59403456.1820.591
40551.1280602.8460.914
A05301896.37502734.6150.693
40490.9400528.9830.928
A1030868.93491123.8710.773
40512.8200547.1820.937
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HAB=30mm和HAB=40mm处火焰中心碳烟拉曼光谱的分峰数据ID1、IG1和ID1/IG1

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工况HAB/mmID1IG1ID1/IG1
N0030939.31501157.6540.811
40447.3980460.3740.972
T10302041.59403456.1820.591
40551.1280602.8460.914
A05301896.37502734.6150.693
40490.9400528.9830.928
A1030868.93491123.8710.773
40512.8200547.1820.937
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Oxidizing characteristic temperatures and mean temperatures of soot samples of four fuel operating conditions

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工况火焰高度/mmTi/℃Tmax/℃T0/℃Tm/℃
N0030548.34636.5659.81614.88
40548.34609.10638.14581.05
T1030561.79646.21668.14625.38
40533.97635.87659.64609.82
A0530560.73639.00662.05620.59
40520.62627.79641.00596.47
A1030552.59636.98660.96616.84
40513.44621.27640.85591.85
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4种燃料工况碳烟样品的氧化特征温度和平均温度

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工况火焰高度/mmTi/℃Tmax/℃T0/℃Tm/℃
N0030548.34636.5659.81614.88
40548.34609.10638.14581.05
T1030561.79646.21668.14625.38
40533.97635.87659.64609.82
A0530560.73639.00662.05620.59
40520.62627.79641.00596.47
A1030552.59636.98660.96616.84
40513.44621.27640.85591.85
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苯甲醚/甲苯掺混对正庚烷扩散火焰碳烟特性的影响
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李卫 1 , 刘俊龙 1 , 李玉娟 1 , 董文龙 2 , 楚化强 2
内燃机学报 | 2025,43(4): 322-332
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内燃机学报 | 2025 , 43 (4) : 322 -332
苯甲醚/甲苯掺混对正庚烷扩散火焰碳烟特性的影响
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李卫1 , 刘俊龙1, 李玉娟1, 董文龙2, 楚化强2
作者信息
  • 1.潍柴动力股份有限公司内燃机与动力系统全国重点实验室，潍坊 261061
  • 2.安徽工业大学能源与环境学院，马鞍山 243002
通讯作者:
楚化强，博士，教授，.
作者简介:

李卫，博士，高级工程师，.

Effect of anisole/toluene blending on soot characteristics of n-heptane diffusion flames
Wei Li1 , Junlong Liu1, Yujuan Li1, Wenlong Dong2, Huaqiang Chu2
Affiliations
  • 1.State Key Laboratory of Engine and Powertrain System，Weichai Power Company Limited，Weifang 261061，China
  • 2.School of Energy and Environment，Anhui University of Technology，Maanshan 243002，China
出版时间: 2025-07-25 doi: 10.16236/j.cnki.nrjxb.202504037
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摘要
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苯甲醚作为一种第二代生物质燃料，与柴油中甲苯具有相似的分子结构．生物质燃料与柴油掺混燃烧被视为解决能源危机的可行方案．基于此，采用液体燃料燃烧系统，选取正庚烷作为基础燃料，在蒸发温度为160℃下对正庚烷、正庚烷掺混10%(体积分数)甲苯(T10)、10%苯甲醚(A10)和5%甲苯/5%苯甲醚(A05)燃料的火焰形态、碳烟粒径分布、纳观结构、微晶参数、有序度、官能团和氧化活性进行了分析．结果表明：在碳烟颗粒的尺寸及纳观结构方面，随着苯甲醚/甲苯掺混，火焰中碳烟平均粒径变大．在碳烟纳观结构方面，苯甲醚和甲苯的加入改变了火焰中碳烟颗粒形态，加速了碳烟生成．在微晶参数方面，掺混苯甲醚/甲苯后，碳烟整体结构更为有序，苯甲醚对正庚烷火焰中碳烟纳观结构的影响小于甲苯．在碳烟有序度方面，D1峰与G1峰强度比(ID1/IG1)从T10到A05的增加幅度为17.3%，从A05到A10的增加幅度为11.5%，碳烟石墨化程度随苯甲醚掺混增大而降低．在只有苯甲醚掺混的工况下，正庚烷火焰中碳烟的石墨化程度提升最小．

苯甲醚  /  甲苯  /  正庚烷  /  碳烟  /  石墨化程度

Anisole, a second-generation biomass fuel, has a similar molecular structure to toluene in diesel. Blending of biomass fuels with diesel is seen as a viable solution to the energy crisis. Using a liquid fuel combustion system and selecting n-heptane as the base fuel, the flame morphology, incipient soot size distribution, nanostructure, microcrystalline parameters, orderliness, functional groups and oxidation activity of the soot in the flame of n-heptane, n-heptane blended with volume fraction of 10% toluene, 10% anisole, and 5% toluene/5% anisole were analyzed at an evaporation temperature of 160 ℃. Results show that, for the size and nanostructure of soot particles, the average size of soot in the flame becomes larger under the anisole/toluene blending. For the nanostructure of soot, the blend of anisole and toluene changes the morphology of soot particles and accelerates the soot formation. From microcrystalline parameters, the overall soot structure is more organized after anisole/toluene blending, and the effect of anisole in n-heptane flame on the nanostructure of soot is less than that of toluene. For soot ordering, the intensity ratio of the D1 peak to the G1 peak(ID1/IG1) increases by 17.3% from T10 to A05 and by 11.5% from A05 to A10, respectively, and the degree of graphitization of soot decreases with the increase of anisole blending. The graphitization of soot in the n-heptane flame is minimized when only anisole is blended.

