Photothermal catalysis represents a promising strategy to utilize the renewable energy source(e.g.,solar energy)to drive chemical reactions more efficiently.Successful and efficient photothermal catalysis relies on th...Photothermal catalysis represents a promising strategy to utilize the renewable energy source(e.g.,solar energy)to drive chemical reactions more efficiently.Successful and efficient photothermal catalysis relies on the availability of ideal photothermal catalysts,which can provide both large areas of catalytically active surface and strong light absorption power simultaneously.Such duplex requirements of a photothermal catalyst exhibit opposing dependence on the size of the catalyst nanoparticles,i.e.,smaller size is beneficial for achieving higher surface area and more active surface,whereas larger size favors the light absorption in the nanoparticles.In this article,we report the synthesis of ultrafine RuOOH nanoparticles with a size of 2–3 nm uniformly dispersed on the surfaces of silica(SiOx)nanospheres of hundreds of nanometers in size to tackle this challenge of forming an ideal photothermal catalyst.The ultrasmall RuOOH nanoparticles exhibit a large surface area as well as the ability to activate adsorbed molecular oxygen.The SiOx nanospheres exhibit strong surface light scattering resonances to enhance the light absorption power of the small RuOOH nanoparticles anchored on the SiOx surface.Therefore,the RuOOH/SiOx composite particles represent a new class of efficient photothermal catalysts with a photothermal energy conversion efficiency of 92.5%for selective aerobic oxidation of benzyl alcohol to benzylaldehyde under ambient conditions.展开更多
Benefiting from their unique delocalized electronic structure, conjugated polymer-based semiconductors are widely applied in the fields of organic electronics, sensors, and biomedical applications. However, the photoc...Benefiting from their unique delocalized electronic structure, conjugated polymer-based semiconductors are widely applied in the fields of organic electronics, sensors, and biomedical applications. However, the photocatalytic properties of conjugated polymers have been seldom studied because of their unsuitable band structures. Herein, we creatively demonstrate that the band structures of conjugated polymers are strongly related to their degree of polymerization （DP）, offering an effective strategy for the design of metal-free photocatalysts with tunable light absorption properties. Taking poly（3- hexylthiophene） （PHT） as an example, we show that PHT nanofibers with a suitable DP are a novel visible light-driven photocatalyst, which can readily convert molecular oxygen into superoxide ions. Benefiting from the high selectivity of the generated superoxides, the PHT nanofibers display outstanding activity for the aerobic oxidation of amines into imines with nearly 100% conversion and selectivity. This study offers a new strategy for the design of advanced coniugated Dolvrner-based Dhotocatalvsts.展开更多
基金supported by the start-up from Temple University
文摘Photothermal catalysis represents a promising strategy to utilize the renewable energy source(e.g.,solar energy)to drive chemical reactions more efficiently.Successful and efficient photothermal catalysis relies on the availability of ideal photothermal catalysts,which can provide both large areas of catalytically active surface and strong light absorption power simultaneously.Such duplex requirements of a photothermal catalyst exhibit opposing dependence on the size of the catalyst nanoparticles,i.e.,smaller size is beneficial for achieving higher surface area and more active surface,whereas larger size favors the light absorption in the nanoparticles.In this article,we report the synthesis of ultrafine RuOOH nanoparticles with a size of 2–3 nm uniformly dispersed on the surfaces of silica(SiOx)nanospheres of hundreds of nanometers in size to tackle this challenge of forming an ideal photothermal catalyst.The ultrasmall RuOOH nanoparticles exhibit a large surface area as well as the ability to activate adsorbed molecular oxygen.The SiOx nanospheres exhibit strong surface light scattering resonances to enhance the light absorption power of the small RuOOH nanoparticles anchored on the SiOx surface.Therefore,the RuOOH/SiOx composite particles represent a new class of efficient photothermal catalysts with a photothermal energy conversion efficiency of 92.5%for selective aerobic oxidation of benzyl alcohol to benzylaldehyde under ambient conditions.
文摘Benefiting from their unique delocalized electronic structure, conjugated polymer-based semiconductors are widely applied in the fields of organic electronics, sensors, and biomedical applications. However, the photocatalytic properties of conjugated polymers have been seldom studied because of their unsuitable band structures. Herein, we creatively demonstrate that the band structures of conjugated polymers are strongly related to their degree of polymerization （DP）, offering an effective strategy for the design of metal-free photocatalysts with tunable light absorption properties. Taking poly（3- hexylthiophene） （PHT） as an example, we show that PHT nanofibers with a suitable DP are a novel visible light-driven photocatalyst, which can readily convert molecular oxygen into superoxide ions. Benefiting from the high selectivity of the generated superoxides, the PHT nanofibers display outstanding activity for the aerobic oxidation of amines into imines with nearly 100% conversion and selectivity. This study offers a new strategy for the design of advanced coniugated Dolvrner-based Dhotocatalvsts.
