CO_(2)催化制备高附加值多碳含氧化合物的研究进展

Research progress on CO_(2) catalytic conversion to value-added oxygenates

将温室气体CO_(2)通过化学反应路径制备高附加值多碳含氧化合物如乙醇、乙酸、丙醛、丙酸、丁醇等具有挑战性。由于C-C偶联反应的复杂性和成键的不可控性,导致合成多碳高值含氧化合物困难。本工作总结了近期在连续流固定床条件下CO_(2)催化合成高附加值多碳含氧化合物的研究进展。首先归纳了CO_(2)加氢路径下可能的反应机理;其次总结了CO_(2)直接加氢(一步法、串联法)、CO_(2)与轻烃重整、CO_(2)氢甲酰化等不同反应路径下具有潜力的催化剂,包括金属碳化物、碱金属修饰的Cu、Fe、Co、Rh等单金属或二元金属制备多碳高值含氧化合物的特点,并进一步阐述了不同催化剂上的作用机制。最后对目前存在的问题和未来可能的解决方案进行了讨论和展望。

Chemical conversion of greenhouse gas CO_(2) into value-added oxygenates such as ethanol,acetic acid,propanal,propionic acid,butanol,etc.is challenging due to the complexity of C−C coupling and the uncontrollable bonding.In this review,recent research progresses on the synthesis of multi-carbon oxygenates from CO_(2) in fixed bed reactor are provided.Firstly,the reaction mechanisms of CO_(2) hydrogenation are summarized.Then,the potential catalysts applied in one-step or tandem CO_(2) hydrogenation,dry reforming with light hydrocarbons and hydroformylation were introduced over metal carbides,alkali metal modified single or binary metal catalysts such as Cu,Fe,Co,Rh,etc.The reaction mechanism over different catalysts were further elaborated.Finally,the problems and outlook are discussed.