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Article(id=1325528749416145193, tenantId=1146029695717560320, journalId=1205116786560364546, issueId=1325528735126151362, articleNumber=null, orderNo=null, doi=10.16236/j.cnki.nrjxb.202501009, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1707408000000, receivedDateStr=2024-02-09, revisedDate=1718726400000, revisedDateStr=2024-06-19, acceptedDate=null, acceptedDateStr=null, onlineDate=1793960280981, onlineDateStr=2026-11-06, pubDate=1737734400000, pubDateStr=2025-01-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1793960280981, onlineIssueDateStr=2026-11-06, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1793960280981, creator=13701087609, updateTime=1793960280981, updator=13701087609, issue=Issue{id=1325528735126151362, tenantId=1146029695717560320, journalId=1205116786560364546, year='2025', volume='43', issue='1', pageStart='1', pageEnd='95', issueExtLink='null', onlineDate='null', pubDate='1737734400000', pubDateStr='2025-01-25', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1793960277585, creator='13701087609', updateTime=1793960521174, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1325529757923951150, tenantId=1146029695717560320, journalId=1205116786560364546, issueId=1325528735126151362, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1325529757923951151, tenantId=1146029695717560320, journalId=1205116786560364546, issueId=1325528735126151362, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=72, endPage=78, ext={EN=ArticleExt(id=1325528749697163562, articleId=1325528749416145193, tenantId=1146029695717560320, journalId=1205116786560364546, language=EN, title=Investigation of catalytic effect in DOC＋SCR system under marine exhaust conditions, columnId=null, journalTitle=Transactions of CSICE, columnName=null, runingTitle=null, highlight=null, articleAbstract=

To investigate the feasibility of utilizing diesel oxidation catalytic converter(DOC) technology in marine medium speed diesel engines, an experimental study was conducted to examine the effects of DOC on selective catalytic reduction(SCR) performance and physicochemical properties of particulate matter(PM) under typical low temperature and high flow conditions in marine diesel engines. The experimental results demonstrate that the utilization of DOC can enhance the catalytic efficiency of the SCR system in typical low temperature and high flow conditions, resulting in a 65% increase in catalytic efficiency under high load(18000h-1) exhaust condition of the diesel engine. The addition of DOC can decrease the degree of graphitization in PM, and this effect is more pronounced at higher exhaust temperatures. The application of DOC can also enhance the concentration of oxygen-containing functional groups on the surface of PM, particularly leading to a 100% increase in the concentration of C—OH functional group. Consequently, this significantly enhances the oxidation activity of PM. In hydrogen-containing functional groups, the concentration of aliphatic C—H functional group, which serves as the growth nucleus of PM, is significantly reduced by 50%, thereby impeding the continued growth and aggregation of PM.

, authors=Yu Sun1, Yejian Qian1, Zhen Gong1, Ze Sun2, authorsList=Yu Sun, Yejian Qian, Zhen Gong, Ze Sun, authorCompany=null, correspAuthors=Yejian 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, fund=null), CN=ArticleExt(id=1325528752561873213, articleId=1325528749416145193, tenantId=1146029695717560320, journalId=1205116786560364546, language=CN, title=基于船舶排气工况下DOC＋SCR后处理系统催化作用, columnId=null, journalTitle=内燃机学报, columnName=, runingTitle=null, highlight=null, articleAbstract=

为研究船舶中速柴油机应用柴油氧化催化器(DOC)技术的可行性，试验了船舶柴油机典型低温大流量工况下DOC对选择性催化还原器(SCR)催化性能及共同作用下颗粒物(PM)理化性质的影响．结果表明：在典型的低温大流量工况下DOC的应用会提升SCR系统的催化效率，在柴油机高负荷排气工况(空速为18000h-1)下催化效率提升了65%；DOC和SCR共同作用会降低PM的石墨化程度，且排气温度越高，石墨化程度越低；共同作用会增加PM表面含氧官能团的浓度，其中C—OH官能团含量增加了100%，PM的氧化活性大幅提升；在碳氢官能团中，作为PM生长核心的脂肪族C—H官能团浓度大幅降低，降低幅度达到了50%，减少了PM的继续生长和聚集的机率．

, authors=孙豫1, 钱叶剑1, 龚震1, 孙泽2, authorsList=孙豫, 钱叶剑, 龚震, 孙泽, authorCompany=null, correspAuthors=钱叶剑, authorNote=

孙豫，博士研究生，.

