铁基燃油添加剂对柴油机排气颗粒物理化特性的影响
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摘要
在国Ⅴ标准0~#车用柴油中分别添加质量分数为150μg/g、300μg/g的铁基添加剂(Fe-FBC),制备Fe150和Fe300两种燃油,并基于发动机台架试验,采用颗粒采样分析仪进行排气颗粒采集。运用热重分析仪和扫描电镜研究颗粒物热解性质与微观形貌结构,采用傅里叶红外光谱仪和光电子能谱仪对颗粒表面官能团进行半定量分析。结果表明:在发动机额定工况下,加入Fe-FBC后排气颗粒干碳烟质量分数降低,氧化温度与表观活化能均有显著下降;相比于纯柴油燃烧颗粒物的积聚体形态,Fe300燃烧颗粒物的团聚程度变弱,存在较多的链状结构;颗粒表面官能团拥有较多的—OH键与C—H键,C—H键为饱和烃CH_3结构;颗粒微晶边缘碳原子更加混乱,石墨化程度降低,容易被氧化;Fe300燃烧颗粒物中C元素含量降低,O元素含量增加,Fe元素价态为+2和+3价,颗粒表面吸附有更多能与Fe元素相结合的含氧基团。
Fe-based additives(Fe-FBC) were added to 0~# diesel(China Ⅴ) with Fe mass fraction of 150 μg/g and 300 μg/g respectively to prepare two blended fuels, which were named as Fe150 and Fe300 correspondingly. On a test bench, AVL Smart Sampler was used to collect exhaust particles at the rated power of the test engine. Thermogravimetric Analysis and Scanning Electron Microscopy were employed to study the micro-morphology of the particles. Fourier Transform Infrared Spectrometer and X-ray Photoelectron Spectrometer were used to analyze the surface functional groups of the particles. The experimental results show that the mass fraction of dry soot decreases with the addition of Fe-FBC, and it was also found both the oxidation temperature and activation energy of the above dry soot decrease significantly. Compared with the agglomeration morphology of particles from normal diesel, particles from Fe300 have less aggregation degree and more chain structures. In addition, for particles from Fe300, their surface functional groups have more —OH and C—H chemical bonds, and C—H bonds are saturated CH_3 structures. For particles from Fe300, it also can be observed that carbon atoms at the edge of granular microcrystalline are more chaotic and the graphitization degree decreases. All the above characteristics indicate that the emission particulates from Fe300 are much easier to be oxidized. Compared with emission particles from normal diesel, there are less carbon contents but more oxygen contents for Fe300 emission particles, in which the valences of most Fe are +2 and +3. As well, more oxygen-containing groups are combined with Fe on the surface of Fe300 emission particles.
Fe-based additives(Fe-FBC) were added to 0~# diesel(China Ⅴ) with Fe mass fraction of 150 μg/g and 300 μg/g respectively to prepare two blended fuels, which were named as Fe150 and Fe300 correspondingly. On a test bench, AVL Smart Sampler was used to collect exhaust particles at the rated power of the test engine. Thermogravimetric Analysis and Scanning Electron Microscopy were employed to study the micro-morphology of the particles. Fourier Transform Infrared Spectrometer and X-ray Photoelectron Spectrometer were used to analyze the surface functional groups of the particles. The experimental results show that the mass fraction of dry soot decreases with the addition of Fe-FBC, and it was also found both the oxidation temperature and activation energy of the above dry soot decrease significantly. Compared with the agglomeration morphology of particles from normal diesel, particles from Fe300 have less aggregation degree and more chain structures. In addition, for particles from Fe300, their surface functional groups have more —OH and C—H chemical bonds, and C—H bonds are saturated CH_3 structures. For particles from Fe300, it also can be observed that carbon atoms at the edge of granular microcrystalline are more chaotic and the graphitization degree decreases. All the above characteristics indicate that the emission particulates from Fe300 are much easier to be oxidized. Compared with emission particles from normal diesel, there are less carbon contents but more oxygen contents for Fe300 emission particles, in which the valences of most Fe are +2 and +3. As well, more oxygen-containing groups are combined with Fe on the surface of Fe300 emission particles.
