The growth and thermal stability of Au clusters on a partially-reduced rutile TiO2 (110)-1 × 1 surface were investigated by high-resolution photoelectron spectroscopy using synchrotron- radiation-light. The val...The growth and thermal stability of Au clusters on a partially-reduced rutile TiO2 (110)-1 × 1 surface were investigated by high-resolution photoelectron spectroscopy using synchrotron- radiation-light. The valence-band photoelectron spectroscopy results demonstrate that the Ti^3+3d feature attenuates quickly with the initial deposition of Au clusters, implying that Au clusters nucleate at the oxygen vacancy sites. The Au4f core-level photoelectron spectroscopy results directly prove the existence of charge transfer from oxygen vacancies to Au clusters. The thermal stability of Au clusters on the partially-reduced and stoichiometric TiO2(110) surfaces was also comparatively investigated by the annealing experiments. With the same film thickness, Au clusters are more thermally stable on the partially-reduced TiO2(110) surface than on the stoichiometric TiO2(110) surface. Meanwhile, large Au nanoparticles are more thermally stable than fine Au nanoparticles.展开更多
Sonophotocatalysis combines ultrasonic and light irradiations to drastically boost the chemical reaction rate and has attracted many interests for its potential applications in the environmental remediation and protec...Sonophotocatalysis combines ultrasonic and light irradiations to drastically boost the chemical reaction rate and has attracted many interests for its potential applications in the environmental remediation and protection. However, it still remains unclear whether the light irradiation could couple with the ultrasound to prompt the sonophotocatalytic process. Here, we selectively excited the TiO2 and Au to manipulate the electronic structures of Au/TiO2 and studied their influence in sonophotocatalytic water(H2 O) reduction. Surprisingly, no significant increase of the hydrogen(H2) production rate was observed under either the UV light irradiation or the visible light irradiation, suggesting that the change in electronic structures of Au/TiO2 does not prompt the generation of free radicals under sonication and the reaction is dominated by the recovery of active sites through ultrasound. Our findings established an indepth understanding of the origin of the enhanced catalytic activity in sonophotocatalysis.展开更多
TiO2 nanotubes were prepared under normal pressure at a temperature of 120 ℃. Ag, Au, Pt nanoparticles supported on TiO2 nanotubes were prepared by m icrowave assisted heating polyol process. TEM images showed that m...TiO2 nanotubes were prepared under normal pressure at a temperature of 120 ℃. Ag, Au, Pt nanoparticles supported on TiO2 nanotubes were prepared by m icrowave assisted heating polyol process. TEM images showed that microwave prepa red Ag, Au, Pt nanoparticles supported on TiO2 nanotubes were small and well dis persed on the surface of the TiO2 nanotubes. UV-Vis absorption spectra showed th at the absorbance of Ag/TiO2 nanotubes and Au/TiO2 nanotubes in the visible ligh t range increased greatly compared to the single titania nanotubes.展开更多
Due to increasingly serious environmental problems,many researchers are investigating green cleanenergy to solve the world’s energy supply issues.So the strategy that Au nanoparticles(Au NPs)and bismuth sulfide(Bi2S3...Due to increasingly serious environmental problems,many researchers are investigating green cleanenergy to solve the world’s energy supply issues.So the strategy that Au nanoparticles(Au NPs)and bismuth sulfide(Bi2S3)NPs are used to evenly decorate TiO2 nanotube arrays(TiO2 NTAs)was carried out.Composite materials demonstrated enhanced solar light absorption ability and excellent photoelectrochemical performance.This was attributed to the presence of Bi2S3 NPs with a narrow band gap and the decoration with noble metallic Au NPs which resulted in local surface plasmon resonance(LSPR)effects.The Au/Bi2S3@TiO2 NTAs composites exhibit improved photocatalytic activity for the degradation of methylene blue(MB)under irradiation of UV and visible light.Moreover,the Au/Bi2S3@TiO2 NTAs exhibits high fluorescence emission at 822 nm.Due to the better binding affinity between Bi2S3,TiO2 and Fe3+ions,the synthesized nanocomposites exhibit high selectivity to Fe3+ions.The number of binding sites for Au/Bi2S3@TiO2 NTAs was estimated to be 1.41 according to the double logarithmic regression method.The calculated value of"K"was 1862 M-1.Fluorescence emission intensity decreases with increasing concentration(30μM–5000μM).The detection limit of the synthesized sensor is 0.221μM.展开更多