, correspAuthorsNote=
钱叶剑，博士，教授，.
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孙豫，博士研究生，.

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孙豫，博士研究生，.

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caption=Comparison of hydrogen-containing functional groups in FTIR characterization results, figureFileSmall=xdVl5TI8ujH6E8u3H2Ht3w==, figureFileBig=amqy8qGBmzV+1Qsl1lpFCA==, tableContent=null), ArticleFig(id=1325528757699895667, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325528749416145193, language=CN, label=图9, caption=FTIR表征结果中碳氢官能团含量对比, figureFileSmall=xdVl5TI8ujH6E8u3H2Ht3w==, figureFileBig=amqy8qGBmzV+1Qsl1lpFCA==, tableContent=null), ArticleFig(id=1325528757767004532, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325528749416145193, language=EN, label=Tab.1, caption=

Engine specifications

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参数数值
型式直列
缸径/mm230
压缩比14.3
循环4
气缸数6
活塞行程/mm320
标定功率/kW1300
标定转速/(r·min-1)900
), ArticleFig(id=1325528757867667829, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325528749416145193, language=CN, label=表1, caption=

发动机相关参数

, figureFileSmall=null, figureFileBig=null, tableContent=
参数数值
型式直列
缸径/mm230
压缩比14.3
循环4
气缸数6
活塞行程/mm320
标定功率/kW1300
标定转速/(r·min-1)900
), ArticleFig(id=1325528757947359606, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325528749416145193, language=EN, label=Tab.2, caption=

Exhaust components of marine diesel engine

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负荷/%体积分数
NOx/10-6CO/10-6THC/10-6CO2/%
103301151743.4
25430761604.5
50505751755.4
75535881456.1
100550851387.1
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船舶柴油机尾气组分参数

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负荷/%体积分数
NOx/10-6CO/10-6THC/10-6CO2/%
103301151743.4
25430761604.5
50505751755.4
75535881456.1
100550851387.1
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Parameters of catalyst

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参数SCRDOC
体积/L5.792.00
孔密度/(个·cm-2)0.620.62
载体堇青石堇青石
负载量/(g·L-1)20025
金属物质的量配比Cu3(Pt∶Pd)
), ArticleFig(id=1325528758173852025, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325528749416145193, language=CN, label=表3, caption=

催化剂参数

, figureFileSmall=null, figureFileBig=null, tableContent=
参数SCRDOC
体积/L5.792.00
孔密度/(个·cm-2)0.620.62
载体堇青石堇青石
负载量/(g·L-1)20025
金属物质的量配比Cu3(Pt∶Pd)
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Conditions of catalytic performance test

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排气温度/℃空速/h-1后处理
1505000，7000，11000，
15000，18000		SCR，
DOC＋SCR
180
220
250
300
350
450
), ArticleFig(id=1325528758370984315, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325528749416145193, language=CN, label=表4, caption=

催化性能试验工况参数

, figureFileSmall=null, figureFileBig=null, tableContent=
排气温度/℃空速/h-1后处理
1505000，7000，11000，
15000，18000		SCR，
DOC＋SCR
180
220
250
300
350
450
), ArticleFig(id=1325528758429704572, tenantId=1146029695717560320, journalId=1205116786560364546, articleId=1325528749416145193, language=EN, label=Tab.5, caption=

Measurement accuracy of exhaust component

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组分体积分数量程精度/%
CO/10-65～5000±1.0(FS)
CO2/%0.1～6.0±1.0(FS)
THC/10-610～20000±1.0(FS)
NOx/10-610～10000±1.0(FS)
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测量精度

, figureFileSmall=null, figureFileBig=null, tableContent=
组分体积分数量程精度/%
CO/10-65～5000±1.0(FS)
CO2/%0.1～6.0±1.0(FS)
THC/10-610～20000±1.0(FS)
NOx/10-610～10000±1.0(FS)
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基于船舶排气工况下DOC＋SCR后处理系统催化作用
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孙豫 1 , 钱叶剑 1 , 龚震 1 , 孙泽 2
内燃机学报 | 2025,43(1): 72-78
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内燃机学报 | 2025 , 43 (1) : 72 -78
基于船舶排气工况下DOC＋SCR后处理系统催化作用
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孙豫1 , 钱叶剑1 , 龚震1, 孙泽2
作者信息
  • 1.合肥工业大学汽车与交通工程学院，合肥 230009
  • 2.安徽江淮汽车集团股份有限公司，合肥 230022
通讯作者:
钱叶剑，博士，教授，.
作者简介:

孙豫，博士研究生，.

