The palladium(Pd)-catalyzed Suzuki reaction is widely applied in the pharmaceutical industry,where constructing highly active and low-cost Pd sites are impendent.Here,we report the fabrication of a heterogeneous Pd/Ti...The palladium(Pd)-catalyzed Suzuki reaction is widely applied in the pharmaceutical industry,where constructing highly active and low-cost Pd sites are impendent.Here,we report the fabrication of a heterogeneous Pd/Tio2 catalyst via engineering of an electronic structure of a single Pd_(1)atom on monolayered Ti_(0.87)O_(2)nanosheet(Pd_(1)-Ti_(0.87)O_(2)).This catalyst motivated the kinetically sluggish C-Br cleavage,thus boosting the Suzuki reaction at room temperature.Pd_(1)-Ti_(0.87)O_(2)exhibited an outstanding activity with turnover frequency(TOF)of 11,110 h-1,exceeding that of PdCl_(2)and Pd(OAc)_(2)catalysts by a factor of>200.Various in situ techniques were employed to investigate the C-Br activation process,which showed that Pd_(1)kinetic-feasibly dissociated the chemisorbed bromobenzene,especially the C-Br bond cleavage.Theoretical calculations further revealed that the improved activity is ascribed to the optimized charge state of Pd_(1)within the Pd_(1)O4 realm via charge transfer.展开更多
The dielectric capacitor has been widely used in advanced electronic and electrical power systems due to its capability of ultrafast charging–discharging and ultrahigh power density.Nevertheless,its energy density is...The dielectric capacitor has been widely used in advanced electronic and electrical power systems due to its capability of ultrafast charging–discharging and ultrahigh power density.Nevertheless,its energy density is still limited by the low dielectric constant(≈2.2)of the commercial dielectric polypropylene(PP).The conventional enhancement strategy by embedding inorganic fillers in PP matrix is still difficult and challenging due to that PP hardly dissolves in any inorganic/organic solvent.In this work,we develop a new strategy including freeze-drying,surface functionalization,and hot-pressing to incorporate Ti_(0.87)O_(2) monolayers in PP film.A series of uniform composited Ti_(0.87)O_(2)@PP film has been successfully fabricated with Ti0.87O2 content range of 0–15 wt%.The maximum dielectric constant of the as-prepared Ti_(0.87)O_(2)@PP film is 3.27 when the Ti_(0.87)O_(2) content is 9 wt%,which is about 1.5 times higher than that of pure PP.Our study provides a feasible strategy to embed two-dimensional material into commercial PP thin-film with superior dielectric performance for practical application.展开更多
基金This study was supported financially by the National Natural Science Foundation of China(grant nos.91961125,21905019,and 21903001)the Fundamental Research Funds for the Central Universities(grant nos.2018JBZ107 and 2019RC035)+2 种基金the Ministry of Science and Technology of China(grant no.2018YFE0124600)the Chemistry and Chemical Engineering Guangdong Laboratory(grant no.1932004)the Natural Science Foundation of Anhui Province(grant no.1908085QB58)。
文摘The palladium(Pd)-catalyzed Suzuki reaction is widely applied in the pharmaceutical industry,where constructing highly active and low-cost Pd sites are impendent.Here,we report the fabrication of a heterogeneous Pd/Tio2 catalyst via engineering of an electronic structure of a single Pd_(1)atom on monolayered Ti_(0.87)O_(2)nanosheet(Pd_(1)-Ti_(0.87)O_(2)).This catalyst motivated the kinetically sluggish C-Br cleavage,thus boosting the Suzuki reaction at room temperature.Pd_(1)-Ti_(0.87)O_(2)exhibited an outstanding activity with turnover frequency(TOF)of 11,110 h-1,exceeding that of PdCl_(2)and Pd(OAc)_(2)catalysts by a factor of>200.Various in situ techniques were employed to investigate the C-Br activation process,which showed that Pd_(1)kinetic-feasibly dissociated the chemisorbed bromobenzene,especially the C-Br bond cleavage.Theoretical calculations further revealed that the improved activity is ascribed to the optimized charge state of Pd_(1)within the Pd_(1)O4 realm via charge transfer.
基金financially supported by the Researching Program of State Grid Corporation of China(GYW17201800011):Research and Application of Key Technologies to Improve the Performance of Film Insulator for High Voltage Capacitive Equipment。
文摘The dielectric capacitor has been widely used in advanced electronic and electrical power systems due to its capability of ultrafast charging–discharging and ultrahigh power density.Nevertheless,its energy density is still limited by the low dielectric constant(≈2.2)of the commercial dielectric polypropylene(PP).The conventional enhancement strategy by embedding inorganic fillers in PP matrix is still difficult and challenging due to that PP hardly dissolves in any inorganic/organic solvent.In this work,we develop a new strategy including freeze-drying,surface functionalization,and hot-pressing to incorporate Ti_(0.87)O_(2) monolayers in PP film.A series of uniform composited Ti_(0.87)O_(2)@PP film has been successfully fabricated with Ti0.87O2 content range of 0–15 wt%.The maximum dielectric constant of the as-prepared Ti_(0.87)O_(2)@PP film is 3.27 when the Ti_(0.87)O_(2) content is 9 wt%,which is about 1.5 times higher than that of pure PP.Our study provides a feasible strategy to embed two-dimensional material into commercial PP thin-film with superior dielectric performance for practical application.