Cold plasma generated by dielectric barrier discharge (DBD) at atmospheric pressure was adopted for preparation of commercial TiO2 Degussa P25 supported Au catalysts (Au/P25- P) with the assistance of the depositi...Cold plasma generated by dielectric barrier discharge (DBD) at atmospheric pressure was adopted for preparation of commercial TiO2 Degussa P25 supported Au catalysts (Au/P25- P) with the assistance of the deposition-precipitation procedure. The influences of the plasma reduction time and calcination on the performance of the Au/P25-P catalysts were investigated. CO oxidation was performed to investigate the catalytic activity of the Au/P25 catalysts. The results show that DBD cold plasma for the fabrication of Au/P25-P catalysts is a fast process, and Au/P25-P (4 min) exhibited the highest CO oxidation activity due to the complete reduction of Au compounds and less consumption of oxygen vacancies. In order to form more oxygen vacancies active species, Au/P25-P was calcined to obtain Au/P25-PC catalysts. Interestingly, Au/P25- PC exhibited the highest activity for CO oxidation among the Au/P25 samples. The results of transmission electron microscopy (TEM) indicated that the smaller size and high distribution of Au nanoparticles are the mean reasons for a high performance of Au/P25-PC. Atmospheric- pressure DBD cold plasma was proved to be of great efficiency in preparing high performance supported Au catalysts.展开更多
Anatase TiO2 nanocrystals and sub-microcrystals with truncated octahedral bipyramidal morphologies were prepared by direct calcination of TiOF2 precursors. The as-prepared TiO2 samples were thoroughly characterized by...Anatase TiO2 nanocrystals and sub-microcrystals with truncated octahedral bipyramidal morphologies were prepared by direct calcination of TiOF2 precursors. The as-prepared TiO2 samples were thoroughly characterized by X-ray diffraction, Raman spectroscopy, field-emission scanning electron microscopy, N2 adsorption-desorption isotherms, X-ray photoelectron spectroscopy, and UV-visible diffuse spectroscopy. It was found that the crystallinity, grain size, and {001}/{101} ratio of the samples can be increased by raising the calcination temperature from 500 to 800℃. The higher crystallinity and {001}/{101} facet ratio resulted in an increase in both aqueous and gas-phase photocatalytic activities, by inhibiting the recombination and separation of electrons and holes. After selecting two TiO2 samples with high crystallinity and {001}/{101} ratio, Au nanoparticles were decorated on their surfaces, and the photocatalytic activity of the resulting samples under visible light illumination was studied. It was found that the visible light-induced photocatalytic activity increased by 2.6 and 4.8 times, respectively, upon Au decoration of the samples prepared by calcination of TiOF2 at 700 and 800℃.展开更多
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China (No.20773113 and No.20803072), the Hundred Talent Program of Chinese Academy of Sciences, the MOE Program for Changjiang Scholars and Innovative Research Team (No.IRT0756), and the MPG-CAS Partner-group Program.
摘要The growth and thermal stability of Au clusters on a partially-reduced rutile TiO2 (110)-1 × 1 surface were investigated by high-resolution photoelectron spectroscopy using synchrotron- radiation-light. The valence-band photoelectron spectroscopy results demonstrate that the Ti^3+3d feature attenuates quickly with the initial deposition of Au clusters, implying that Au clusters nucleate at the oxygen vacancy sites. The Au4f core-level photoelectron spectroscopy results directly prove the existence of charge transfer from oxygen vacancies to Au clusters. The thermal stability of Au clusters on the partially-reduced and stoichiometric TiO2(110) surfaces was also comparatively investigated by the annealing experiments. With the same film thickness, Au clusters are more thermally stable on the partially-reduced TiO2(110) surface than on the stoichiometric TiO2(110) surface. Meanwhile, large Au nanoparticles are more thermally stable than fine Au nanoparticles.
基金supported by the National Science Foundation 9(NSF, No. DMR-1352328)supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, under Contract No. DE-SC0012704
摘要Sonophotocatalysis combines ultrasonic and light irradiations to drastically boost the chemical reaction rate and has attracted many interests for its potential applications in the environmental remediation and protection. However, it still remains unclear whether the light irradiation could couple with the ultrasound to prompt the sonophotocatalytic process. Here, we selectively excited the TiO2 and Au to manipulate the electronic structures of Au/TiO2 and studied their influence in sonophotocatalytic water(H2 O) reduction. Surprisingly, no significant increase of the hydrogen(H2) production rate was observed under either the UV light irradiation or the visible light irradiation, suggesting that the change in electronic structures of Au/TiO2 does not prompt the generation of free radicals under sonication and the reaction is dominated by the recovery of active sites through ultrasound. Our findings established an indepth understanding of the origin of the enhanced catalytic activity in sonophotocatalysis.
