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	铑催化合成气制乙醇反应中CO断键途径的研究; The Pathway For Cleavage of C O Bond of CO in Syngas Conversion to Ethanol over Rhodium Catalysts
	汪海有 ; 刘金波 ; 许金来 ; 傅锦坤 ; 林种玉 ; 张鸿斌 ; 蔡启瑞
	1994
关键词	铑 合成气 乙醇 CO断键 Rhodium Syngas Ethanol C-O bond cleavage.
英文摘要	利用程序升温表面反应─红外（TPSr-Ir）动态技术考察CO吸附物种对氢的反应性能并检验表面反应生成的中间物，结果表明线式CO对氢的反应性能高于桥式CO，即线式CO更可能是活性吸附态；表面反应生成了HCO、CH2等中间物.用键级守恒（bOC）-MOrSE势方法计算比较了CO→CH2过程中各可能基元步骤在rH（111）面上的反应活化能和反应热，结果表明CO经其部分氢化物种（如H2CO、HCOH）的氢解反应断裂C─O键在能量上最有利.根据这些实验结果，提出铑基催化剂上合成气转化反应主要按缔合式机理进行；CO的优势断键途径为先部分氢化，而后氢助断键.; The main pathway For C-O bond cleavage in ethanol Formation reaction has been studied by using TPSR-IR dynamic method and Bond-Order-Conservation(BOC)-Morse potential approach.The partially hydrogenated CO species, H CO(1589 cm(-1)),and CH2 species(2933 cm(-1))are simultaneously detected by IR in CO adsorption-TPSR(in H2 Flow) dynamic process over Rh-Mn(1:1)/SiO2 catalyst,and a good correlation between the detected surFace Formyl intensity and the ethanol activity is also observed,implying that Formyl species is a key intermediate in the ethanol synthesis and that C-O bond cleavage occurs From a partially hydrogenated CO species.BOC-Morse potential approach predicts the activation energies For C-O bond cleavage on Rh(111) surFace according to dissociation mechanisms(including direct and hydrogen assisted dissociation of adsorbed CO)and association mechanisms(including direct and hydrogen assisted dissociation of partially hydrogenated CO such as H CO,H2 CO,HCOH),showing that the activation energy For hydrogen assisted dissociation of H2CO(or H COH)is the lowest.Based on the results of IR study and BOC calculation,it may be concluded that C-O bond cleavage occurs via hydrogen assisted dissociation of partially hydrogenated CO species.; 国家自然科学基金
语种	zh_CN
内容类型	期刊论文
源URL	[http://dspace.xmu.edu.cn/handle/2288/107312]
专题	化学化工－已发表论文
推荐引用方式 GB/T 7714	汪海有,刘金波,许金来,等. 铑催化合成气制乙醇反应中CO断键途径的研究, The Pathway For Cleavage of C O Bond of CO in Syngas Conversion to Ethanol over Rhodium Catalysts[J],1994.
APA	汪海有.,刘金波.,许金来.,傅锦坤.,林种玉.,...&蔡启瑞.(1994).铑催化合成气制乙醇反应中CO断键途径的研究..
MLA	汪海有,et al."铑催化合成气制乙醇反应中CO断键途径的研究".(1994).

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