anisole  /  toluene  /  n-heptane  /  soot  /  graphitization
李卫, 刘俊龙, 李玉娟, 董文龙, 楚化强. 苯甲醚/甲苯掺混对正庚烷扩散火焰碳烟特性的影响. 内燃机学报, 2025 , 43 (4) : 322 -332 . DOI: 10.16236/j.cnki.nrjxb.202504037
Wei Li, Junlong Liu, Yujuan Li, Wenlong Dong, Huaqiang Chu. Effect of anisole/toluene blending on soot characteristics of n-heptane diffusion flames[J]. Transactions of CSICE, 2025 , 43 (4) : 322 -332 . DOI: 10.16236/j.cnki.nrjxb.202504037
正文
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内燃机(包括柴油机、喷气发动机和燃气机)因其具有热效率高、续航时间长、成本低和使用方便等优点，仍是最主要的动力来源[1]，但其污染物排放，尤其是碳烟颗粒是世界上最重要的挑战之一[2]．目前含氧生物燃料已被用于与化石燃料混合使用，以提高发动机热效率，减少碳烟和碳排放[3]．苯甲醚是典型的第二代生物质含氧燃料，可用作燃油添加剂进行清洁燃烧应用[4]．
Donkerbroek等[5]研究发现，当柴油机的喷射持续时间少于点火延迟时间，柴油/苯甲醚混合物碳烟生成量可以忽略不计．Nowakowska等[6]研究了苯甲醚的热解和氧化动力学，发现苯甲醚的苯氧基自由基会在热解和氧化反应下形成环戊二烯基自由基．Wu等[7]研究发现，苯甲醚提高了汽油替代燃料层流火焰速度，而Wagnon等[8]通过射流搅拌反应器研究苯甲醚燃烧反应机理，结果表明：苯氧基和环戊二烯基的分解和氧化反应是苯甲醚具有相对较快的层流燃烧速度的原因．Atiku等[9]通过扩散火焰研究松木燃烧过程初级热解产物(如苯甲醚)燃烧时碳烟生成的机制，发现木材是通过环戊二烯基中间体这类热解产物参与氢提取乙炔加成(HACA)反应的机制，形成碳烟．Matteo等[10]发现，苯甲醚燃烧过程的碳烟生成主要来源于苯酚和芳香族组分的气相反应．Zare等[11]指出，苯甲醚具有较高的层流燃烧速度，且可以通过提高温度和降低压力来提高苯甲醚的层流燃烧速度．Xiong等[12]使用消光法测量了逆流层流扩散火焰中正庚烷/苯甲醚混合物形成的碳烟，最大碳烟体积分数是苯甲醚比例的指数函数，这主要归因于苯甲醚在燃烧过程中促进了热解、氧化过程中多环芳香烃(PAHs)和碳烟的形成．Londhe等[13]研究了柴油发动机中使用苯甲醚对柴油机性能和排放特性的影响，发现生物柴油掺混苯甲醚会减少柴油机运行过程中HC和CO排放．Sommerer等[14]研究发现，掺混体积分数为10%的苯甲醚对异辛烷的点火延迟影响非常小．Büttgen等[15]在快速压缩机中进行苯甲醚反应性的试验、理论和动力学建模研究，苯甲醚均未表现出负温度系数行为．Rajesh等[16]和Han等[17]发现，苯甲醚可以抑制柴油机燃烧过程中碳烟的生成，并实现低NOx和碳烟排放平衡．Zhang等[18]通过层流预混火焰发现，苯甲醚的加入会促进多环芳香烃的生成．Wei等[19]研究发现，甲苯的掺混会导致碳烟集聚体表现为更大尺寸的团簇，而Nie等[20]通过层流扩散火焰发现，随着掺混甲苯含量的增加，正庚烷火焰中碳烟石墨化程度不断加深．
