Photocatalyst was prepared by immobilizing TiO2 on glass beads using the traditional sol-gel method. Ultraviolet light （UV） produced by pulsed streamer discharge was then used to induce photocatalytic activity of Ti...Photocatalyst was prepared by immobilizing TiO2 on glass beads using the traditional sol-gel method. Ultraviolet light （UV） produced by pulsed streamer discharge was then used to induce photocatalytic activity of TiO2 photocatalyst. Decolouration efficiency of the representative azo dye （acid orange 7, AOT） was investigated using the synergistic system of pulsed streamer discharge plasma and TiO2 photocatalysis. The obtained results showed that the decolouration rate of AO7 could be increased by 16.7% under the condition of adding supported TiO2 in the pulsed streamer discharge system, compared to that in the sole pulsed streamer discharge plasma system, due to the synergistic effect of pulsed streamer discharge and TiO2 photocatalysis induced by pulsed streamer discharge. The synergistic system of pulsed streamer discharge and TiO2 photocatalyst was found to have more reactive radicals for degradation of organic compounds in water.展开更多
It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced ...It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.展开更多
TiO_2 sols modified by rare earth (RE) ions (Ce^(4+), Eu^(3+), or Nd^(3+))were prepared by coprecipitation-peptization method. The photocatalysis activity was studied byinvestigating the photodegradation effects of ac...TiO_2 sols modified by rare earth (RE) ions (Ce^(4+), Eu^(3+), or Nd^(3+))were prepared by coprecipitation-peptization method. The photocatalysis activity was studied byinvestigating the photodegradation effects of active brilliant red dye X-3B. It is found that TiO_2sols modified by Ce^(4+), Eu^(3+), or Nd^(3+) have the anatase crystalline structure, which areprepared at 70℃. All RE^(n+)-TiO_2 sol samples have uniform nanoparticles with similar morphology,which are homogenously distributed in aqueous colloidal systems. The particle sizes are 10, 8, and12 nm for Nd^(3+)-TiO_2, Eu^(3+)-TiO_2, and Ce^(4+)-TiO_2, respectively. The character of ultrafineand positive charge sol particles contributes to the good adsorption of X-3B dye molecule on thesurface of titania (about 30% X-3B adsorption amount). Experimental results exhibit thatRE^(n+)-TiO_2 sol photocatalysts have the capability to photodegrade X-3B under visible lightirradiation. Nd^(3+)-TiO_2 and Eu^(3+)-TiO_2 show higher photocatalytic activity than Ce^(4+)-TiO_2,which is due to the difference of standard redox potential of RE^(n+)/RE^((n-1)+). RE^(n+)-TiO_2sols demonstrate more excellent interfacial adsorption and photodegradation effects to X-3B thanP_(25) TiO_2 crystallites. Moreover, the degradation mechanism of X-3B is proposed as dyephotosensitization and electron scavenging by rare earth ions.展开更多
Based on the TiO2 photocatalysis mechanism, a new method of simultaneous desulfurization and denitrification from flue gas was proposed. Preparation of TiO2 photocatalyst, design of photocatalysis reactor and influenc...Based on the TiO2 photocatalysis mechanism, a new method of simultaneous desulfurization and denitrification from flue gas was proposed. Preparation of TiO2 photocatalyst, design of photocatalysis reactor and influencing factors for simul- taneous removal of SO2 and NO, and removal mechanism of SO2 and NO were studied. After the optimal values of concentration of O2 in flue gas, the relative humidity of flue gas and the irradiation time in the photocatalysis reactor were used, the efficiencies of removal for SO2 and NO can be achieved above 98% and about 67%, respectively. According to the results of removal products analysis, the re- moval mechanism of SO2 and NO based on TiO2 photocatlysis can be put forward, namely, SO2 was oxidized to SO3 partly, the bulk of NO was oxidized to NO2, and both were removed by resorbing finally.展开更多
