磷化镍催化腈类化合物选择性生成伯胺的研究

发布时间：2018-05-14 21:24

本文选题：磷化物 + 氨硼烷　；参考：《云南师范大学》2017年硕士论文

【摘要】：胺类化合物是化学和生物学中一类重要的化合物,广泛应用于医药、精细化工、农用化学品、聚合物、染料生产、颜料和增塑剂的生产。现有的制备伯胺的方法,不仅使用有毒的试剂,而且还有选择性差,原子利用率低等缺点。从经济和环境角度所需,本论文研究了一个高选择性腈还原为伯胺的新合成方法。磷化镍作为双功能催化剂,氨硼烷为氢源,在水与乙醇的体系中,在催化氨硼烷水解释氢同时催化腈类化合物选择性生成相应的伯胺。具有高效催化加氢化学选择性的催化剂,是腈类化合物还原为伯胺的关键。催化剂决定了腈加氢的反应历程生成伯胺,仲胺,叔胺的趋势,选择合适的催化剂及反应体系能有效提高生成伯胺的选择性。本研究的实验体系,建立在磷化镍作为催化剂,对合成伯胺的选择性高,且对腈类衍生物,硝基类衍生物都有较高的催化活性。此外,反应体系是在常温常压下进行,反应体系具有优良的特性:(1)非贵金属磷化物催化剂,尤其是Ni2P,不仅合成容易,具有高效活性,而且可重复使用,无污染;(2)反应是在室温下进行,且在较短反应时间内获得高收益;(3)Ni2P作为双功能催化剂,催化氨硼烷脱氢及其催化腈基或硝基加氢;(4)使用高储氢密度和易于处理的清洁氢源氨硼烷;(5)腈类衍生物在体系中同样获得了很高的选择性;(6)研究显示了该体系能将硝基和腈基同时还原为相应的一级胺,不仅具有优良的转化率,还有很好的化学选择性。
[Abstract]:Amines are important compounds in chemistry and biology. They are widely used in medicine, fine chemicals, agricultural chemicals, polymers, dyestuffs, pigments and plasticizers. The existing methods for the preparation of primary amines not only use toxic reagents, but also have the disadvantages of poor selectivity and low atomic utilization. In this paper, a new synthesis method of high selectivity nitrile reduction to primary amine was studied in terms of economic and environmental requirements. Nickel phosphide was used as bifunctional catalyst and ammonioborane as hydrogen source. In the system of water and ethanol, nickel phosphide was used to interpret hydrogen and selectively catalyze nitrile compounds to produce corresponding primary amines in the system of water and ethanol. The catalyst with high catalytic hydrogenation selectivity is the key to the reduction of nitriles to primary amines. The selectivity of primary amines, secondary amines and tertiary amines can be improved effectively by selecting suitable catalyst and reaction system. The experimental system is based on the high selectivity of nickel phosphide as catalyst for the synthesis of primary amines, and has high catalytic activity for nitrile derivatives and nitro derivatives. In addition, the reaction system is carried out at room temperature and atmospheric pressure. The reaction system has excellent properties: 1) Non-precious metal phosphates catalyst, especially Ni _ 2P, which is not only easy to synthesize, but also has high activity and can be reused. The reaction was carried out at room temperature and in a short reaction time to obtain a high yield of Ni2P as a bifunctional catalyst. Catalytic dehydrogenation of aminoborane and its catalyzing nitrile or nitro hydrogenation using high hydrogen storage density and easy to deal with clean hydrogen source ammonia borane 5) nitrile derivatives have also obtained very high selectivity in the system. Nitro and nitrile groups were reduced to corresponding primary amines at the same time. It has not only excellent conversion, but also good chemical selectivity.
【学位授予单位】：云南师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O643.36;TQ226.31

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