甲苯作为柴油中芳香族成分的重要代表[21]，一定程度上增加了碳烟的生成，但与其结构相似、性质相似的苯甲醚可用作甲苯的替代燃料．综上可知，以正庚烷作基础燃料，以甲苯表征燃油中芳香族成分，再以苯甲醚逐步替代甲苯，探究苯甲醚、甲苯两种不同芳香族燃料对火焰中碳烟生成机理的影响规律有重要的理论和应用价值[22-23]．基于此，笔者在燃料中碳流量不变的条件下，结合火焰的形态学进行苯甲醚/甲苯掺混下正庚烷火焰中碳烟生成的特性研究，以期为生物质燃油添加剂替代品的研究提供参考．
1　试验方案与分析方法
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1.1　试验方案
图1为液体雾化燃烧试验系统示意．试验采用课题组自主设计的液体燃料层流扩散火焰系统，该系统由同轴扩散燃烧器、蒸发器、空气预热器和可控管路加热装置组成．蒸发器的蒸发温度为160℃．同轴扩散燃烧器采用改进的Gülder燃烧器，由燃料管路及同心空气管路组成，燃料管是内径为10.8mm、壁面厚度为1.0mm的不锈钢管，空气管内径为88.8mm，燃料管和空气管之间由多孔金属泡沫板和直径为5.0mm的玻璃珠填充，以保证氧化剂的平稳流出．选用直链烷烃-正庚烷来表征烷烃成分，甲苯来表征芳香烃成分，以正庚烷作为试验的基础燃料建立层流扩散火焰，4种燃料工况如表1所示，甲苯和苯甲醚按照体积比掺混入正庚烷中，碳氢比为燃料混合物中碳原子数和氢原子数的比值．
由于甲苯和苯甲醚的芳香环结构对碳烟形成有很强的促进作用，因而试验工况设计中选择较低比例的苯甲醚和甲苯进行掺混，以A10作为基础组，在0%～10%体积分数范围内使用苯甲醚对甲苯进行替换，达到试验需求的燃料设计．在燃料流量的设计上，需保证各试验组的碳通量相同，笔者将燃料的碳通量设为9.07g/h、载气流量设为0.23L/min．试验中碳通量为燃料流中碳的质量含量．
1.2　采样和分析方法
对火焰中碳烟的采样方法主要包括热泳探针采样法和毛细管稀释采样法，采样装置如图2所示．热泳探针采样法利用火焰与铜网之间巨大温差产生的热泳力进行采样，铜网快速进出火焰，铜网驻留火焰中心的时间为38ms．试验采样高度分别为距燃烧器高度(HAB)20、30和40mm处，每个采样高度重复3次采样．
试验分析装置包括电荷耦合元件(CCD)相机、透射电子显微镜(TEM)、热重分析仪(TGA)、高分辨率透射电镜(HRTEM)、拉曼光谱(Raman spectroscopy)仪和傅里叶变换红外(FI-TR)光谱仪．其中，试验中使用拉曼光谱仪(英国Renishaw公司生产的InVia型)，用氩离子激光器作激发光源，激发线波长为532nm，激光输出功率为20mW，照射在样品表面上的功率为1mW．傅里叶红外光谱仪选用美国Nicolet6700型光谱仪，试验中首先对溴化钾(KBr)和碳烟粉末样品进行24h干燥，之后将二者研磨并压成片状进行测量．
2　结果与讨论
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2.1　火焰高度
正庚烷仅掺混单一燃料为掺混组，分别为N00、T10、A10；研究苯甲醚替代甲苯在正庚烷中的比例为替换组，分别为T10、A05、A10．图3分别为掺混组与替换组的火焰图像，图中红色虚线代表层流扩散火焰暗部和火焰高度的变化．可以看出，与加入甲苯的T10工况相比，N00工况(纯正庚烷)虽然火焰的碳通量和载气流量相同，但由于甲苯组分加入燃烧，火焰亮部高度明显提高，且火焰的暗部高度明显下降，火焰的碳烟分布区域显著变大．在苯甲醚掺混组分的火焰中该趋势仍明显，正庚烷火焰中加入芳烃组分后会对碳烟的生成过程产生显著的促进效果，增强了碳烟的生成趋势．
由图3(a)可知，T10火焰在火焰形态上的变化明显大于A10火焰，说明甲苯对正庚烷火焰的影响大于苯甲醚．图3(b)中，当苯甲醚替换甲苯比例越大时，火焰的亮部高度下降，暗部高度上升，火焰中黄色火焰区域占比呈线性下降．
