Considering the importance of the valorization of CO_(2),a number of phosphine-containing ruthenium pincer complexes have been successfully heterogenized using a“direct knitting”strategy without any premodification....Considering the importance of the valorization of CO_(2),a number of phosphine-containing ruthenium pincer complexes have been successfully heterogenized using a“direct knitting”strategy without any premodification.The resulting porous organometallic polymers(POMPs)with high specific-surface areas,hierarchical pores,and uniformly dispersed Ru single-sites exhibited outstanding catalytic activity toward the N-formylation of diverse amines with CO_(2).Besides excellent turnover number(TON,5×10^(5))and turnover frequency(TOF,5592 h-1),the obtained formamides were readily hydrogenated to methanol with the same catalyst.Consequently,an amine-assisted direct hydrogenation system of CO_(2)to methanol was established by POMPs with higher activity and TON(1.46×10^(4))than their molecular precursors,shedding light on the direct valorization of CO_(2)and carbon neutral recycling.展开更多
基金Financial support from the National Natural Science Foundation of China(grant nos.21871059 and 21861132002)the National Key R&D Program of China(grant no.2016YFA0202902)Department of Chemistry,Fudan University are gratefully acknowledged.
文摘Considering the importance of the valorization of CO_(2),a number of phosphine-containing ruthenium pincer complexes have been successfully heterogenized using a“direct knitting”strategy without any premodification.The resulting porous organometallic polymers(POMPs)with high specific-surface areas,hierarchical pores,and uniformly dispersed Ru single-sites exhibited outstanding catalytic activity toward the N-formylation of diverse amines with CO_(2).Besides excellent turnover number(TON,5×10^(5))and turnover frequency(TOF,5592 h-1),the obtained formamides were readily hydrogenated to methanol with the same catalyst.Consequently,an amine-assisted direct hydrogenation system of CO_(2)to methanol was established by POMPs with higher activity and TON(1.46×10^(4))than their molecular precursors,shedding light on the direct valorization of CO_(2)and carbon neutral recycling.