Two-dimensional (2D) ultrathin MoS2-modified black Ti^3+-TiO2 nanotubes were fabricated using an electrospinning-hydrothermal treatment-reduction method.Bare TiO2 nanotubes were fabricated via electrospinning.Then,2D ...Two-dimensional (2D) ultrathin MoS2-modified black Ti^3+-TiO2 nanotubes were fabricated using an electrospinning-hydrothermal treatment-reduction method.Bare TiO2 nanotubes were fabricated via electrospinning.Then,2D MoS2 lamellae were grown on the surface of the nanotubes and Ti^3+/Ov ions were introduced by reduction.The photocatalytic performance of the 2D MoS2/Ti^3+-TiO2 nanotubes was^15 times better than that of TiO2.The HER enhancement of the MoS2/Ti^3+-TiO2 nanotubes can be attributed to the Pt-like behavior of 2D MoS2 and the presence of Ti^3+-ions,which facilitated the quick diffusion of the photogenerated electrons to water,reducing the H2 activation barrier.The presence of Ov ions in the nanotubes and their hollow structure increased their solar utilization.展开更多
Low‐temperature selective catalytic reduction(SCR)of NO with NH3 was tested over Ho‐doped Mn–Ce/TiO2 catalysts prepared by the impregnation method.The obtained catalysts with different Ho doping ratios were charact...Low‐temperature selective catalytic reduction(SCR)of NO with NH3 was tested over Ho‐doped Mn–Ce/TiO2 catalysts prepared by the impregnation method.The obtained catalysts with different Ho doping ratios were characterized by Brunauer‐Emmett‐Teller(BET),X‐ray diffraction(XRD),temperature‐programmed reduction(H2‐TPR),temperature‐programmed desorption of NH3(NH3‐TPD),X‐ray photoelectron spectroscopy(XPS),and scanning electron microscopy(SEM).The catalytic activities were tested on a fixed bed.Their results indicated that the proper doping amount of Ho could effectively improve the low‐temperature denitrification performance and the SO2 resistance of Mn–Ce/TiO2 catalyst.The catalyst with Ho/Ti of 0.1 presented excellent catalytic activity,with a conversion of more than 90%in the temperature window of 140–220°C.The characterization results showed that the improved SCR activity of the Mn–Ce/TiO2 catalyst caused by Ho doping was due to the increase of the specific surface area,higher concentration of chemisorbed oxygen,higher surface Mn4+/Mn3+ratio,and higher acidity.The SO2 resistance test showed that the deactivating influence of SO2 on the catalyst was irreversible.The XRD and XPS results showed that the main reason for the catalyst deactivation was sulfates that had formed on the catalyst surface and that Ho doping could inhibit the sulfation to some extent.展开更多
A series of phosphorus-modified titanium dioxide samples with varying P/Ti atomic ratio were conveniently prepared via a conventional solgel route. The effects of phosphorus content and calcination temperature on the ...A series of phosphorus-modified titanium dioxide samples with varying P/Ti atomic ratio were conveniently prepared via a conventional solgel route. The effects of phosphorus content and calcination temperature on the crystalline structure, grain growth, surface area, and the photocatalytic activity of P-modified TiO2 were investigated. The XRD results showed that P species slow down the particle growth of anatase and increase the anatase-to-rutile phase transformation temperature to more than 900°C. Kinetic studies on the P-modified TiO2 to degraded 4-chlorophenol had found that the TP5500 prepared by adopting a P/Ti atomic ratio equal to 0.05 and calcined at 500°C had an apparent rate constant equal to 0.0075 min 1, which is superior to the performance of a commercial photocatalyst Degussa P25 Kapp = 0.0045 min 1 and of unmodified TiO2 （TP0500） Kapp = 0.0022 min 1. From HPLC analyses, various hydroxylated intermediates formed during oxidation had been identified, including hydroquinone （HQ）, benzoquinone （BQ） and （4CC） 4-chlorocatechol as main products. Phytotoxicity was assessed before and after irradiation against seed germination of tomato （Lycopersicon esculentum） whereas acute toxicity was assessed by using Folsomia candida as the test organism. Intermediates products were all less toxic than 4-chlorophenol and a significant removal of the overall toxicity was accomplished展开更多
