中文摘要：

随着全球“温室效应”和能源危机的加剧,近几年二氧化碳作为一种丰富、无毒、廉价的碳一原料广受关注.目前,在温和条件下实现二氧化碳的化学转化仍然是一个十分具有挑战性的课题,其关键的科学问题是二氧化碳分子的有效活化.本文发现,在不添加任何助催化剂的条件下,季膦盐型双功能金属Salen配合物不仅能够以有机胺、含氢硅烷和二氧化碳为原料,在温和条件下通过N-甲酰化反应实现系列甲酰胺类衍生物的高效合成,而且能够催化二氧化碳和环氧化合物的环加成反应,从而实现环状碳酸酯的宏量制备.

英文摘要：

The chemical transformation of CO2under mild conditions remains a great challenge because of itsexceptional kinetic and thermodynamic stability.Two important reactions in the transformation ofCO2are the N‐formylation reaction of amines using hydrosilanes and CO2,and the cycloaddition ofCO2to epoxides.Here,we report the high efficiency of bifunctional metallosalen complexes bearingquaternary phosphonium salts in catalyzing both of these reactions under solvent‐free,mild conditionswithout the need for co‐catalysts.The catalysts’bifunctionality is attributed to an intramolecularcooperative process between the metal center and the halogen anion.Depending on the reaction,this activates CO2by permitting either the synergistic activation of Si–H bond via metal–hydrogen coordinative bond(M–H)or the dual activation of epoxide via metal–oxygen coordinativebond(M–O).The one‐component catalysts are also shown to be easily recovered and reusedfive times without significant loss of activity or selectivity.The current results are combined withprevious work in the area to propose the relevant reaction mechanisms.