We report a colloidal process to coat a layer of TiO2onto SiO2composite nanofibers containing embedded CdS and upconversion nanoparticles(UCNPs).The SiO2composite nanofibers were fabricated by electrospinning.To impro...We report a colloidal process to coat a layer of TiO2onto SiO2composite nanofibers containing embedded CdS and upconversion nanoparticles(UCNPs).The SiO2composite nanofibers were fabricated by electrospinning.To improve the energy transfer efficiency,UCNPs and CdS nanoparticles were bound in close proximity to each other within the SiO2matrix.β‐NaYF4:Yb(30%),Tm(0.5%)@NaYF4:Yb(20%),Er(2%)core–shell nanoparticles were used as nanotransducers for near infrared light.These nanoparticles exhibited enhanced upconversion fluorescence compared withβ‐NaYF4:Yb(30%),Tm(0.5%)orβ–NaYF4:Yb(30%),Tm(0.5%)@NaYF4nanoparticles.The morphologies,size and chemical compositions have been extensively investigated using field emission scanning electron microscopy(FESEM),transmission electron microscopy(TEM),X‐ray diffraction(XRD)and X‐ray photoelectron spectra(XPS),respectively.The TEM images showed that the TiO2composite nanotubes were embedded with a large amount of UCNPs and CdS nanoparticles.The composite TiO2nanotubes degraded more than90%of rhodamine B(RhB)dye during20min of irradiation by simulated solar light.In particular,more than50%of RhB was decomposed in70min,under irradiation of near infrared light(NIR).This high degradation was attributed to the full spectrum absorption of solar light,and the enhanced transfer efficiency for near infrared light.The as‐prepared nanostructures can harness solar energy,and provide an alternative to overcome energy shortages and environmental protection.展开更多
Bandgap engineering by doping and co‐catalyst loading are two primary approaches to designing efficient photocatalysts by promoting visible‐light absorption and charge separation,respectively.Shifting of the TiO2con...Bandgap engineering by doping and co‐catalyst loading are two primary approaches to designing efficient photocatalysts by promoting visible‐light absorption and charge separation,respectively.Shifting of the TiO2conduction band edge is frequently applied to increase visible‐light absorption but also lowers the reductive properties of photo‐excited electrons.Herein,we report a visible‐light‐driven photocatalyst based on valance band edge control induced by oxygen excess defects and modification with a CuxO electron transfer co‐catalyst.The CuxO grafted oxygen‐rich TiO2microspheres were prepared by ultrasonic spray pyrolysis of the peroxotitanate precursor followed by a wet chemical impregnated treatment.We found that oxygen excess defects in TiO2shifted the valence band maximum upward and improved the visible‐light absorption.The CuxO grafted onto the surface acted as a co‐catalyst that efficiently reduced oxygen molecules to active intermediates(i.e.,O2??radial and H2O2),thus consuming the photo‐generated electrons.Consequently,the CuxO grafted oxygen‐rich TiO2microspheres achieved a photocatalytic activity respectively8.6,13.0and11.0as times high as those of oxygen‐rich TiO2,normal TiO2and CuxO grafted TiO2,for degradation of gaseous acetaldehyde under visible‐light irradiation.Our results suggest that high visible‐light photocatalytic efficiency can be achieved by combining oxygen excess defects to improve visible‐light absorption together with a CuxO electron transfer co‐catalyst.These findings provide a new approach to developing efficient heterojunction photocatalysts.展开更多
化工、纺织印染与农药化肥等产业的蓬勃发展推动着人类社会的进步,但同时也给环境治理带来了巨大难题。目前,光催化降解局限于在特定波长下针对单一有机污染物进行降解,然而现实中的情况往往更复杂。因此,开发一种多功能光催化材料用于...化工、纺织印染与农药化肥等产业的蓬勃发展推动着人类社会的进步,但同时也给环境治理带来了巨大难题。目前,光催化降解局限于在特定波长下针对单一有机污染物进行降解,然而现实中的情况往往更复杂。因此,开发一种多功能光催化材料用于光催化降解不同有机污染物显得尤为重要。采用一步无模板溶剂热法合成了核壳结构的C-TiO_(2)复合材料前驱体,并在氩气气氛下煅烧得到高结晶度的C-TiO_(2)复合光催化材料。运用SEM、TEM、XRD和TG等表征手段对材料进行表征,结论如下:550℃煅烧时的样品为包含少量碳的高结晶度的锐钛矿相TiO 2,且550℃煅烧时的样品依然保持了完整的核壳结构。此外,C-TiO_(2)复合材料的比表面积高达85.69 m 2·g^(-1),平均孔径为16.4 nm以及孔体积为0.423 m 3·g^(-1)。在UV-Vis光照射下,C-TiO_(2)复合材料分别对罗丹明B(RhB)、亚甲基蓝(MB)和刚果红(CR)3种染料显示出增强的光催化降解活性。展开更多
基金supported by the National Natural Science Foundation Committee of China(No.20377006)Foundation of Education Ministry of China(No.2005141002)
文摘Photocatalyst was prepared by immobilizing TiO2 on glass beads using the traditional sol-gel method. Ultraviolet light （UV） produced by pulsed streamer discharge was then used to induce photocatalytic activity of TiO2 photocatalyst. Decolouration efficiency of the representative azo dye （acid orange 7, AOT） was investigated using the synergistic system of pulsed streamer discharge plasma and TiO2 photocatalysis. The obtained results showed that the decolouration rate of AO7 could be increased by 16.7% under the condition of adding supported TiO2 in the pulsed streamer discharge system, compared to that in the sole pulsed streamer discharge plasma system, due to the synergistic effect of pulsed streamer discharge and TiO2 photocatalysis induced by pulsed streamer discharge. The synergistic system of pulsed streamer discharge and TiO2 photocatalyst was found to have more reactive radicals for degradation of organic compounds in water.