黄色火焰部分被认为是碳烟颗粒发热产生热辐射的发光现象[24]，因而火焰中黄色火焰的区域也代表了火焰中的碳烟分布情况．分析4种燃料工况发现，在燃料碳通量不变的条件下，苯甲醚每替换燃料中5%(体积分数)甲苯成分，火焰的亮部高度降低1mm，暗部高度升高1mm．火焰结构的变化可能是由于苯甲醚替换甲苯后，火焰的反应池中加入的芳烃量不变，但由于苯甲醚替换甲苯后反应池中的甲氧基替换了甲基，为火焰的反应池带来额外的含氧基团，影响了火焰中的碳烟生成，抑制了初生碳烟的形成，并且增强了碳烟的氧化反应，促使碳烟生成延迟．
2.2　普通透射电子显微镜分析
对每个采样点采集的碳烟颗粒样品进行TEM分析，每组图像中约分析100个碳烟单颗粒，以此保证数据的可靠性．
图4为纯正庚烷和甲苯/苯甲醚掺混火焰采用热泳探针所采集的TEM图像，以研究碳烟的团簇情况及燃料工况改变时碳烟形态的演变．由图4可知，当HAB＝20mm时，N00火焰的中心碳烟样品大多数以粒径较小的单核颗粒存在，而加入甲苯和苯甲醚组分后，采集的碳烟样品中以团聚体形式存在的碳烟明显增加，且存在浸有分离核的液态透明碳烟颗粒，该形态的碳烟颗粒相较于单一核形态的碳烟石墨化程度更高，初生碳烟生成提前．笔者发现，相较于纯正庚烷，无论是甲苯还是苯甲醚，都会加速火焰中碳烟的生成，且在苯甲醚替换甲苯组分的试验组T10、A05和A10中，火焰中心的碳烟粒径随苯甲醚替换比例的增加而变小．当HAB=30mm时，碳烟颗粒的粒径明显变大，但在苯甲醚替换甲苯组分的试验组T10、A05和A10中，碳烟的粒径和团聚体大小随苯甲醚替换甲苯比例的变大而变小．当HAB=40mm时，火焰中心采集到的碳烟样品与HAB=30mm的现象相似．
4种燃料工况下，3个采样高度火焰中心碳烟颗粒形貌的变化是由于在加入甲苯和苯甲醚组分后，火焰中的燃烧反应池相较于纯正庚烷火焰中增加的芳烃组分，促进了火焰中第一苯环的形成．在碳烟的形成过程中，第一苯环的形成是碳烟形成的关键限速步骤，因而反应池中苯环结构的体积分数增加后，加速了火焰中PAHs的生成，进一步影响了后续的碳烟形成过程．但在苯甲醚替换甲苯燃料工况(T10、A05和A10)中，在相同的火焰高度下，随着苯甲醚对燃料中甲苯组分替换比例增大，火焰中碳烟粒径减小．在贫燃条件下，羟基自由基主导了火焰中碳烟的氧化反应，而苯甲醚中苯氧基自由基在热解过程中增加了火焰中羟基自由基浓度，促进了碳烟的氧化反应，抑制了碳烟的形成，导致了碳烟颗粒的粒径和团聚形态存在差异．
此外，碳烟的形成与成熟也受到火焰温度的影响．碳烟的形成会增加火焰的辐射热，使局部温度发生显著变化，并影响碳烟的碳化过程与形貌．火焰中心线上碳烟形成的区域有3个[25]，具体为：(1)液态颗粒起始区，温度为1100～1400K，颗粒多为透明单一；(2)固态碳烟起始区域，温度为1500K左右，其形态为小的固态核浸没在液态颗粒中；(3)温度高于1500K时存在固态颗粒的成熟碳化碳烟聚集区域．温度上的差异导致在HAB=20mm时，纯正庚烷火焰中心的碳烟大多是以透明单一核态颗粒存在，而添加甲苯和苯甲醚导致不同程度的固态核浸没在液态透明颗粒形态的碳烟中[17,20]．
2.3　高分辨率透射电子显微镜分析
笔者使用自主开发的Fringe软件对碳烟颗粒的HRTEM图像进行分析[20,26]，如图5所示，得到的碳烟颗粒内部的纳观结构参数(微晶曲率、微晶长度和微晶层间距)中，微晶长度代表HRTEM图像中微晶碳层的长度，其大小体现了碳烟颗粒内部的分子结合连续性．微晶曲率代表碳烟颗粒内部微晶碳层的弯曲程度，微晶曲率越大，碳烟颗粒内部微晶碳层的弯曲程度越大．微晶层间距为平行且相邻微晶碳层之间的间距，表示碳烟颗粒内部碳层结构的疏松程度．
