In this work, we designed and synthesized cationic carbon dots(CDs) with a size distribution of 1.6–3.7 nm, which exhibited dark blue fluorescence in the aqueous solution. Based on its excellent luminescence properti...In this work, we designed and synthesized cationic carbon dots(CDs) with a size distribution of 1.6–3.7 nm, which exhibited dark blue fluorescence in the aqueous solution. Based on its excellent luminescence properties, we used it as an energy donor to construct a sequential artificial light-harvesting system(LHS) by employing the energy-matching dyes eosin Y disodium salt(EY) and sulforhodamine101(SR101), which could regulate the white light emission(Commission Internationale de l'Eclairage(CIE) coordinate:(0.30, 0.31)) with the energy transfer efficiency(ΦET) of 53.9% and 20.0%. Moreover, a single-step artificial LHS with white light emission(0.32, 0.28) can be constructed directly using CDs and dye solvent 43(SR) with ΦETand antenna effect(AE) of 48.8% and 6.5, respectively. More importantly,CDs-based artificial LHSs were firstly used in photocatalytic of α-bromoacetophenone, with a yield of90%. This work not only provides a new strategy for constructing CDs-based LHSs, but also opens up a new application for further applying the energy harvested in CDs-based LHSs to the field of the aqueous solution photocatalysis.展开更多
In this work,we have designed and synthesized a cyano-substituted p-phenylenevinylene derivative(PPTA),which can self-assemble into positively charged nanoparticles in an aqueous solution with a deep green fluorescenc...In this work,we have designed and synthesized a cyano-substituted p-phenylenevinylene derivative(PPTA),which can self-assemble into positively charged nanoparticles in an aqueous solution with a deep green fluorescence.An anionic polyelectrolyte material guar gum modified by carboxylic acid(GP5A)was chosen to build an artificial light-harvesting system(LHS)through self-assembly with PPTA,in which two acceptors Eosin Y(EY)and Nile red(NiR)were loaded into the PPTA-GP5A assemblies through electrostatic interaction and Van der Waals force.By adjusting the molar ratio of PPTA-GP5A/EY at 1:0.004,the one-step artificial LHS can exhibit high energy transfer efficiency(Φ_(ET))(38.9%)and antenna effect(AE)(4.6).Subsequently,with the addition of NiR,theΦET and AE of the two-step sequential artificial LHS were calculated to be 71.9%and 13.5,respectively.Moreover,the two-step artificial LHS constructed by the polyelectrolyte material GP5A can be used as a nanoreactor to photocatalyst alkylation of C-H bonds of phenyl vinyl sulfone(PVS)and tetrahydrofuran(THF)in water with a yield of 42%.Therefore,we have constructed an artificial LHS with two-step energy transfer based on polyelectrolytes through the electrostatic interaction to improve energy transfer efficiency,which can also be used as a nanoreactor for photocatalysis.展开更多
基金the financial support from the National Natural Science Foundation of China (Nos.52205210 and 22002075)the Natural Science Foundation of Shandong Province (Nos.ZR2020MB018 and ZR2022QE033)。
文摘In this work, we designed and synthesized cationic carbon dots(CDs) with a size distribution of 1.6–3.7 nm, which exhibited dark blue fluorescence in the aqueous solution. Based on its excellent luminescence properties, we used it as an energy donor to construct a sequential artificial light-harvesting system(LHS) by employing the energy-matching dyes eosin Y disodium salt(EY) and sulforhodamine101(SR101), which could regulate the white light emission(Commission Internationale de l'Eclairage(CIE) coordinate:(0.30, 0.31)) with the energy transfer efficiency(ΦET) of 53.9% and 20.0%. Moreover, a single-step artificial LHS with white light emission(0.32, 0.28) can be constructed directly using CDs and dye solvent 43(SR) with ΦETand antenna effect(AE) of 48.8% and 6.5, respectively. More importantly,CDs-based artificial LHSs were firstly used in photocatalytic of α-bromoacetophenone, with a yield of90%. This work not only provides a new strategy for constructing CDs-based LHSs, but also opens up a new application for further applying the energy harvested in CDs-based LHSs to the field of the aqueous solution photocatalysis.
基金We are grateful for the financial support from the National Natural Science Foundation of China(Nos.52205210 and 22005179)the Natural Science Foundation of Shandong Province(Nos.ZR2020MB018,ZR2022QE033,ZR2020QB113 and ZR2018BEE015).
文摘In this work,we have designed and synthesized a cyano-substituted p-phenylenevinylene derivative(PPTA),which can self-assemble into positively charged nanoparticles in an aqueous solution with a deep green fluorescence.An anionic polyelectrolyte material guar gum modified by carboxylic acid(GP5A)was chosen to build an artificial light-harvesting system(LHS)through self-assembly with PPTA,in which two acceptors Eosin Y(EY)and Nile red(NiR)were loaded into the PPTA-GP5A assemblies through electrostatic interaction and Van der Waals force.By adjusting the molar ratio of PPTA-GP5A/EY at 1:0.004,the one-step artificial LHS can exhibit high energy transfer efficiency(Φ_(ET))(38.9%)and antenna effect(AE)(4.6).Subsequently,with the addition of NiR,theΦET and AE of the two-step sequential artificial LHS were calculated to be 71.9%and 13.5,respectively.Moreover,the two-step artificial LHS constructed by the polyelectrolyte material GP5A can be used as a nanoreactor to photocatalyst alkylation of C-H bonds of phenyl vinyl sulfone(PVS)and tetrahydrofuran(THF)in water with a yield of 42%.Therefore,we have constructed an artificial LHS with two-step energy transfer based on polyelectrolytes through the electrostatic interaction to improve energy transfer efficiency,which can also be used as a nanoreactor for photocatalysis.