| RuCo催化剂CO加氢形成含氧物的中间体：甲酰基 |
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| 引用本文： | 肖丰收,市川胜,郭燮贤. RuCo催化剂CO加氢形成含氧物的中间体：甲酰基[J]. 物理化学学报, 1993, 9(1): 56-62. DOI: 10.3866/PKU.WHXB19930110 |
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| 作者姓名： | 肖丰收 市川胜 郭燮贤 |
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| 作者单位： | Department of Chemsitry, Jilin University, Changchun 130023; Catalysis Research Center, Hokkaido University, Sapporo 060, Japan; National Laboratory for Catalysis, Dalian Institute of Chemical Physics, Dalian 116023 |
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| 摘 要： | 进行了在SiO_2担载的Ru-Co双金属原子簇催化剂上合成气(CO+H_2)反应和模型化合物吸附的红外、质谱研究. 结果表明, 在原子簇制备的Ru-Co/SiO_2催化剂上, 在453 K下合成气(CO+H_2)反应在红外谱图产生了1584 cm~(-1)谱带, 它与CO加氢反应中含氧化台物的生成速率成线性关系. 因此提出了此谱峰对应着在CO加氢反应中生成古氧化合物的一个十分重要的中间体. 以CO+D_2、~(13)CO+H_2和~(13)CO+D_2代替CO+H_2, 在Ru-Co/SiO_2催化剂中, 1584 cm~(-1)谱带分别位移至1575、1542和1539 cm~(-1)处. 还观察到, 1584 cm~(-1)物种与H_2反应, 产物给出了CH_4和CH_3OH; 如果1584 cm~(-1)物种和D_2反应则生成CHD_3和CHD_2OD. 这些结果提出了1584 cm~(-1)谱带归属于表面甲酰基的羰基振动, 这同Ru-Co/SiO_2催化剂吸附甲醛的结果基本一致.
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| 关 键 词： | Ru-Co双金属原子簇 含氧化合物 CO加氢反应 表面甲酰基 |
| 收稿时间： | 1991-09-07 |
| 修稿时间： | 1992-03-30 |
FORMYL:AN INTERMEDIATE FOR FORMATION OF OXYGENATES IN CO HYDROGENATION OVER SUPPORTED RuCo CARBONYL CLUSER-DERIVED CATALYSTS |
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| Xiao Fengshou. FORMYL:AN INTERMEDIATE FOR FORMATION OF OXYGENATES IN CO HYDROGENATION OVER SUPPORTED RuCo CARBONYL CLUSER-DERIVED CATALYSTS[J]. Acta Physico-Chimica Sinica, 1993, 9(1): 56-62. DOI: 10.3866/PKU.WHXB19930110 |
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| Authors: | Xiao Fengshou |
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| Affiliation: | Department of Chemsitry, Jilin University, Changchun 130023; Catalysis Research Center, Hokkaido University, Sapporo 060, Japan; National Laboratory for Catalysis, Dalian Institute of Chemical Physics, Dalian 116023 |
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| Abstract: | The reaction and adsorption of syngas and paraformaldehyde on Ru-Co/SiO_2 ca-talysts prepared from Ru-Co bimetallic carbonyl clusters have been investigated byWULI HUAXUE XUEBAO(Acta Phys.Chim)1993 infrared,mass spectroscopies.The spectra of reaction of CO+H_2 with Ru-Co/SiO_2catalysts showed a band appearing at 1584cm~(-1),which has a good relationship to theactivity and selectivity for oxygenates in CO hydrogenation.Thus it was proposedthat 1584cm~(-1) is a possible intermediate to produce oxygenated products.Isotopictracer studies of D_2 and ~(13)CO suggest that 1584cm~(-1) can possibly be assigned to theformyl group,which is in good agreement with the adsorption of paraformaldehyde.The chemical trapping of 1584cm~(-1) adspecies provided an evidence to demonstratethat 1584cm~(-1) is attributed to formyl.The reaction of 1584cm~(-1) species with H_2produced CH_4 and CH_3OH,and the introduction of D_2 into 1584cm~(-1) species resul-ted in the formation of CHD_3 and CHD_2OD. |
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| Keywords: | Ru-Co bimetallic carbonyl cluster Oxygenates CO hydrogenation Surface formyl |
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