图6为不同阶段碳烟颗粒的形貌示意．图7示出不同高度火焰中心碳烟颗粒HRTEM图像．根据纳米结构的不同，碳烟颗粒分为年轻碳烟、部分成熟碳烟和成熟碳烟3种．年轻碳烟正处于老化的早期阶段，碳烟从聚结转变为附聚，并从液体状的初始碳烟形成颗粒结构，因而颗粒边界粗糙，内部呈疏松多孔结构．PAHs结晶层呈不规则取向，最明显的特征是没有石墨壳．部分成熟碳烟已形成球形结构，该阶段主要涉及脱氢和表面反应．颗粒开始形成石墨壳，但边界仍然很粗糙．成熟碳烟的PAHs晶体排列变为同心取向．这些颗粒形成了高度球形的光滑石墨壳．在火焰燃烧后期碳烟结构的表面由氧化反应主导，会发生破碎．
图8示出4种燃料工况下碳烟样品的微晶长度数量分数和微晶曲率数量分数分布．可以看到，在HAB=20mm处的微晶长度分布拟合曲线更高、更窄，说明在HAB=20mm处的碳烟微晶长度分布在0～1nm区间内的比例更高，平均微晶长度更短．在HAB=30mm和HAB=40mm处，碳烟微晶长度的分布拟合曲线形态相似，均呈低矮的分布形态．微晶长度的整体变化趋势呈HAB=20mm<HAB=40mm<HAB=30mm．从HAB= 20mm到HAB=30mm，碳烟在燃烧反应中碳化，碳烟粒径变大，碳烟表面迅速堆叠生长，微晶碳层变长，且微晶碳层的弯曲度变小，使碳烟颗粒的整体结构有序度变大，微晶碳层更长且更平整．从HAB=30mm到HAB=40mm，碳烟表面被氧化反应主导，碳烟粒径变小，碳烟表面的有序碳层减少，微晶长度变短，且微晶碳层的弯曲度变大，碳烟的有序程度变低．
在HAB=20mm处，正庚烷掺混甲苯/苯甲醚可使碳烟颗粒的微晶长度增加，同时微晶曲率减小．在T10、A05和A10工况下，正庚烷火焰中心的碳烟微晶长度分别从0.675nm变大至0.711、0.706和0.688nm．在微晶曲率方面，在甲苯/苯甲醚掺混后微晶曲率变小，曲线向着峰位置更小和峰宽更窄的方向发展．此高度处于碳烟生成的初步阶段，总体有序度程度上表现为T10>A05>A10>N00．在碳烟微晶参数变化上，甲苯对正庚烷火焰产生的影响要大于苯甲醚．
随着火焰高度的变化，碳烟颗粒的碳化加深，在HAB=30mm处，N00中碳烟的平均微晶长度为0.879nm，平均微晶曲率为1.199．在T10、A05和A10工况下，火焰中心碳烟的平均微晶长度分别从0.675nm变大至0.711、0.706和0.688nm．相比于HAB=20mm，HAB=30mm处碳烟的平均微晶长度变化幅度增大，在1～2nm的微晶长度分布上分层明显．在掺混甲苯和苯甲醚后，碳烟的有序结构变多，微晶长度变长，整体微晶碳层变得长而平直．
在HAB=40mm高度下，碳烟颗粒的粒径开始变小，碳烟的表面由氧化反应主导．在HAB=40mm处，N00中碳烟的微晶长度为0.774nm、微晶曲率为1.287．在T10下碳烟的微晶长度为0.826nm，相对增加了0.052nm，微晶曲率减小为1.241；在A05工况下微晶长度为0.806nm，相对增加了0.032nm，微晶曲率减小为1.263；在A10工况下火焰中心的碳烟微晶长度为0.788，相对增加了0.014nm，微晶曲率减小为1.277．在碳烟的氧化反应过程中，碳烟微晶长度变小，微晶碳层弯曲度变大，这是由于碳烟表面的有序微晶碳层在氧化反应中减少，碳烟的有序度降低．但各工况碳烟的微晶参数趋势仍与火焰中上游的碳烟趋势相同，微晶长度曲线的变化幅度变小，且在微晶曲率分布中各工况几乎重合，无明显的分布变化，与HRTEM图像的观察结果一致．
2.4　拉曼光谱分析结果
图9为不同燃料工况火焰中心碳烟在拉曼位移的一阶拉曼光谱．碳材料拉曼光谱在1800～1000cm-1区域提供了碳组织的相关信息，对碳烟的分子和多环芳族单元的化学键和振动频率敏感．