基金the National Natural Science Foundation of China (22209091)the Natural Science Foundation of Shandong Province (ZR2020QB057)+1 种基金the Key Program of National Natural Science Foundation of China (22133006)the Yankuang Group 2019 Science and Technology Program (YKKJ2019AJ05JG-R60)。
文摘It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.
基金This work was financially supported by the Hi-Tech Research and Development Program (863 Program) of China (No. 2002AA302304)the National Natural Science Foundation of China (No. 60121101)the Education Department Foundation of Jiangsu Province (JHOl-
文摘TiO_2 sols modified by rare earth (RE) ions (Ce^(4+), Eu^(3+), or Nd^(3+))were prepared by coprecipitation-peptization method. The photocatalysis activity was studied byinvestigating the photodegradation effects of active brilliant red dye X-3B. It is found that TiO_2sols modified by Ce^(4+), Eu^(3+), or Nd^(3+) have the anatase crystalline structure, which areprepared at 70℃. All RE^(n+)-TiO_2 sol samples have uniform nanoparticles with similar morphology,which are homogenously distributed in aqueous colloidal systems. The particle sizes are 10, 8, and12 nm for Nd^(3+)-TiO_2, Eu^(3+)-TiO_2, and Ce^(4+)-TiO_2, respectively. The character of ultrafineand positive charge sol particles contributes to the good adsorption of X-3B dye molecule on thesurface of titania (about 30% X-3B adsorption amount). Experimental results exhibit thatRE^(n+)-TiO_2 sol photocatalysts have the capability to photodegrade X-3B under visible lightirradiation. Nd^(3+)-TiO_2 and Eu^(3+)-TiO_2 show higher photocatalytic activity than Ce^(4+)-TiO_2,which is due to the difference of standard redox potential of RE^(n+)/RE^((n-1)+). RE^(n+)-TiO_2sols demonstrate more excellent interfacial adsorption and photodegradation effects to X-3B thanP_(25) TiO_2 crystallites. Moreover, the degradation mechanism of X-3B is proposed as dyephotosensitization and electron scavenging by rare earth ions.
文摘Based on the TiO2 photocatalysis mechanism, a new method of simultaneous desulfurization and denitrification from flue gas was proposed. Preparation of TiO2 photocatalyst, design of photocatalysis reactor and influencing factors for simul- taneous removal of SO2 and NO, and removal mechanism of SO2 and NO were studied. After the optimal values of concentration of O2 in flue gas, the relative humidity of flue gas and the irradiation time in the photocatalysis reactor were used, the efficiencies of removal for SO2 and NO can be achieved above 98% and about 67%, respectively. According to the results of removal products analysis, the re- moval mechanism of SO2 and NO based on TiO2 photocatlysis can be put forward, namely, SO2 was oxidized to SO3 partly, the bulk of NO was oxidized to NO2, and both were removed by resorbing finally.
