N-杂环的催化氧化脱氢的研究进展

Research Progress of Catalytic Oxidative Dehydrogenation of N-Heterocycles

由于氢气高质量能量密度(120MJ·kg^(-1))和无碳燃烧产物,其生产正越来越多地与过剩的可再生电力相结合。但是以氢作为储能介质仍然无法大规模利用,主要障碍在于氢不利的元素特性。N-杂环或其他能与氢气结合并在环境条件下储存的化合物,为克服经典的氢气储存加氢和脱氢释放有关的问题提出了一个替代方案。探索一种简单、高效、稳定和绿色的催化体系是实现这一典型转化的关键。总结了过去5年来开发Ru、Ni、Co、Fe和Mn催化剂与n杂环化合物催化氧化脱氢反应所取得的显著进展,期望这一领域的研究结果能够启发其他人进一步制备新型高效、可控和绿色的催化剂,用于氢的借用或氢气转移的应用,从而能够促进在不久的将来建立适合燃料电池的供氢体系。

Due to its high gravimetric energy density(120 MJ·kg^(-1))and carbon-free combustion products,hydrogen production is increasingly being integrated with surplus renewable electricity.The primary hindrance for large scale hydrogen utilization as an energy storage medium lies in its unfavorable elemental properties.N-heterocycles or other chemical compounds to which hydrogen is bound to and stored at ambient conditions,present a promising alternative to overcome the problems.Thence,catalytic oxidative dehydrogenation of N-heterocycles maybe a promising pathway that can not only improve the hydrogen storage and release,transportation and distribution,but also supply hydrogen with stable trend.Thus,the key point is needed to explore a simple,efficient,stable and green catalytic system to achieve this typical transformation.In this paper,the remarkable progress in developing Ru,Ni,Co,Fe,and Mn catalysts in the past five years for catalytic oxidative dehydrogenation reactions with N-heterocyclic compounds was summarized,expecting that the findings in this field will inspire others to further fabricate new high-efficient,controllable and green catalysts for borrowing hydrogen or hydrogen transfer applications.