笔者采用分峰拟合碳烟颗粒样品的一阶拉曼光谱[27]，在碳烟拉曼光谱中最显著的两个特征峰处于D(defect)和G(graphite)波段，分别位于1350cm-1和1590cm-1左右．G峰由碳材料结构(芳香环或链烯烃)的sp2杂化面内的伸缩振动引起，最初归属于石墨晶体结构中具有E2g对称的理想石墨晶格振动模式，与石墨晶格面内的C—C拉伸相关．D峰也被称为无序峰，其强度与六元芳环的存在密切相关，因而D峰和G峰强度比值ID/IG常被用作估计碳材料结构的有序性和石墨化程度．
碳材料的一阶拉曼光谱存在4个D峰位置和1个G峰位置，对于这些特征峰的展开了解有助于对碳烟石墨化程度影响因素的分析[27]．这些拉曼特征峰的含义对碳烟石墨化程度的研究具有重要的指导意义．经验证，D1、D2、D3和D4峰采用Lorentz函数拟合，对G峰采用Gaussian函数拟合的组合函数拟合方式得到了较好的分峰拟合曲线．由于试验中的G峰和D2峰较难区分，且G峰强与D2峰强差异较大，为保证拟合峰数据更接近实际的D峰和G峰，拟合模型中将G＋D2峰和为G1峰，以布雷特-维格纳-法诺(Breit-Wigner-Fano)函数对其进行拟合，以有效表示G峰的不对称展宽．
图10为不同工况下HAB=30mm的碳烟样品一阶拉曼光谱及分峰拟合．通过研究不同燃料工况的D1和G1分峰拟合曲线，可以发现在HAB=30mm的碳烟拉曼曲线中，纯正庚烷火焰的D1峰和G1峰的相对强度差最小．在加入体积分数为10%甲苯后D1峰和G1峰产生了较大的强度差，且在A05和A10工况中，随着燃料中被替换的甲苯比例升高，苯甲醚的比例增加后，光谱中D1峰和G1峰的高度差逐渐缩小．
图11为不同工况下HAB=40mm的碳烟颗粒样品一阶拉曼光谱及分峰拟合．在HAB=40mm时，不论是纯正庚烷火焰还是甲苯和苯甲醚掺混工况的火焰，其D1峰和G1峰的强度差异不大，但D1峰的半高宽明显大于G1峰，峰面积也明显更大，且在各工况下D1峰和G1峰的强度差异并不明显．一阶拉曼光谱的分峰拟合详细数据如表2所示，其中包括ID1、IG1和ID1/IG1的数值．ID1/IG1越大则碳烟颗粒的石墨化程度越低，结构的有序性越差．
在HAB=30mm处的火焰中心，N00、T10、A05和A10碳烟一阶拉曼光谱拟合的ID1/IG1分别为0.811、0.591、0.693和0.773．这说明在正庚烷中掺混体积分数为10%甲苯后，在HAB=30mm处碳烟的多芳环层面积、芳烃含量以及碳烟的有序程度相对于无序结构快速增加．在加入体积分数为10%苯甲醚后，火焰中碳烟的ID1/IG1同样下降，A10的ID1/IG1为0.773，相较于N00的ID1/IG1降低了4.7%，火焰中心的碳烟石墨化程度增加，但ID1/IG1的变化幅度较小．相较于T10，A10火焰中碳烟石墨化程度的变化明显更弱．虽然苯甲醚和甲苯的基本结构相似，对碳烟形成影响程度却存在很大差异．参考Chu等[28]的工作，造成这一差异的原因可能是由于苯甲醚的甲氧基苯环结构直接参与到PAHs的生成路径中．在燃料燃烧过程中，苯甲醚需要先通过分解、重组生成C5H5．随后从C5H5到PAHs，从而促进碳烟的生成．相比于甲苯，作为HACA机理碳烟生成路径上的反应中间物加入到燃烧反应中直接影响PAHs的形成，苯甲醚对碳烟生成的促进作用明显更弱．
在HAB=40mm处，N00、T10、A05和A10碳烟拉曼光谱拟合的ID1/IG1分别为0.972、0.914、0.928和0.937，其大小顺序仍为N00>A10>A05>T10．在HAB=40mm处碳烟拉曼光谱的ID1/IG1相较于HAB=30mm处普遍增大，整体的石墨化程度降低，可能是由于火焰下游碳烟的表面生长停止，且表面正处于氧化反应阶段，石墨层的堆叠降低．在此高度相较于N00工况，T10工况下ID1/IG1降低了6.0%，A10工况下ID1/IG1降低了3.5%．T10工况下碳烟石墨化程度提高仍强于A10，但甲苯和苯甲醚对碳烟石墨化程度的影响差异较小．在A05和A10的苯甲醚替换甲苯工况中，相比于A10工况，在ID1/IG1上分别上升了1.5%和1.0%，碳烟的石墨化程度随苯甲醚替换甲苯的比例增高而下降，但变化趋势并不明显．
