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催化氧化反应中柴油机碳烟颗粒纳观结构的演化

Nanostructure Changes of Diesel Soot in Catalytic Oxidation Reaction

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【作者】 于潇吕刚乔约翰宋崇林

【Author】 Yu Xiao;Lü Gang;Qiao Yuehan;Song Chonglin;State Key Laboratory of Engines,Tianjin University;

【通讯作者】 吕刚;

【机构】 天津大学内燃机燃烧学国家重点实验室

【摘要】 本文采用热重分析仪构建的催化/非催化氧化反应环境制备了不同氧化程度的碳烟样品,并利用高分辨率透射电子显微镜(HRTEM)和拉曼光谱仪(RS)研究了Pt基催化剂与O2气氛下的催化氧化过程中碳烟纳观结构的变化规律,并与非催化氧化处理的碳烟纳观结构进行了对比分析.结果表明,在整个催化氧化过程中,碳烟基本粒子粒径缩减25%以上,微晶曲率减小,微晶尺寸增加,石墨化程度提高;与非催化氧化处理的碳烟基本粒子对比发现,相同氧化程度下,催化氧化处理的碳烟基本粒子粒径缩减幅度最高增大7.5%,微晶尺寸增加幅度最多减少7%,微晶曲率减少幅度更大;同时,通过比较部分催化氧化碳烟样品与原始碳烟样品的基本粒子纳观结构特征参数发现,催化氧化过程中,尺寸在0.5~0.9 nm及曲率在1.1~1.3的微晶优先被氧化,表明催化作用生成的高活性氧化物种优先氧化短而曲折的微晶,从而提高了碳烟颗粒的石墨化程度.

【Abstract】 In this paper,the soot with different oxidation degrees was treated in catalytic/non-catalytic oxidation reaction environment constructed by thermogravimetric analyzer(TGA). The nanostructure changes of soot particles during catalytic oxidation in the environment of Pt-based catalyst and O2 atmosphere were studied by highresolution transmission electron microscope(HRTEM)and Raman spectroscopy(RS). The nanostructures of soot particles with catalytic oxidation and with non-catalytic oxidation were compared. Experimental results showed that the size of soot particles decreased by more than 25%,the tortuosity of soot particles decreased,the fringe length of soot particles increased,and the graphitization degree of soot increased in the whole catalytic oxidation process.Compared with the non-catalytic oxidized soot particles,it was found that under the same oxidation degree,the extent of particle size reduction of catalytic oxidized soot particles increased by 7.5%,the extent of fringe length increase decreased by 7% maximally,and the decrease of tortuosity was even greater. At the same time,the nanostructural characteristic parameters of partially catalytic oxidized soot particles and original soot particles were compared,and it was found that in the catalytic oxidation process the soot particles with the fringe length of 0.5—0.9 nm and the tortuosity of 1.1—1.3 were preferentially oxidized,indicating that the oxidation active species generated by catalytic oxidation preferentially oxidized soot particles with short and flexural fringes,thus improving the graphitization degree of soot particles.

【关键词】 碳烟氧化催化剂纳观结构石墨化程度
【Key words】 sootoxidationcatalystnanostructuregraphitic degree
【基金】 国家自然科学基金资助项目(51876142);天津市自然科学基金重点资助项目(19JCZDJC40100)
  • 【文献出处】 燃烧科学与技术 ,Journal of Combustion Science and Technology , 编辑部邮箱 ,2023年03期
  • 【分类号】TK421.5
  • 【下载频次】12
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