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Mechanism of Coal Liquefaction - Reaction of Model Compounds

煤液化机理-模型化合物的反应

基本信息

批准号：
02650595
负责人：
ITOH Hironori
金额：
$ 1.28万
依托单位：
Hokkaido University
依托单位国家：
日本
项目类别：
Grant-in-Aid for General Scientific Research (C)
财政年份：
1990
资助国家：
日本
起止时间：
1990 至 1991
项目状态：
已结题

项目摘要

Benzyl phenyl ether and dibenzyl as model compounds of coal were hydrogenolyzed under high pressure of hydrogen in the presence of stabilized nickel or synthetic pyrite as the catalyst to elucidate the reaction mechanism of coal liquefaction. The reactions were carried out at 250-500ﾟC, under 3-10MPa of hydrogen for 0-60inin with naphthalene, tetralin and decalin as the solvent.In the case of stabilized nickel used as catalyst, which has strong ability in hydrogenation, the benzene rings of benzyl phenyl ether or dibenzyl were hydrogenated at 250-350ﾟC. Benzyl phenyl ether was split at C-0 bond almost completely at 250ﾟC and converted to phenol and toluene. Phenol was easily hydrogenated to cyclohexanol. At the higher temperature than 370ﾟC, cyclohexane and benzene increased due to dehydroxylation and dehydrogenation. With the increase in hydrogen pressure, hydrogenation and dehydroxylation accelated and gas formation and condensation were reduced.In the case of the synthetic pyrite as catalyst, benzyl phenyl ether produced little the hydrogenated products because of the weak hydrogenation ability. The larger amount of the condensed products such as dibenzyl phenol or tribenzyl phenol were produced in the reaction with decalin as solvent. These condensed products were produced in the early stage of reaction and then decomposed to benzyl phenol, phenol and toluene as the reaction proceeded. Djbenzyl reacted little at the lower temperature than 450ﾟC with the synthetic pyrite, that is difference from the stabilized nickel.

以苄基苯基醚和二苄基为煤的模型化合物，在稳定镍或合成黄铁矿催化剂存在下，在高压氢气下进行氢解反应，以阐明煤液化的反应机理。以萘、四氢萘、十氢萘为溶剂，在250-500 ℃，氢气压力3- 10 MPa，反应时间0- 60 min的条件下，以加氢能力强的稳定镍为催化剂，在250-350 ℃下对苄基苯基醚或二苄基的苯环进行加氢。苄基苯基醚在250 ℃时在C-0键上几乎完全裂解，转化为苯酚和甲苯。苯酚易于加氢生成环己醇。在高于370 ℃的温度下，环己烷和苯由于脱羟基和脱氢而增加。随着氢压的增加，加氢和脱羟基反应加速，气体生成和缩合反应减少，在合成黄铁矿催化剂上，苄基苯醚加氢能力弱，加氢产物生成少。以十氢萘为溶剂时，生成的缩合产物较多，如二苄基苯酚、三苄基苯酚等。这些缩合产物在反应初期生成，然后随着反应的进行分解为苄基苯酚、苯酚和甲苯。在低于450 ℃的温度下，二苄基与合成黄铁矿几乎不发生反应，这与稳定镍不同。