2.5　热重分析
热重(TG)曲线表征了碳烟样品当前重量和初始重量比值随温度或时间的变化，微商热重(DTG)曲线是对TG曲线的一阶微分曲线．图12为各工况下纯正庚烷和甲苯/苯甲醚掺混条件下碳烟样品的TG和DTG曲线．在HAB=30mm处，各工况碳烟的TG图像在失重过程中更为平缓一些．火焰中心的碳烟都处于碳化程度较高的阶段，该高度的火焰中心碳烟结构上较为有序，石墨化程度更高，因而氧化活性较低，在甲苯/苯甲醚掺混条件下曲线的区分度较低，A05、A10和N00曲线贴合较为接近．在HAB= 40mm处，各工况火焰中心碳烟粒径减小，有序程度降低，处于碳烟的氧化反应阶段．由图12(c)可知，在甲苯或苯甲醚掺混后，TG曲线变陡，且失重温度提前，各工况曲线分层明显．由图12(d)可知，在体积分数为10%甲苯掺混后曲线峰位置向右偏移明显，在后续的A05和A10工况中苯甲醚每替换5%甲苯，相比于T10曲线向左偏移，到A10曲线峰位值接近N00曲线，但峰位值温度仍大于N00工况．
笔者根据TG和DTG曲线的特点，对碳烟颗粒的特征氧化温度进行统计分析．碳烟的特征氧化温度包括：(1)起始氧化温度Ti，每组样品从氧化开始到氧化过程消耗掉样品总质量10%时的温度；(2)达到最大氧化速度时的温度Tmax，对应DTG曲线峰值温度，是碳烟颗粒质量减少最快的温度，同时对应TG曲线中斜率最大的温度；(3)燃尽温度T0，每组样品从开始氧化到氧化过程消耗掉样品总质量10%的温度[28]，对应TG曲线中曲线上纵坐标为10%的温度．当这3个氧化特性温度越低时，说明碳烟颗粒越容易被氧化，其表观活化能越低．
表3为N00、T10、A05和A10工况下碳烟在热重分析中的3个氧化特征温度以及平均温度Tm．在平均氧化温度中，相较于纯正庚烷火焰，在T10和A10工况下，火焰中任意区域的碳烟氧化特征温度都会增加，说明甲苯/苯甲醚都会使正庚烷火焰中碳烟的表征活化能增加．相较于A10工况，T10工况对碳烟的氧化特征温度影响更大．在T10、A05和A10的苯甲醚替换甲苯试验组中，随苯甲醚对甲苯替换比例的增加，在HAB=30mm处，氧化特征温度分别从625.38℃减小到620.59℃，再减小到616.84℃，随苯甲醚替换甲苯的比例增加，氧化特征温度呈线性减小．热重分析证实了在柴油替代燃料中，以苯甲醚成分对甲苯成分进行替换，来取代燃料中的芳烃成分，可以有效降低生成碳烟的氧化特性温度，提高碳烟的氧化活性．苯甲醚的加入会加速火焰底部初级粒子的成核和生长过程，同时加强火焰顶端的氧化过程．随火焰高度增加，火焰中初级粒径尺寸的差距减小，但混合燃油火焰组成团聚体的初级粒子数增加，导致碳烟团聚体总体尺寸增加．同时，苯甲醚的加入还会使火焰中碳烟的分形维数降低．结合图4和图7可知，苯甲醚的加入会加速初级粒子的成核和生长过程，可在较低的火焰高度下观测到较大的初级颗粒及碳烟团聚体．此外，苯甲醚的加入还会促进火焰的氧化作用，使正庚烷/苯甲醚混合燃油火焰尖端初级粒径与纯正庚烷火焰尖端初级粒径相差不大[18]．
2.6　傅里叶变换红外光谱分析
图13为4种燃料工况在HAB=30mm和HAB=40mm处碳烟的原始红外吸收光谱．由于图谱无法直观地对处于不同波段的特征峰进行定性和定量分析，因而需进行后续的拟合处理．
图14示出对图13进行处理后各燃料工况火焰在HAB=30mm和HAB=40mm处碳烟的红外光谱，图中标注了对应官能团的特征峰．可知，各工况不同高度的碳烟颗粒其芳香族C—H官能团特征峰(3100～3010cm-1)都不太明显．此外，在860、780和725cm-1处的小峰表明碳烟中存在催化缩合的芳香族化合物．470cm-1附近的特征峰是长碳链存在的依据[29]．