摘要TiO2 nanotubes were prepared under normal pressure at a temperature of 120 ℃. Ag, Au, Pt nanoparticles supported on TiO2 nanotubes were prepared by m icrowave assisted heating polyol process. TEM images showed that microwave prepa red Ag, Au, Pt nanoparticles supported on TiO2 nanotubes were small and well dis persed on the surface of the TiO2 nanotubes. UV-Vis absorption spectra showed th at the absorbance of Ag/TiO2 nanotubes and Au/TiO2 nanotubes in the visible ligh t range increased greatly compared to the single titania nanotubes.
基金supported by the National Natural Science Foundation of China(Nos.51972063 and 21501127)the 111 Project(No.D17005)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
摘要Due to increasingly serious environmental problems,many researchers are investigating green cleanenergy to solve the world’s energy supply issues.So the strategy that Au nanoparticles(Au NPs)and bismuth sulfide(Bi2S3)NPs are used to evenly decorate TiO2 nanotube arrays(TiO2 NTAs)was carried out.Composite materials demonstrated enhanced solar light absorption ability and excellent photoelectrochemical performance.This was attributed to the presence of Bi2S3 NPs with a narrow band gap and the decoration with noble metallic Au NPs which resulted in local surface plasmon resonance(LSPR)effects.The Au/Bi2S3@TiO2 NTAs composites exhibit improved photocatalytic activity for the degradation of methylene blue(MB)under irradiation of UV and visible light.Moreover,the Au/Bi2S3@TiO2 NTAs exhibits high fluorescence emission at 822 nm.Due to the better binding affinity between Bi2S3,TiO2 and Fe3+ions,the synthesized nanocomposites exhibit high selectivity to Fe3+ions.The number of binding sites for Au/Bi2S3@TiO2 NTAs was estimated to be 1.41 according to the double logarithmic regression method.The calculated value of"K"was 1862 M-1.Fluorescence emission intensity decreases with increasing concentration(30μM–5000μM).The detection limit of the synthesized sensor is 0.221μM.
基金supported by National Natural Science Foundation of China(Nos.11505019,21173028)the Science and Technology Research Project of Liaoning Provincial Education Department(No.L2013464)+1 种基金the Scientific Research Foundation for the Doctor of Liaoning Province(No.20131004)the Dalian Jinzhou New District Science and Technology Plan Project(No.KJCX-ZTPY-2014-0001)
摘要Cold plasma generated by dielectric barrier discharge (DBD) at atmospheric pressure was adopted for preparation of commercial TiO2 Degussa P25 supported Au catalysts (Au/P25- P) with the assistance of the deposition-precipitation procedure. The influences of the plasma reduction time and calcination on the performance of the Au/P25-P catalysts were investigated. CO oxidation was performed to investigate the catalytic activity of the Au/P25 catalysts. The results show that DBD cold plasma for the fabrication of Au/P25-P catalysts is a fast process, and Au/P25-P (4 min) exhibited the highest CO oxidation activity due to the complete reduction of Au compounds and less consumption of oxygen vacancies. In order to form more oxygen vacancies active species, Au/P25-P was calcined to obtain Au/P25-PC catalysts. Interestingly, Au/P25- PC exhibited the highest activity for CO oxidation among the Au/P25 samples. The results of transmission electron microscopy (TEM) indicated that the smaller size and high distribution of Au nanoparticles are the mean reasons for a high performance of Au/P25-PC. Atmospheric- pressure DBD cold plasma was proved to be of great efficiency in preparing high performance supported Au catalysts.
基金supported by the National Natural Science Foundation of China(51772230,51461135004)the Hubei Foreign Science and Technology Cooperation Project(2017AHB059)the Japan Society for the Promotion of Science(JSPS)for an Invitational Fellowship for Foreign Researchers(L16531)~~
摘要Anatase TiO2 nanocrystals and sub-microcrystals with truncated octahedral bipyramidal morphologies were prepared by direct calcination of TiOF2 precursors. The as-prepared TiO2 samples were thoroughly characterized by X-ray diffraction, Raman spectroscopy, field-emission scanning electron microscopy, N2 adsorption-desorption isotherms, X-ray photoelectron spectroscopy, and UV-visible diffuse spectroscopy. It was found that the crystallinity, grain size, and {001}/{101} ratio of the samples can be increased by raising the calcination temperature from 500 to 800℃. The higher crystallinity and {001}/{101} facet ratio resulted in an increase in both aqueous and gas-phase photocatalytic activities, by inhibiting the recombination and separation of electrons and holes. After selecting two TiO2 samples with high crystallinity and {001}/{101} ratio, Au nanoparticles were decorated on their surfaces, and the photocatalytic activity of the resulting samples under visible light illumination was studied. It was found that the visible light-induced photocatalytic activity increased by 2.6 and 4.8 times, respectively, upon Au decoration of the samples prepared by calcination of TiOF2 at 700 and 800℃.