N杂化石墨烯气凝胶制备反应过程研究

Study on the reaction process during the synthesis of nitrogen-doped graphene aerogels

摘要:

以含有氨基的试剂还原氧化石墨烯分散液可以制备含N的石墨烯气凝胶,这种气凝胶应用十分广泛。本文以对苯二胺为还原剂和功能化试剂制备了N杂化石墨烯气凝胶,研究了其制备反应过程。由于羰基的强吸电子效应,对苯二胺上的氨基首先与羧基上的羟基发生反应。之后氨基与醚键发生反应,这一反应不仅向氧化石墨烯上引入了吡咯N,而且改变了其层间距。反应过程很好地解释了N杂化石墨烯气凝胶制备过程中的组成和结构变化,加深了对其制备反应过程的理解,有助于其组成和结构的优化。同时这些发现也有助于理解其它氨基试剂还原制备石墨烯气凝胶的反应过程。

Abstract:

Reducing graphene oxide suspension with amino agent can prepare N-containing graphene aerogels useful in many applications. This work studied the reaction process during the synthesis of N-doped graphene aerogels (NDGA) with p-phenylene diamine (PPD) as reducing and functionalizing agent based on the experimental and calculated results. The amino group in the PPD firstly reacts with the hydroxyl in the carboxyl for the strong electron-donating effect of carbonyl. Then the reaction happens between the amino group and the epoxy group. This reaction not only induces the forming of the pyrrolic N, but also changes the interlayer distance. The reaction process ideally explains the reasons for the structure and composition change during synthesis. This work provides a more thorough understanding of the reaction process during the synthesis of NDGA, which is significant for the optimization of the aerogels. And these findings are also useful for understanding the reaction process and reaction mechanisms during the synthesis of reduced graphene oxide aerogels with other amino agent as reductant.