Adding a small amount of nanocrystalline TiO2@C （TiO2 supported on nano- porous carbon） composite dramatically decreases the operating temperatures and improves the reaction kinetics for hydrogen storage in NaAlH4. ...Adding a small amount of nanocrystalline TiO2@C （TiO2 supported on nano- porous carbon） composite dramatically decreases the operating temperatures and improves the reaction kinetics for hydrogen storage in NaAlH4. The nano- crystalline TiO2@C composite synthesized at 900 ℃ （referred as TiO2@C-900） exhibits superior catalytic activity to other catalyst-containing samples. The onset dehydrogenation temperature of the TiO2@C-900-containing sample is lowered to 90 ℃; this is 65 ℃ lower than that of the pristine sample. The dehydrogenated sample is completely hydrogenated at 115 ℃ and 100 bar of hydrogen pressure with a hydrogen capacity of 4.5 wt.%. Structural analyses reveal that the Ti undergoes a reduction process of Ti^4＋→Ti^3＋→Ti^2＋→Ti during the ball milling and heating processes, and further converts to Ti hydrides or forms Ti-Al species after rehydrogenation. The catalytic activities of Ti-based catalytic species decrease in the order Al-Ti-species 〉 TiH0.71 〉 TiH2 〉 TiO2. This understanding guides further improvement in hydrogen storage properties of metal alanates using nanocrvstalline transition metal-based additives.展开更多
Carbon and few-layer MoS2 nanosheets co- modified TiO2 nanocomposites （defined as MoS2-C@TiO2） were prepared through a facile one-step pyrolysis reaction technique. In this unique nanostructure, the TiO2 nanosh- eet...Carbon and few-layer MoS2 nanosheets co- modified TiO2 nanocomposites （defined as MoS2-C@TiO2） were prepared through a facile one-step pyrolysis reaction technique. In this unique nanostructure, the TiO2 nanosh- eets with stable structure serve as the backbones, and carbon coating and few-layer MoS2 tightly adhere onto the surface of the TiO2. It needs to be pointed out that the carbon coating improves the overall electronic conductivity and the few-layer MoS2 facilitates the diffusion of lithium ions and offers more active sites for lithium-ion storage. As a result, when evaluated as lithium-ion battery anodes, the MoS2-C@TiO2 nanocomposites exhibit markedly enhanced lithium storage capability compared with pure TiO2. A high specific capacity of 180 mA.h.g-1 has been achieved during the preliminary cycles, and the specific capacity can maintain 160 mA.h.g-1 at a high current density of 1C （1C=167 mA.g-1） even after 300 discharge/ charge cycles, indicating the great potential of the MoS2- C@TiO2 on energy storage.展开更多
The adsorption equilibrium of a fluoride solution on 1-2 mm granular activated alumina modified by Fe2(SO4)3 solution was investigated.The experiments were conducted using a wide range of initial fluoride concentratio...The adsorption equilibrium of a fluoride solution on 1-2 mm granular activated alumina modified by Fe2(SO4)3 solution was investigated.The experiments were conducted using a wide range of initial fluoride concentrations(0.5 to 180 mg·L-1 at pH～7.0) and an adsorbent dose of 1.0 g·L-1.The application of Langmuir and Freundlich adsorption isotherm models(linear and nonlinear forms) generally showed that a single Langmuir or Freundlich equation cannot fit the entire concentration gap.Experimental data on low equilibrium concentrations(0.1 to 5.0 mg·L-1) was in line with both Langmuir and Freundlich isotherm models,whereas that of high equilibrium concentrations(5.0 to 150 mg·L-1) was more in line with the Freundlich isotherm model.A new LangmuirFreundlich function was used for the entire concentration gap,as well as for low and high concentrations.展开更多
TiO2 nanotube arrays were prepared by means of an electrochemical anodization technique in an organic electrolyte solution doped with polyvinyl pyrrolidone (PVP) and were subsequently modified with phosphomolybdic aci...TiO2 nanotube arrays were prepared by means of an electrochemical anodization technique in an organic electrolyte solution doped with polyvinyl pyrrolidone (PVP) and were subsequently modified with phosphomolybdic acid (PMoA) to obtain PMoA/TiO2 nanotube arrays. The microstructure and photochromic properties were investigated via X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), ultraviolet-visible spectroscopy (UV-vis), and X-ray