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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

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)催化反应动力学通过测量Pd(110)上振动激发产物分子(1-1)CO+O_2的红外发射，提出了用红外发射强度分析Pd(111)反应的方法，并测量了振动温度随表面温度的变化。(1-2)CO+NO在Pd(110)，Pd(111)上的反应首次发现了CO+NO反应活性的结构敏感性。(1-3)CO+O_2在铂(110)上的反应活性高于在铂(111)上的活性。(2)甲烷分子束直接催化部分氧化CH_4和C_2H_6(2-1)甲烷分子束的能量活化促进效应：甲烷在稳态CH_4+O_2反应中选择性地生成合成气CO+H_2(特别是H_2)。(2-2)甲烷和乙烷在铂和罗丹明上催化平行反应的对比研究根据反应级数的测定结果，一个可能的解释是，高能活化的甲烷和乙烷与吸附的氧反应生成甲氧基和乙氧基物种，它们被认为是生成氢的前驱物质。