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煤高温快速液化过程中的单原子与双原子氢转移机理

     

摘要

氢转移对煤的加氢液化至关重要,理解氢转移机理对于改善煤液化过程具有重要意义。在微型反应釜中通过考察氢气的溶解、溶剂类型以及不同类型催化剂对煤高温快速液化的影响,揭示了煤高温快速液化过程中单原子氢和双原子氢的转移机理。结果表明,在以四氢萘、氢气为条件的高温快速液化过程中,主要的活性氢来源于溶剂所提供的单原子;在以四氢萘、氮气为条件的高温快速液化过程中,不同催化剂对溶剂提供单原子氢的影响不同。在以四氢萘和萘、氢气为条件的高温快速液化过程中,双原子氢基本未参与液化反应,溶解并不是其参与液化反应的主要影响因素。以萘为溶剂、氢气气氛下的高温快速液化过程中,双原子氢参与反应需要一定的时间。在以萘或四氢萘、氢气为条件的高温快速液化过程中通过加入一定量的催化剂,可以促使双原子氢快速参与反应。%Hydrogen transfer is crucially important for coal hydroliquefaction, so the understanding of the hydrogen transfer mechanism is of great significance to improve the coal liquefaction process. By examining the effect of pre-dissolved hydrogen, solvent types and different types of catalysts on the quick coal liquefaction at high temperature in a micro stirred reactor, this paper reveals the monatomic and biatomic hydrogen transfer mechanism during quick coal liquefaction at high temperature in a micro autoclave. The results show that the active hydrogen is mainly provided by monatomic hydrogen generated from solvent with tetralin and hydrogen as hydrogen resource. The effects of different catalysts on monatomic hydrogen donation of solvent are different under the condition of tetralin and nitrogen. In naphthalene and hydrogen, biatomic hydrogen needs a certain time to take part in coal direct liquefaction reaction. In tetralin, naphthalene and hydrogen, a certain amount of catalysts can quickly promote biatomic hydrogen to take part in the coal direct liquefaction reaction.

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