温室气体二氧化碳化学转化与利用的方法学

Methodologies for Chemical Utilization of Carbon Dioxide

二氧化碳既是温室气体的主要组成又是储量丰富的碳资源,研究二氧化碳的化学转化和利用有着重要的意义。基于二氧化碳与催化剂的弱相互作用以及催化活化原理,通过采用环境友好的反应介质(如超临界二氧化碳、聚乙二醇和离子液体等)及催化剂的设计、分离和循环利用策略,设计各类单组分双功能或双组分双功能的高效催化剂用于合成有机碳酸酯和唑啉酮类化合物,建立具有重要工业应用背景的碳酸酯、唑啉酮和羧酸酯合成新方法以及环境友好的新工艺。超临界二氧化碳既作为一种反应物(可再生资源),又作为环境友好、性质可调的反应介质。在高密度二氧化碳体系中的聚乙二醇自由基化学是一个环境友好的氧化体系。在一定的条件下,聚乙二醇通过氧化降解产生的自由基能应用于脂肪醇的甲酰化、苄醇的氧化、C-H键的活化等氧化反应。

Development of catalytic methods for chemical transformation of CO2 into useful compounds is of paramount importance from a standpoint of C1 chemistry and so-called green chemistry and sustainable development. Based on its activation via either metal coordination or weak interaction between active species and CO2 molecule, a variety of catalysts have been developed for the synthesis of organic carbonates and oxazolidinones, where the environmentally benign media have been used and the separation process is very simple. A concept and device originating from free-radical chemistry of PEG thermal degradation in conjunction with compressed CO2 would herein be introduced, whereby PEG radical assumed to be generated from PEG thermal oxidative degradation to successfully initiate a broad spectrum of free radical reactions in a practically utilizable manner with cost-efficient and environmentally friendly benefits, in which PEG/O2/CO2 acts as initiator, oxidant and solvent, respectively.