Investigation of catalytic effect in DOC＋SCR system under marine exhaust conditions
Yu Sun1 , Yejian Qian1 , Zhen Gong1, Ze Sun2
Affiliations
  • 1.School of Automotive and Transportation Engineering，Hefei University of Technology，Hefei 230009，China
  • 2.Anhui Jianghuai Automobile Group Company Limited，Hefei 230022，China
出版时间: 2025-01-25 doi: 10.16236/j.cnki.nrjxb.202501009
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为研究船舶中速柴油机应用柴油氧化催化器(DOC)技术的可行性，试验了船舶柴油机典型低温大流量工况下DOC对选择性催化还原器(SCR)催化性能及共同作用下颗粒物(PM)理化性质的影响．结果表明：在典型的低温大流量工况下DOC的应用会提升SCR系统的催化效率，在柴油机高负荷排气工况(空速为18000h-1)下催化效率提升了65%；DOC和SCR共同作用会降低PM的石墨化程度，且排气温度越高，石墨化程度越低；共同作用会增加PM表面含氧官能团的浓度，其中C—OH官能团含量增加了100%，PM的氧化活性大幅提升；在碳氢官能团中，作为PM生长核心的脂肪族C—H官能团浓度大幅降低，降低幅度达到了50%，减少了PM的继续生长和聚集的机率．

船舶柴油机  /  碳烟颗粒  /  石墨化程度  /  表面官能团  /  后处理系统

To investigate the feasibility of utilizing diesel oxidation catalytic converter(DOC) technology in marine medium speed diesel engines, an experimental study was conducted to examine the effects of DOC on selective catalytic reduction(SCR) performance and physicochemical properties of particulate matter(PM) under typical low temperature and high flow conditions in marine diesel engines. The experimental results demonstrate that the utilization of DOC can enhance the catalytic efficiency of the SCR system in typical low temperature and high flow conditions, resulting in a 65% increase in catalytic efficiency under high load(18000h-1) exhaust condition of the diesel engine. The addition of DOC can decrease the degree of graphitization in PM, and this effect is more pronounced at higher exhaust temperatures. The application of DOC can also enhance the concentration of oxygen-containing functional groups on the surface of PM, particularly leading to a 100% increase in the concentration of C—OH functional group. Consequently, this significantly enhances the oxidation activity of PM. In hydrogen-containing functional groups, the concentration of aliphatic C—H functional group, which serves as the growth nucleus of PM, is significantly reduced by 50%, thereby impeding the continued growth and aggregation of PM.