引文
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[25]俞瑶,吕刚,宋崇林,等.氧化反应温度对柴油机颗粒物表面官能团演变的影响[J].燃烧科学与技术,2016,22(1):37-44.(YU Yao,LGang,SONG Chonglin,et al.Impact of oxidation reaction temperature on surface functional groups transformation of diesel particles[J].Journal of Combustion Science&Technology,2016,22(1):37-44.)
[26]王世昌,姚强,胡刚刚.我国动力煤TGA法表观活化能/指前因子分布规律[J].煤炭学报,2013,38(6):1078-1083.(WANG Shichang,YAO Qiang,HUGanggang.Distribution of apparent activation energy and apparent pre-exponential factor of Chinese power coals from TGA method[J].Journal of China Coal Society,2013,38(6):1078-1083.)
[2]刘少康,孙平,刘军恒,等.铈基燃油催化剂改善柴油机颗粒物捕集器再生效果[J].农业工程学报,2016,32(1):112-117.(LIU Shaokang,SUN Ping,LIUJunheng,et al.Ce-based fuel borne catalyst enhancing regenerative effect of diesel particulate filter[J].Transactions of the Chinese Society of Agricultural Engineering,2016,32(1):112-117.)
[3]陈明虎,孙泽,祝先标,等.FBC添加剂对发动机及DPF的影响研究[J].汽车实用技术,2017(10):129-131.(CHEN Minghu,SUN Ze,ZHU Xianbiao,et al.The influence of FBC additives on engine and DPFresearch[J].Automobile Applied Technology,2017(10):129-131.)
[4]马林才.柴油发动机环保型高效燃料添加剂的研究[J].石油学报(石油加工),2007,23(2):93-98.(MALincai.Study of environmental protecting and high effective fuel additive for diesel engine[J].Acta Petrolei Sinica(Petroleum Processing Section),2007,23(2):93-98.)
[5]NASH D G,SWANSON N B,PRESTON W T,et al.Environmental implications of iron fuel borne catalysts and their effects on diesel particulate formation and composition[J].Journal of Aerosol Science,2013,58(4):50-61.
[6]王玉梅,孙平,冯浩杰,等.柴油机燃用铁基FBC燃油的微粒排放特性[J].浙江大学学报(工学版),2017,51(10):1981-1987.(WANG Yumei,SUN Ping,FENG Haojie,et al.Particulate emission characteristics of diesel engine fueled with diesel and Fe-FBC blends[J].Journal of Zhejiang University(Engineering Science),2017,51(10):1981-1987.)
[7]HARVEL G D,CHANG J S,TUNG A,et al.Threedimension deposited soot distribution measurement in silicon carbide diesel particulate filters by dynamic neutron radiography[C]//Detroit:SAE 2011 World Congress&Exhibition,2011.
[8]WANG D,LIU Z C,HAN Y Q,et al.Experimental studies on pressure drop performance and regeneration safety of diesel particulate filter[C]//Wuhan:International Conference on Electric Information and Control Engineering,2011:2175-2178.
[9]TWIGG M V.Progress and future challenges in controlling automotive exhaust gas emissions[J].Applied Catalysis B Environmental,2007,70(1/2/3/4):2-15.
[10]王丹,刘忠长,王忠恕,等.柴油机微粒捕集器缸内次后喷主动再生方法[J].吉林大学学报(工学版),2012,42(3):551-556.(WANG Dan,LIU Zhongchang,WANG Zhongshu,et al.Diesel particulate filter active regeneration by in-cylinder late post injection[J].Journal of Jilin University(Engineering and Technology Edition),2012,42(3):551-556.)
[11]ALKEMADE U G,SCHUMANN B.Engines and exhaust after treatment systems for future automotive applications[J].Solid State Ionics,2006,177(26):2291-2296.
[12]田径,韩永强,刘忠长,等.柴油机燃油催化微粒后处理器性能与再生[J].吉林大学学报(工学版),2011,41(1):18-23.(TIAN Jing,HAN Yongqiang,LIUZhongchang,et al.Performance and regeneration of diesel particulate filter with fuel borne catalyst on diesel engine[J].Journal of Jilin University(Engineering and Technology Edition),2011,41(1):18-23.)