photoelectron spectroscopy (XPS). The results indicated that the Keggin structure of PMoA and the nanotube structure of TiO2 were not destroyed, and there was a strong degree of interaction between PMoA and TiO2 at the biphasic interface with lattice interlacing during the compositing process. The XPS results further indicated that there was a change in the chemical microenvironment during the formation process of the composite, and a new charge transfer bridge was formed through the Mo-O-Ti bond. Under visible light irradiation, the colorless PMoA/TiO2 nanotube array quickly turned blue and exhibited a photochromic response together with reversible photochromism in the presence of H2O2. After visible light irradiation for 60s, the appearance of Mo^5+ species in the XPS spectra indicated a photoreduction process in accordance with a photoinduced electron transfer mechanism.展开更多
In this study,CuBi2O4 photocathodes were prepared using a simple electrodeposition method for photoelectrochemical(PEC)hydrogen production.The prepared photocathodes were modified with amorphous TiO2 and a Pt co‐cata...In this study,CuBi2O4 photocathodes were prepared using a simple electrodeposition method for photoelectrochemical(PEC)hydrogen production.The prepared photocathodes were modified with amorphous TiO2 and a Pt co‐catalyst,which resulted in the formation of CuBi2O4/TiO2 p‐n heterojunctions,and enhanced the activities of the as‐prepared photocathodes.The novel Pt/TiO2/CuBi2O4 photocathode exhibited a photocurrent of 0.35 mA/cm2 at 0.60 V vs.Reversible Hydrogen Electrode(RHE),which was nearly twice that of the Pt/CuBi2O4 photocathode.The present study provides a facile method for increasing the efficiency of photocathodes and provides meaningful guidance for the preparation of high‐performance CuBi2O4 photocathodes.展开更多
As the oxygen redox ability shows great effects on the catalytic performances of ceria-zirconia based materials,many strategies have been utilized to improve the oxygen storage capacity.Here in this study,we report a ...As the oxygen redox ability shows great effects on the catalytic performances of ceria-zirconia based materials,many strategies have been utilized to improve the oxygen storage capacity.Here in this study,we report a simple and facile approach to prepare a SO_(4)^(2-)-modified La,Y-doped ceria-zirconia material(SO/CZLY-f)with high oxygen storage capacity.Due to the additional redox process between SO_(4)^(2-)and S^(2-),oxygen storage capacity of SO/CZLY-f(745.3μmol O_(2)/g)is about 1.6 times higher than that of La,Ydoped ceria-zirconia material without SO_(4)^(2-)modification.Moreover,the catalytic activities and stability of the corresponding Pd-only three-way catalyst were measured.Compared to that of Pd@CZLY-f,the operation window of CO,full conversion temperature of HC and NO over Pd@SO/CZLY-f are obviously widened and lowered,respectively.After aging treatment at 1100℃for 4 h,the superiority of aged Pdloading composite is still maintained.展开更多
The ZnO-modified TiO2 electrode was prepared by adding Zn（CH3COO）2·2H2O to the TiO2 colloid during the sol-gel production process, and was used in dye-sensitized solar cells （DSCs）. The open circuit voltage ...The ZnO-modified TiO2 electrode was prepared by adding Zn（CH3COO）2·2H2O to the TiO2 colloid during the sol-gel production process, and was used in dye-sensitized solar cells （DSCs）. The open circuit voltage （Voc） and fill factor （if） of the cells were improved sig- nificantly. The performances of the ZnO-modified TiO2 electrode such as dark current, transient photocurrent, impedance, absorption spectra, and fiat band potential （Vfb） were investigated. It is found that the interface charge recombination impedance increases and Vfb shifts about 200 mV toward the cathodic potential. The effect mechanism of ZnO modification on the performance of DSCs may be that ZnO occupies the surface states of the TiO2 film.展开更多
