基于COFs衍生杂原子掺杂碳纳米片构筑高效全固态FLPs非金属加氢催化剂及催化性能

目前常用的金属加氢催化剂存在活性组分易流失、失活、污染产品及环境等问题，开发H2为氢源的非金属加氢催化剂显得尤为重要。近年来提出的“受阻路易斯酸碱对”(FLPs)分子体系虽加氢活性高，但稳定性差且难以循环使用。项目针对上述问题，提出基于FLPs概念，利用共价有机框架材料（COFs）构筑新型高效B,N-及B,P-共掺杂碳纳米片全固态FLPs非金属加氢催化剂。围绕材料中B/N FLPs及B/P FLPs活性位点空间构型及活性位点-H2-底物间作用机制关键问题，探究COFs自模板特性、基底中杂原子与引入的B、N、P杂原子共掺杂规律及催化剂构-效关系，获得新型高效非金属加氢催化剂可控制备方法；结合分子模拟计算和原位表征手段揭示反应机理。项目可为低成本、环境友好碳基全固态FLPs非金属加氢催化剂设计及应用提供借鉴，对推动共掺杂碳纳米片全固态FLPs非金属催化剂应用及拓展FLPs化学理论具有重要意义。

Currently commonly used metal hydrogenation catalysts have the problem of loss of active component, deactivation, contamination of products and environment, hence it is important to research and development metal free hydrogenation catalysts using hydrogen as hydrogen source. The Frustrated Lewis Pairs (FLPs) molecular system proposed in recent years has the advantage of high hydrogenation activity. However, it is unstable and it is hard to be recycled. To resolve above mentioned problems, this project propose to construction of newly highly active B,N- and B,P- co-doped carbon nanosheet all-solid state FLPs metal free hydrogenation catalysts based on conception of FLPs and covalent organic framework materials. Revolving around the key problem of spatial configuration of B/N FLPs and B/P FLPs and the action mechanism among the active sites-H2-substrate, the self template property of COFs, the co-doped law between the basal heteroatom and the introduced B, N, P heteroatom, and the structure-activity relationship of catalysts will be studied so as to obtain the controllable preparation method of newly highly active metal free hydrogenation catalyst and reveal the reaction mechanism combining molecular simulation calculations and in situ characterizations. The project can provide reference for design and application of low-cost, environment-friendly carbon based all-solid state FLPs metal free hydrogenation catalysts, and is of great significance for promoting the application of co-doped carbon nanosheet all-solid state FLPs metal free hydrogenation catalysts and broadening FLPs chemical theory.