marine diesel engines  /  particulate matter  /  graphitization  /  surface functional groups  /  aftertreatment
孙豫, 钱叶剑, 龚震, 孙泽. 基于船舶排气工况下DOC＋SCR后处理系统催化作用. 内燃机学报, 2025 , 43 (1) : 72 -78 . DOI: 10.16236/j.cnki.nrjxb.202501009
Yu Sun, Yejian Qian, Zhen Gong, Ze Sun. Investigation of catalytic effect in DOC＋SCR system under marine exhaust conditions[J]. Transactions of CSICE, 2025 , 43 (1) : 72 -78 . DOI: 10.16236/j.cnki.nrjxb.202501009
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当前船舶柴油机的排放法规已提升至Tier Ⅲ阶段，减少有害排放和提高燃油经济性成为船舶柴油机面临的主要问题．碳烟颗粒物(PM)是柴油机尾气中最主要的污染物[1]．对于缸径更大、转速更低的船用柴油机，单独的机内净化方法[2-3]很难满足严苛的排放法规，需要结合相应的后处理控制措施．
船舶柴油机控制PM排放的后处理措施主要是湿式洗涤法[4]，但该方法会产生大量的污水，对氮氧化物(NOx)的催化转化也没有促进作用，限制了其进一步发展．船舶柴油机排气流量大、排气温度相对较低(<280℃)，若采用颗粒捕集器(DPF)控制PM排放会导致排气背压升高，影响柴油机工作性能[5-6]．作为氧化型催化器，柴油机氧化催化器(DOC)的催化活性窗口温度宽，能促进PM的氧化反应，适用于低温大排量的排气工况[7]．Liang等[8]在一台排量为199L的船舶柴油机上研究了DOC对碳烟颗粒的影响，发现PM的氧化活性随着DOC轴向流动而线性增加，DOC的高效氧化反应能有效控制PM排放．García等[9]也指出DOC能有效降低瞬态工况下柴油机的PM和一氧化碳(CO)排放．因此，DOC装置具备降低船舶柴油机PM排放的潜力[8,10]．
研究发现，在后处理系统中DOC还具有一定的耦合促进作用．Boutikos等[11]发现DOC提升了NOx和PM氧化活性，增强了下游的催化反应．Hu等[12]提出“热延迟效应”概念来表征DOC对系统催化效率的提升．Leskovjan等[13]研究了重型柴油机不同的DOC和选择性催化还原(SCR)组合，发现DOC能促进不同SCR系统的催化性能．此外，DOC还能影响PM表面官能团．由于表面官能团首先参与PM的氧化反应，其浓度会显著影响PM氧化活性．Liati等[14]发现PM流经DOC后其微观层面衍生出易氧化的特征结构，但DOC对PM表面官能团的影响机制还不明确．
综上所述，DOC不仅能降低PM排放，还能提升SCR催化效率和PM的氧化活性．不过，上述研究结论多来源于车用柴油机的研究，典型船舶柴油机工况下DOC对SCR催化性能及颗粒物理化特性的影响机理尚未厘清．笔者开展了船舶中速柴油机排气工况下不同后处理组合方式(SCR和DOC＋SCR)的台架试验，利用拉曼光谱仪(RS)、X射线光电子能谱仪(XPS)和傅里叶红外光谱仪(FTIR)分析表征DOC对PM的石墨化程度、氧化活性和表面官能团浓度等变化规律，相关研究可为船舶中速柴油机排放控制提供有意义的参考．
1　试验系统与分析方法
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1.1　台架试验系统
船舶柴油机的排量大、工作转速与工况稳定，排气具有温度低、流量大的特点．鉴于大型船舶柴油机试验的经济成本与时间成本高昂[2,15]，笔者等开发了一套柴油机后处理评价系统，如图1所示．该系统以一台3.0L排量、直列4缸高压共轨柴油机作为尾气来源，相关参数见表1．通过温度和流量控制模块，解耦尾气状态参数(温度、流量和压力)与发动机负荷之间的联系，模拟船舶柴油机低温、大流量排气工况．
选取型号为DE-23的6缸船舶中速柴油机为研究对象，依据船用D2试验循环的排气测试数据如表2所示，将试验尾气调整为：碳氢化合物(THC)体积分数为160×10-6，氮氧化物(NOx)体积分数为500×10-6，CO2体积分数为5%，CO体积分数为100×10-6，O2体积分数为15%．