基金supported in part by the National Natural Science Foundation of China(21471043,21304028,51403195,31501576)~~
文摘We report a colloidal process to coat a layer of TiO2onto SiO2composite nanofibers containing embedded CdS and upconversion nanoparticles(UCNPs).The SiO2composite nanofibers were fabricated by electrospinning.To improve the energy transfer efficiency,UCNPs and CdS nanoparticles were bound in close proximity to each other within the SiO2matrix.β‐NaYF4:Yb(30%),Tm(0.5%)@NaYF4:Yb(20%),Er(2%)core–shell nanoparticles were used as nanotransducers for near infrared light.These nanoparticles exhibited enhanced upconversion fluorescence compared withβ‐NaYF4:Yb(30%),Tm(0.5%)orβ–NaYF4:Yb(30%),Tm(0.5%)@NaYF4nanoparticles.The morphologies,size and chemical compositions have been extensively investigated using field emission scanning electron microscopy(FESEM),transmission electron microscopy(TEM),X‐ray diffraction(XRD)and X‐ray photoelectron spectra(XPS),respectively.The TEM images showed that the TiO2composite nanotubes were embedded with a large amount of UCNPs and CdS nanoparticles.The composite TiO2nanotubes degraded more than90%of rhodamine B(RhB)dye during20min of irradiation by simulated solar light.In particular,more than50%of RhB was decomposed in70min,under irradiation of near infrared light(NIR).This high degradation was attributed to the full spectrum absorption of solar light,and the enhanced transfer efficiency for near infrared light.The as‐prepared nanostructures can harness solar energy,and provide an alternative to overcome energy shortages and environmental protection.
基金supported by the National Natural Science Foundation of China(51072032,51372036,51702235)~~
文摘Bandgap engineering by doping and co‐catalyst loading are two primary approaches to designing efficient photocatalysts by promoting visible‐light absorption and charge separation,respectively.Shifting of the TiO2conduction band edge is frequently applied to increase visible‐light absorption but also lowers the reductive properties of photo‐excited electrons.Herein,we report a visible‐light‐driven photocatalyst based on valance band edge control induced by oxygen excess defects and modification with a CuxO electron transfer co‐catalyst.The CuxO grafted oxygen‐rich TiO2microspheres were prepared by ultrasonic spray pyrolysis of the peroxotitanate precursor followed by a wet chemical impregnated treatment.We found that oxygen excess defects in TiO2shifted the valence band maximum upward and improved the visible‐light absorption.The CuxO grafted onto the surface acted as a co‐catalyst that efficiently reduced oxygen molecules to active intermediates(i.e.,O2??radial and H2O2),thus consuming the photo‐generated electrons.Consequently,the CuxO grafted oxygen‐rich TiO2microspheres achieved a photocatalytic activity respectively8.6,13.0and11.0as times high as those of oxygen‐rich TiO2,normal TiO2and CuxO grafted TiO2,for degradation of gaseous acetaldehyde under visible‐light irradiation.Our results suggest that high visible‐light photocatalytic efficiency can be achieved by combining oxygen excess defects to improve visible‐light absorption together with a CuxO electron transfer co‐catalyst.These findings provide a new approach to developing efficient heterojunction photocatalysts.
文摘化工、纺织印染与农药化肥等产业的蓬勃发展推动着人类社会的进步,但同时也给环境治理带来了巨大难题。目前,光催化降解局限于在特定波长下针对单一有机污染物进行降解,然而现实中的情况往往更复杂。因此,开发一种多功能光催化材料用于光催化降解不同有机污染物显得尤为重要。采用一步无模板溶剂热法合成了核壳结构的C-TiO_(2)复合材料前驱体,并在氩气气氛下煅烧得到高结晶度的C-TiO_(2)复合光催化材料。运用SEM、TEM、XRD和TG等表征手段对材料进行表征,结论如下:550℃煅烧时的样品为包含少量碳的高结晶度的锐钛矿相TiO 2,且550℃煅烧时的样品依然保持了完整的核壳结构。此外,C-TiO_(2)复合材料的比表面积高达85.69 m 2·g^(-1),平均孔径为16.4 nm以及孔体积为0.423 m 3·g^(-1)。在UV-Vis光照射下,C-TiO_(2)复合材料分别对罗丹明B(RhB)、亚甲基蓝(MB)和刚果红(CR)3种染料显示出增强的光催化降解活性。