[13]ZHANG Z H,BALASUBRAMANIAN R.Influence of an iron-based fuel-borne catalyst on physicochemical and toxicological characteristics of particulate emissions from a diesel engine[J].Applied Energy,2015,146(3/4):270-278.
[14]张川,孟忠伟,陈超,等.铁基燃油添加剂对柴油机颗粒排放影响的试验研究[J].车用发动机,2016(2):88-92.(ZHANG Chuan,MENG Zhongwei,CHEN Chao,et al.Experimental investigation on influence of Febased fuel additive on diesel engine particle emission[J].Vehicle Engine,2016(2):88-92).
[15]NEEFT J P A,PRUISSEN O P V,MAKKEE M,et al.Catalysts for the oxidation of soot from diesel exhaust gasesⅡ:Contact between soot and catalyst under practical conditions[J].Applied Catalysis B:Environmental,1997,12(1):21-31.
[16]王玉梅.铁基FBC影响柴油机颗粒物氧化特性的试验研究[D].镇江:江苏大学,2017.
[17]van GULIJK C,MARIJNISSEN J C M,MAKKEE M,et al.Measuring diesel soot with a scanning mobility particle size and an electrical low-pressure impactor:Performance assessment with a model for fractal-like agglomerates[J].Aerosol Science,2004,35(5):633-655.
[18]何振娟,王录全,庾正伟,等.基于MATLAB和分形理论的复合材料第二相颗粒分布均匀性评价方法[J].中国粉体技术,2014,20(3):76-79.(HE Zhenjuan,WANG Luquan,YU Zhengwei,et al.Evaluation method of uniformity distribution of second phase particles in composites based on MATLAB and fractal theory[J].China Powder Science&Technology,2014,20(3):76-79.)
[19]王忠,杨丹,冯渊,等.氧化时间对生物柴油性能及排放的影响[J].石油学报(石油加工),2017,33(5):959-965.(WANG Zhong,YANG Dan,FENG Yuan,et al.Effect of biodiesel oxidation stability on diesel engine performance and emission[J].Acta Petrolei Sinica(Petroleum Processing Section),2017,33(5):959-965.)
[20]GILHAM R J J,SPENCER S J,BUTTERFIELD D,et al.On the applicability of XPS for quantitative total organic and elemental carbon analysis of airborne particulate matter[J].Atmospheric Environment,2008,42(16):3888-3891.
[21]瞿磊,王忠,李铭迪,等.正丁醇/柴油燃烧颗粒的碳官能团及氧化活性研究[J].中国电机工程学报,2016,36(16):4484-4489.(QU Lei,WANG Zhong,LIMingdi,et al.Study on the carbon functional groups and oxidation activity of n-butanol/diesel combustion particles[J].Proceedings of the CSEE,2016,36(16):4484-4489.)
[22]HU C,LI W,LIN Q,et al.Impact of ferrocene on the nanostructure and functional groups of soot in a propane/oxygen diffusion flame[J].RSC Advances,2017,7(9):5427-5436.
[23]MLLER J O,SU D S,JENTOFT R E,et al.Morphology-controlled reactivity of carbonaceous materials towards oxidation[J].Catalysis Today,2005,102/103:259-265.
[24]SU D S,JENTOFT R E,MLLER J O,et al.Microstructure and oxidation behaviour of Euro IV diesel engine soot:A comparative study with synthetic model soot substances[J].Catalysis Today,2004,90(1/2):127-132.
[25]俞瑶,吕刚,宋崇林,等.氧化反应温度对柴油机颗粒物表面官能团演变的影响[J].燃烧科学与技术,2016,22(1):37-44.(YU Yao,LGang,SONG Chonglin,et al.Impact of oxidation reaction temperature on surface functional groups transformation of diesel particles[J].Journal of Combustion Science&Technology,2016,22(1):37-44.)
[26]王世昌,姚强,胡刚刚.我国动力煤TGA法表观活化能/指前因子分布规律[J].煤炭学报,2013,38(6):1078-1083.(WANG Shichang,YAO Qiang,HUGanggang.Distribution of apparent activation energy and apparent pre-exponential factor of Chinese power coals from TGA method[J].Journal of China Coal Society,2013,38(6):1078-1083.)