后处理系统中DOC的贵金属Pt与Pd物质的量比为3，采用了均匀涂覆技术；SCR为Cu-SSZ-13分子筛型催化剂，具体参数见表3．试验时，采用等效空速的方式控制流经后处理催化装置的废气流量，使用HORIBA公司的CVS-ONE-MV-HE定容采样系统采集PM；采集PM时稀释尾气的温度不超过52℃，通过聚四氟乙烯滤纸进行采集，抑制PM的团聚和氧化，确保试验的准确性．
参考船舶柴油机的排气工况和催化剂特性，试验工况如表4所示．其中，测量工况为SCR/DOC＋SCR-排气温度-空速，采集工况为SCR/DOC＋SCR-PM-排气温度．为了使试验结果能准确反映出船舶柴油机尾气处理特点，试验工况拓宽了排气温度和空速范围．其中用于石墨化分析碳烟样品工况选取了150、180、250和300℃；用于表面官能团分析的样品工况选择了250℃和11000h-1；排气温度采集点位于发动机排气管出口，该位置也是后处理装置入口处；PM采集位置位于后处理装置出口处．
在试验台架的测量系统中使用了HORIBA公司的MEXA-ONE-RS系统测量尾气排放，利用AVL公司的SESAM160FT傅里叶变化红外光谱仪实时监测氨逃逸量；相关测量精度如表5所示．其中，CO和CO2采用了非分散红外(NDIR)技术，THC采用了火焰离子化检测(FID)技术，NOx采用了热化学发光检测(Heated-CLD)技术．
1.2　表征分析方法
为了提高后处理系统催化效率，明确后处理系统催化剂的优化方向，拟研究DOC对PM理化性质的影响．PM的氧化活性影响了后处理系统的能力需求，氧化特性受表面官能团类型和石墨化程度的影响．
拉曼光谱分析法可以检测石墨烯晶格的尺寸和缺陷，是表征PM石墨化程度的重要方式．表征试验使用HORIBA公司的LabRam HR Evolution型拉曼光谱仪，激光波长为532nm，功率设定为5～6mW，光斑直径为1.2μm，目镜放大10倍，物镜放大50倍．为保证样品均匀度及拉曼分析的可重复性，碳烟样品选取3处区域进行扫描，扫描时间为20s．样品均匀度如图2所示，3次测量结果的峰值相位与峰值强度误差较小，表明制备样品均匀度满足试验要求．其中，1360cm-1处的D1峰为无序特征峰，1600cm-1处的G峰为有序化碳层特征峰．结果图谱可采用四峰拟合的方法进行分析，并根据D1峰与G峰面积比和D1峰的半峰宽来衡量PM的石墨化程度．
PM表面含有丰富的芳香族C—H、C＝C和C—O等官能团．在PM氧化过程中，官能团可为氧化反应提供更多的反应位点；官能团的种类和特性也影响了PM的氧化特性．PM表面主要官能团分为含氧和碳氢官能团，利用对C—H健更为敏感的傅里叶红外光谱(FTIR)仪来表征碳氢官能团，使用X射线光电子能谱仪(XPS)表征含氧官能团．FTIR分析采用了美国Thermo Nicolet公司的Nicolet型傅里叶变换红外光谱仪，分辨率设置为4cm-1，扫描范围为400～4-1．为了保证试验结果的可重复性，对样品的均匀度和采样方法均进行了3次独立对比．XPS表征采用美国Thermo Nicolet公司的ESCALAB250Xi型X射线光电子能谱仪，全谱扫描步长设置为1eV，通能为80eV；精细谱扫描步长设置为0.1eV，通能为40eV．
2　试验结果分析
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2.1　船舶排气工况下DOC装置对催化效率的影响
针对船用柴油机排气的低温大流量特点，基于等效空速的方式开展了台架试验，测量了不同后处理系统布置方式(SCR/DOC＋SCR)下催化性能的变化规律．图3(a)显示了不同空速下SCR系统的NOx催化效率随发动机排气出口温度的变化规律．在不同空速工况下，随着排气温度的增大，NOx的催化效率增加．当排气温度高于250℃时，催化效率保持在90%左右；排气温度处于150～250℃时，催化效率与排气温度的变化呈线性关系，催化效率从20%提升至了90%．此外，随着排气空速由5000h-1提升至18000h-1，催化效率总体上呈下降趋势．其中，在排气温度为220℃时，空速为7000h-1下催化效率要比18000h-1下催化效率高了30%．造成此现象的原因是空速增大意味着单位时间内通过催化剂的气体量增加，若催化剂上反应位点浓度不变，参与反应的NOx量不变，催化效率降低．若排气温度增加，NOx催化还原反应速率加快，单位时间内参与反应的NOx量增加，导致不同空速下催化效率的差异变小．
