Detection, role and utilization of excited molecules in catalytic reaction by means of IR chemiluminescence

红外化学发光法检测催化反应中激发分子的作用和利用

基本信息

批准号：
17560679
负责人：
KUNIMORI Kimio
金额：
$ 2.36万
依托单位：
University of Tsukuba
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2005
资助国家：
日本
起止时间：
2005 至 2007
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-17560679/
关键词：
IR chemiluminescence Vibrationally-excited molecules Dynamics of catalytic reaction Molecular beam of excited methane Production of CO and H_2 メタン・エタン励起分子線

IR chemiluminescence Vibrationally-excited molecules Dynamics of catalytic reaction Molecular beam of excited methane Production of CO and H_2 メタン・エタン励起分子線

项目摘要

(1) Dynamics of catalytic reactions by measurement of IR emission of the vibrationally-excited product molecules(1-1) CO+O_2 reaction on Pd (110), Pd (111)Analysis method using intensities of IR emission was proposed, and changes in vibrational temperatures were measured with increasing surface temperature.(1-2) CO+NO reaction on Pd (110), Pd (111)Large structure-sensitivity in the activity of the CO+NO reaction was found for the first time. NO Dissociation does not take place on Pd (111), and nascent oxygen from NO is formed on Pd (110) because NO dissociation is limited.(1-3) CO+0_2 reaction on Pt (110), Pt (111)Activity was higher on Pt (110) than on Pt (111). Changes in vibrational temperatures were observed due to the reconstruction of (l x l) into (1 x 2) on Pt (110).(2) Direct catalytic partial oxidation of CH_4 and C_2H_6 using heatable and seeded molecular beam technique(2-1) The promoting effect of energetic activation of a methane molecular beam: production of syngasCO+H_2 (in particular H_2) were produced selectively during steady-state CH_4+O_2 reaction on Pt by exciting methane. The reaction also takes place on Rh by reducing O_2.(2-2) Comparative study between methane and ethane in the catalytic paratial reaction on Pt and RhBased on the results of the reaction order measurements one possible explanation for the promotion is that energetically activated methane and ethane react with adsorbed oxygen and produce methoxy and ethoxy species, which are regarded as precursors for hydrogen formation.

（1）通过测量IR发射的IR发射的振动振动产物分子（1-1）CO+O_2在PD上的反应（110），PD（111）分析方法使用IR发射的强度分析方法，并提出了振动温度的变化（110）CO（1-2）CO（110）（110）（110）（110）（110）（110）（110）（110）（110）（110）（110）。在CO+的活性中，第一次没有反应。在PD（111）上不进行解离，并且在PD（110）上形成了NO的新生氧，因为没有分离受到限制。（1-3）CO+0_2 PT上的反应PT（110），PT（111）的PT（111）活性在Pt（110）上（110）高于PT（111）。由于（110）对（1 x 2）重建（1 x 2），观察到振动温度的变化。（2）使用可热和播种分子束技术（2-1）使用甲烷束的促进效应，是甲烷的生产+hhsygasco syngasco的促进效应，直接催化CH_4和C_2H_6的c_2H_6氧化。在稳态CH_4+O_2在PT上通过刺激的甲烷反应。该反应还通过降低O_2。（2-2）在PT上的催化性负体反应中的甲烷和乙烷之间的比较研究，并根据反应顺序测量结果的结果进行了促进的一种可能的解释，即能量活化活化活化的甲烷和乙烷与吸附的氧气和产生甲氧含量和氧化物的形式，这些甲烷反应与甲氧含量和氧化物相关的形式，这些形式是水分的精良。