由图14可知，3440cm-1附近存在强度较高的特征峰，该特征峰与OH基团相关[29]，推测此处的强度可能是由颗粒与空气中的水分相结合导致检测时产生的较大强度特征峰．在1060cm-1附近的特征峰是由—OH官能团引起的[29]，代表了碳烟中存在的几个醛、羧酸和酯等含氧官能团．此特征峰的相对强度随燃料中苯甲醚含量的增加而增加，可能是由于苯甲醚中甲氧基的加入，导致碳烟中含氧官能团物质的增加[18]．在1620cm-1附近的特征峰代表了碳烟中C=C的含量[29]，在正庚烷掺混甲苯/苯甲醚后，该特征峰位置向波数更低的方向发生偏移，说明碳烟中的碳碳双键从烯烃碳碳双键官能团偏向芳烃碳碳双键骨架，证明碳烟中的芳香特性增强．
3　结论
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(1) 在火焰形态与温度方面，不论是甲苯还是苯甲醚，在掺混条件下都会使火焰的亮部高度增加、暗部高度降低，火焰发光区域变大；甲苯和苯甲醚掺混正庚烷都提前了正庚烷火焰中初生碳烟的生成．
(2) 甲苯和苯甲醚掺混工况相较于纯正庚烷工况，碳烟的微晶长度变大，微晶曲率减小，甲苯和苯甲醚的添加对碳烟表面生长有促进作用，生成了更多的有序微晶碳层，整体的微晶碳层表现的长度更长且平直，有序度增加．
(3) D1峰与G1峰强度比ID1/IG1从T10到A05的增加幅度为17.3%，从A05到A10的增加幅度为11.5%，相较于甲苯，苯甲醚对火焰中碳烟有序程度的提升明显小于甲苯；以苯甲醚替换甲苯可以提高碳烟的氧化活性，降低碳烟的氧化消除难度．
基金
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  • 国家自然科学基金资助项目(52306125)
  • 内燃机与动力系统全国重点实验室开放课题资助项目(skleps-sq-2023-224)
文献
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2025年第43卷第4期
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doi: 10.16236/j.cnki.nrjxb.202504037
  • 接收时间：2024-12-15
  • 首发时间：2026-11-06
  • 出版时间：2025-07-25
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  • 收稿日期：2024-12-15
  • 修回日期：2025-03-01
基金
国家自然科学基金资助项目(52306125)
内燃机与动力系统全国重点实验室开放课题资助项目(skleps-sq-2023-224)
作者信息
    1.潍柴动力股份有限公司内燃机与动力系统全国重点实验室，潍坊 261061
    2.安徽工业大学能源与环境学院，马鞍山 243002

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楚化强，博士，教授，.
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2种不同金属材料的力学参数
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Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
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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