保持相同的试验工况，图3(b)显示了不同空速下DOC＋SCR对NOx催化效率随发动机排气出口温度的变化规律．随着排气温度的增加，不同空速下NOx催化效率都呈现出上升趋势．当排气温度超过250℃后，催化效率稳定在90%～100%．在DOC＋SCR布置方式下，随着空速的增加，催化效率也在提升，这与图3(a)中催化效率随空速的变化规律是相反的．原因可能是后处理系统中DOC会影响NOx组分中物质的量n(NO)/n(NO2)的值，进而影响SCR对NOx催化还原反应过程．当快速SCR反应占比增加后，提高了NOx还原反应速率，空速的增加可能加快了反应产物脱离催化反应位点，使得反应平衡正向移动，因而NOx催化效率随空速的提升而增加．随着排气温度的增加，不同空速工况下催化效率的差异也保持了减小的趋势，说明排气温度的升高对NOx催化还原反应的促进作用弥补了空速变化带来的差异性．试验结果表明，在船舶排气工况下DOC的应用对NOx的催化还原有促进作用．
船舶柴油机的排气温度相对较低，CO和HC也是主要排放污染物．图4展示了在较低发动机排气出口温度(150℃和180℃)工况下后处理系统有/无DOC条件下CO催化效率随空速的变化规律．若后处理系统没有DOC，CO催化效率维持在15%～20%，当排气温度提升至180℃后，CO催化效率增加至88%～92%．当采用DOC＋SCR后处理系统、排温为150℃和180℃下，CO的催化效率基本保持在100%．这说明在船舶排气工况下，DOC能改善低温排气净化性能．此外，随着排气空速的提升，CO催化效率的变化幅度在3%以内，说明空速变化对CO的催化效率影响较小．
2.2　催化装置对PM石墨化程度的影响
PM是由碳烟微晶片层堆积形成的复杂颗粒，根据堆叠方式可以分为无定型碳和有序石墨晶体．PM的石墨化程度一定程度上表征了PM的氧化能力．由于燃烧温度对碳烟石墨化程度的影响较大，试验时按照排气温度分类采集碳烟．为了便于比较分析，拉曼光谱图分析时利用分峰面积与总拟合面积的对比结果进行了归一化处理．
图5展示了后处理系统(SCR和DOC＋SCR)试验条件下PM的拉曼光谱分析测试结果．由图5(b)可知，位于1360cm-1处的D1峰是由晶体的对称性转变而产生，通常称为无序峰；G峰则是由声子振动模产生，并且该峰对碳原子的网格形式很敏感，通常可用来表征微粒中有序化碳层结构．D1峰和G峰的面积比值(AD1/AG)表示了无序化参数比上有序化参数，可以表征材料的石墨化程度．由图5(a)可以看出，DOC＋SCR工况中AD1/AG的值始终高于SCR工况，表明DOC＋SCR工况下碳烟石墨化程度要低于SCR工况．这说明在相同工况下DOC的应用会降低PM的石墨化程度，原因可能是PM在DOC中发生了氧化反应．柴油机尾气中的氧气含量一般在13%～15%，对于PM的氧化反应可能是富氧环境，所以氧化作用是大于碳化作用，经DOC＋SCR处理PM的石墨化程度更低．此外，在流经DOC后PM的表面官能团特征参数发生了明显变化，说明DOC对PM的化学特性产生的影响较大．
由图5可知，随着排气温度的升高，AD1/AG值增加了20%左右．不同工况下D1峰的半峰宽(FWHM)的对比如图6所示；半峰宽表示峰值高度的一半，用于衡量信号或光谱的分辨率、精确性和带宽等特征．应用DOC后，PM的D1峰的FWHM值始终较大．当排气温度大于150℃时，随着排气温度的提升，两个工况下的D1峰的FWHM值均增加．这说明组成颗粒的碳晶体内部的六方对称性在丢失或者失去了对称性，颗粒中晶体的无序程度在增加，原因可能是PM趋于石墨化的外层占比降低；或者颗粒内部氧化造成结构破碎，间接造成PM无序程度加大．所以随着排气温度的提升，DOC会减小PM的石墨化程度．另外，在SCR工况下PM的D1峰的FWHM值没有表现出随排气温度的规律性变化趋势，说明SCR对PM石墨化程度的影响较小．
2.3　催化装置对PM表面官能团的影响
PM表面存在大量不同类型的官能团，官能团的存在影响了PM的氧化特性．主要对含氧官能团(C—O)和碳氢官能团(C—H)进行表征测试，对比分析DOC装置的添加对PM表面官能团的影响．在采集工况中排气温度为250℃、空速为11000h-1，样品收集自SCR和DOC＋SCR两套后处理装置出口．图中部分数据结果通过特征峰面积和总拟合面积的比来获得归一化的数据结果．
图7为不同后处理方式(SCR和DOC＋SCR)下PM的XPS表征结果，对比了碳元素(C 1s)和氧元素(O 1s)的含量．图7(a)和图7(b)对比了C 1s和O 1s的特征峰积分面积A．PM经过DOC处理后，碳元素含量降低，氧元素含量增加，氧与碳的面积比值(AO/AC)由0.08911提升至0.21089，增加了2.4倍．这说明PM经过DOC时，颗粒表面发生了较强的氧化作用，消耗了部分碳，形成了较多的含氧官能团．此外，在颗粒氧化初始阶段，形成的较短微晶提供了大量的活性位点，这些位点可以吸附尾气中大量的氧气，也会导致AO/AC值大幅度增加．AO/AC值增加表明含氧官能团含量的上升，PM的氧化活性增强．具体含氧官能团种类的变化规律，需要对XPS图谱中C 1s峰的精细扫描图谱进行深入分析．
