摘要
CO_2 is one of the most important ＂renewable＂ carbon sources.To transform CO_2 to useful organic compounds,we examined the reactivity of two model silicon-based ＂waste＂ materials,disilanes and metallic Si powder,as reducing agents.In these reactions,fluoride salts were found to be active catalysts：CO_2 was converted to formic acid at atmospheric pressure in the presence of H_2O as a proton source and the silicon-based reducing reagents.Based on in-situ NMR and kinetics analyses,a hydrosilane and penta-coordinate Si species are proposed as the reaction intermediate and active species,respectively.
CO_2是最重要的可再生碳源之一.为了将CO_2转化为有用的有机化合物,我们研究了二种模型硅基"废"材料—乙硅烷和硅粉的反应活性.在这些反应中,氟盐的催化活性最高,在常压、在质子源水和硅基还原剂的存在下,CO_2可转化为甲酸.原位NMR和动力学分析表明,含氢硅烷和五配位的硅物种分别是反应中间物和活性物种.
基金
supported by JSPS KAKENHI(15H04182)
JSPS Grant-in-Aid for Scientific Research on Innovative Areas "3D Active-Site Science(26105003)","Precisely Designed Catalysts with Customized Scaffolding(16H01010)"
Grant for Challenging Research Award,Tokyo Institute of Technology
