Single-crystal-like TiO2 mesoporous microspheres have been reported with high photocatalytic activity under ultraviolet light (UV light) because of their high specific surface areas and single-crystal-like channel w...Single-crystal-like TiO2 mesoporous microspheres have been reported with high photocatalytic activity under ultraviolet light (UV light) because of their high specific surface areas and single-crystal-like channel walls. In this work, plasmonic gold nanoparticles (Au NPs) and fl-NaYF4: Yb3+, Er3+ upconversion nanoparticles (UCNPs) were composited with single-crystal-like TiO2 mesoporous microspheres through a series of facile approaches, aiming at broadening response region of solar light from UV to visible and near infrared light and enhancing the photocata- lyric activity further. The structure was rationally designed by modifying the pore size of TiO2 mesoporous micro- spheres so as to anchor plasmonic Au NPs, and covering β-NaYF4: Yb3+, Er3+ with SiO2 in order to embed UCNPs into TiO2 mesoporous microspheres via hydrophilic interaction. This work studied the attribution of Au NPs and UCNPs to photocatalysis and found out that combining Au NPs and certain amount of UCNPs with single-crystal- like TiO2 mesoporous microspheres in a monolithic architecture would bring enhanced broadband photocatalytic activity under simulated solar light. Consequently, the composite photocatalyts containing 150 mg UCNPs showed a significant enhancement in reaction rate, which was 36.02% higher than commercial P25 and 85.09% higher than pure TiO2 mesoporous microspheres under simulated solar light.展开更多
Mesoporous TiO2microsphere(MTM)was synthesized via a simple solution route and then mixed with commercial TiO2(P25)to form highly homogeneous and stable TiO2colloid by simple hydrothermal treatment.The TiO2colloid was...Mesoporous TiO2microsphere(MTM)was synthesized via a simple solution route and then mixed with commercial TiO2(P25)to form highly homogeneous and stable TiO2colloid by simple hydrothermal treatment.The TiO2colloid was coated onto the plastic conductive substrate to prepare mesoporous TiO2film for flexible dye-sensitized solar cells(DSSCs)by low-temperature heat treatment.The influence of MTM content on the physicochemical properties of the flexible TiO2film was characterized by scanning electron microscope,transmission electron microscopy,X-ray diffraction,energy-dispersive X-ray spectrometer,N2adsorption-desorption isotherms,UV–vis absorption and diffuse reflectance spectra.It is revealed that with increasing the MTM content,the dye-loading capability of TiO2film and light-harvesting efficiency of flexible DSSCs are improved due to MTM having high surface area and acting as a light scattering center,respectively,resulting in the enhancement of photocurrent of flexible DSSCs.However,more and larger cracks having negative effect on the performances of flexible DSSCs are formed simultaneously.Under the optimal condition with MTM content of 20%,a flexible DSSC with overall light-to-electric energy conversion efficiency of 2.74%is achieved under a simulated solar light irradiation of 100 mW cm 2(AM 1.5),with 26%improvement in comparison with DSSCs based on P25 alone.展开更多
基金This work is supported by the National Natural Science Foundation of China (Nos. 21236003, 21322607, 21406072, 21471056, 21676093 and 91534202), Shanghai Educational Development Foundation (No. 14CG29), the Basic Research Program of Shanghai (No. 14JCI406402), China Postdoctoral Science Foundation (Nos. 2014M560307, 2014M561497, 2015T80408), and the Fundamental Research Funds for the Central Universities.
文摘Single-crystal-like TiO2 mesoporous microspheres have been reported with high photocatalytic activity under ultraviolet light (UV light) because of their high specific surface areas and single-crystal-like channel walls. In this work, plasmonic gold nanoparticles (Au NPs) and fl-NaYF4: Yb3+, Er3+ upconversion nanoparticles (UCNPs) were composited with single-crystal-like TiO2 mesoporous microspheres through a series of facile approaches, aiming at broadening response region of solar light from UV to visible and near infrared light and enhancing the photocata- lyric activity further. The structure was rationally designed by modifying the pore size of TiO2 mesoporous micro- spheres so as to anchor plasmonic Au NPs, and covering β-NaYF4: Yb3+, Er3+ with SiO2 in order to embed UCNPs into TiO2 mesoporous microspheres via hydrophilic interaction. This work studied the attribution of Au NPs and UCNPs to photocatalysis and found out that combining Au NPs and certain amount of UCNPs with single-crystal- like TiO2 mesoporous microspheres in a monolithic architecture would bring enhanced broadband photocatalytic activity under simulated solar light. Consequently, the composite photocatalyts containing 150 mg UCNPs showed a significant enhancement in reaction rate, which was 36.02% higher than commercial P25 and 85.09% higher than pure TiO2 mesoporous microspheres under simulated solar light.
基金supported financially by the National High Technology Research and Development Program of China(2009AA03Z217)the National Natural Science Foundation of China(90922028)+1 种基金the Key Project of Chinese Ministry of Education(211204)the Fund of Fujian Provincial Key Laboratory of Nanomaterials(NM10-5)
文摘Mesoporous TiO2microsphere(MTM)was synthesized via a simple solution route and then mixed with commercial TiO2(P25)to form highly homogeneous and stable TiO2colloid by simple hydrothermal treatment.The TiO2colloid was coated onto the plastic conductive substrate to prepare mesoporous TiO2film for flexible dye-sensitized solar cells(DSSCs)by low-temperature heat treatment.The influence of MTM content on the physicochemical properties of the flexible TiO2film was characterized by scanning electron microscope,transmission electron microscopy,X-ray diffraction,energy-dispersive X-ray spectrometer,N2adsorption-desorption isotherms,UV–vis absorption and diffuse reflectance spectra.It is revealed that with increasing the MTM content,the dye-loading capability of TiO2film and light-harvesting efficiency of flexible DSSCs are improved due to MTM having high surface area and acting as a light scattering center,respectively,resulting in the enhancement of photocurrent of flexible DSSCs.However,more and larger cracks having negative effect on the performances of flexible DSSCs are formed simultaneously.Under the optimal condition with MTM content of 20%,a flexible DSSC with overall light-to-electric energy conversion efficiency of 2.74%is achieved under a simulated solar light irradiation of 100 mW cm 2(AM 1.5),with 26%improvement in comparison with DSSCs based on P25 alone.