XPS图谱中C 1s峰的精细图谱扫描结果如图8所示，分峰拟合过程中主要分为3种碳原子的杂化形式(SP、SP2和SP3杂化)、C—OH官能团、C＝O官能团和COO官能团．经过DOC处理的PM，C—O官能团的占比提高了一倍，COO官能团占比增加了20%，而C＝O官能团含量相对下降．在PM表面官能团的相关研究中，C—OH官能团是颗粒表面主要的含氧官能团(含量为6.10%～10.57%)，这可能与该官能团的热稳定性有关．因此，PM在流经DOC时发生的表面氧化过程中形成大量C—OH官能团．C＝O官能团的热稳定性较差，DOC内部的氧化放热反应会导致温度上升，破坏部分C＝O官能团，呈现出下降趋势．
此外，图5测试结果也表明，经过DOC后颗粒的石墨化程度减小，碳微晶层边缘处的供给的碳原子增加，使得COO官能团和C—OH官能团的含量增加．
Wang[16]认为C—H官能团是PM外壳结构的主要成分，含量的变化直接影响着颗粒的微观结构和表面氧化性．图9为脂肪族C—H官能团和芳香族C—H官能团含量在两种后处理方式下变化趋势．PM经过DOC处理后，脂肪族C—H官能团含量下降了约50%，芳香族C—H官能团含量有少量的提升，增加幅度最大为6%．说明PM在DOC氧化过程中，主要是脂肪族C—H官能团进行氧化反应，芳香族C—H官能团的反应活性较低．这是因为脂肪族C—H官能团是一种链状结构，其带有短支链的C—H具有更高的活性，更容易与氧气和自由基进行反应．C—H官能团含量的下降说明颗粒在DOC中进行了较为强烈的氧化反应．另外，作为PM生长过程中主要的影响物质，脂肪族C—H官能团含量的下降会进一步降低PM的形成几率．在PM氧化反应中，芳香族C—H官能团热稳定较高，高温下不易分解；并且该类型官能团含量通常会与PM的石墨化程度呈现反比的趋势[16]；所以DOC降低了PM的石墨化程度，芳香族C—H官能团的含量少量提升6%．
DOC的应用会显著影响PM的官能团含量．DOC会增加PM含氧官能团的含量，提升颗粒表面的氧化特性，PM更易处理．DOC还会降低碳氢官能团的含量，尤其是脂肪族C—H官能团含量，会进一步抑制PM的生长或者聚集趋势．
3　结论
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(1) PM流经DOC和SCR后颗粒的石墨化程度降低，颗粒内部有序和对称的碳晶结构发生坍塌和丢失，无序性增加，PM整体的氧化活性得到了提升．
(2) PM经过DOC和SCR后表面官能团的含量发生显著变化；作为PM生长核心的脂肪族C—H官能团被大量消耗，降低了PM的继续生长的机率；含氧官能团含量增加，PM的氧化活性得以增强；在典型的船舶柴油机排放工况下DOC能有效降低船舶柴油机的PM排放，能进一步提高后处理系统的整体催化效率．
基金
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  • 安徽省科技重大专项资助项目(202003a05020023)
文献
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2025年第43卷第1期
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doi: 10.16236/j.cnki.nrjxb.202501009
  • 接收时间：2024-02-09
  • 首发时间：2026-11-06
  • 出版时间：2025-01-25
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  • 收稿日期：2024-02-09
  • 修回日期：2024-06-19
基金
安徽省科技重大专项资助项目(202003a05020023)
作者信息
    1.合肥工业大学汽车与交通工程学院，合肥 230009
    2.安徽江淮汽车集团股份有限公司，合肥 230022

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钱叶剑，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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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
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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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