Ordered porous solid strong bases(OPSSBs)have attracted great research interest due to the excellent performance as heterogeneous catalysts in various reactions.The main obstacle for fabricating OPSSBs is the requirem...Ordered porous solid strong bases(OPSSBs)have attracted great research interest due to the excellent performance as heterogeneous catalysts in various reactions.The main obstacle for fabricating OPSSBs is the requirement of high temperature to produce strong basicity on ordered porous materials.For example,the temperatures of 600-650℃ are required for the decomposition of base precursor NaNO_(3)to basic sites on mesoporous silica SBA-15 and zeolite Y.Such high decomposition temperatures are energy-intensive and harmful to the structure of supports.Herein,we report the fabrication of OPSSBs by utilizing the redox interaction between base precursor and low-valence metal centers(e.g.,Cr^(3+))in metal-organic frameworks(MOFs).The base precursor NaNO_(3)on MIL-101(Cr)can be converted to basic sites entirely at 300℃,which is quite lower than those of the conventional thermal conversion on SBA-15 and zeolite Y(600-650℃).The exploration on decomposition mechanism reveals that the valence change of Cr^(3+)to Cr^(6+)takes place during the conversion of NaNO_(3)to basic sites.In this way,MOFs-derived base catalysts have been synthesized successfully by the host-guest redox strategy and exhibit high catalytic activity in typical base-catalyzed reactions.展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.21878149,22078155 and 21722606)National Science Fund for Distinguished Young Scholars(No.22125804)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Ordered porous solid strong bases(OPSSBs)have attracted great research interest due to the excellent performance as heterogeneous catalysts in various reactions.The main obstacle for fabricating OPSSBs is the requirement of high temperature to produce strong basicity on ordered porous materials.For example,the temperatures of 600-650℃ are required for the decomposition of base precursor NaNO_(3)to basic sites on mesoporous silica SBA-15 and zeolite Y.Such high decomposition temperatures are energy-intensive and harmful to the structure of supports.Herein,we report the fabrication of OPSSBs by utilizing the redox interaction between base precursor and low-valence metal centers(e.g.,Cr^(3+))in metal-organic frameworks(MOFs).The base precursor NaNO_(3)on MIL-101(Cr)can be converted to basic sites entirely at 300℃,which is quite lower than those of the conventional thermal conversion on SBA-15 and zeolite Y(600-650℃).The exploration on decomposition mechanism reveals that the valence change of Cr^(3+)to Cr^(6+)takes place during the conversion of NaNO_(3)to basic sites.In this way,MOFs-derived base catalysts have been synthesized successfully by the host-guest redox strategy and exhibit high catalytic activity in typical base-catalyzed reactions.