Exploring low-cost and highly active photocatalysts is very urgent to accomplish complete removal of phenolic contaminants and overcome the limitations of the existing photocatalysts.In this study,we designed and synt...Exploring low-cost and highly active photocatalysts is very urgent to accomplish complete removal of phenolic contaminants and overcome the limitations of the existing photocatalysts.In this study,we designed and synthesized noble metal-free TiO2 photocatalysts by introducing bismuth nanoparticles as modifiers of a TiO2 single crystal(Bi-SCTiO2).The Bi-SCTiO2 can make full use of the synergistic effect of a small band overlap and low charge carrier density(Bi)with a high conductivity(single crystal),significantly boosting the separation and migration of the photogenerated charge pairs.Therefore,the Bi-SCTiO2 photocatalyst exhibits a significantly enhanced degradation rate(12 times faster)of 4-nitrophenol than a TiO2 single crystal under simulated sunlight irradiation.Notably,the complete removal of phenolic contaminants is achieved in various water matrices,which not only successfully overcomes the incomplete degradation in many reported photocatalytic systems,but also manifests a significant practical potential for sewage disposal.Therefore,this work presents a new insight in designing and constructing noble metal-free decorated semiconductor single-crystal photocatalysts with excellent activity and cyclability.展开更多
A novel rapid and continuous process has developed for the synthesis of nitrogen-doped TiO2（N-TiO2）with flame spray pyrolysis（FSP） method. The nitrogen incorporation into TiO2 was achieved by a facile modification...A novel rapid and continuous process has developed for the synthesis of nitrogen-doped TiO2（N-TiO2）with flame spray pyrolysis（FSP） method. The nitrogen incorporation into TiO2 was achieved by a facile modification（addition of dilute nitric acid） in the precursor for the synthesis. The catalysts were characterized by X-ray diffraction, Raman spectroscopy, transmission electron microscopy, diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy. The doping of nitrogen into the TiO2 was confirmed by X-ray photoelectron spectroscopy（XPS） and energy dispersive X-ray（EDX） spectroscopy. The UV-vis spectra of the modified catalysts（with primary N source） exhibited band-gap narrowing for 4 N-TiO2 with band gap energy of 2.89 eV, which may be due to the presence of nitrogen in TiO2 structure. The introduction of secondary N-source（urea） into TiO2 crystal lattice results in additional reduction of the band gap energy to 2.68 eV and shows a significant improvement of visible light absorption. The N-TiO2 nanoparticles modified by using secondary N-source showed significant photocatalytic activity under visible light much higher than TiO2. The higher activity is attributed to the synergetic interaction of nitrogen with the TiO2 lattice. The lowering of the band-gap energy for the flame made N-doped TiO2 materials implies that the nitrogen doping in TiO2 by aerosol method is highly effective in extending the optical response of TiO2 in the visible region. The nitrogen atomic percentage has increased monotonically（0.09%-0.15%）with the increase in primary nitrogen source（nitric acid）, and significantly boosted to 0.97% when secondary nitrogen source（urea） was introduced. The highest rate of phenol degradation was obtained for catalysts with secondary N source due to increase in N content in the catalyst.展开更多
TiO2 nanotubes （TiNT） were prepared by a hydrothermal treatment and modified by three kinds of amines,namely ethylenediamine,polyetherimide and tetraethylenepentamine （TEPA）,to study their CO2 adsorption propertie...TiO2 nanotubes （TiNT） were prepared by a hydrothermal treatment and modified by three kinds of amines,namely ethylenediamine,polyetherimide and tetraethylenepentamine （TEPA）,to study their CO2 adsorption properties from gas streams.The resultant samples were characterized by X-ray diffraction,transmission electron microscopy,and infrared spectroscopy,as well as low temperature N 2 adsorption.CO2 capture was investigated in a dynamic packed column at 30℃.TEPA-modified TiO2 nanotubes showed the highest adsorption capacity of 167.64 mg/g because it had the highest amino-group content among the three amines.CO2 fixation on TiNT impregnated by TEPA was investigated at 30,50,and 70℃,and the adsorption capacity increased slightly with temperature.Following the adsorption step,the sorbents were regenerated by temperature programmed desorption,and the TiNT-TEPA sample,as CO2 sorbent,was found to be readily regenerated and energy-efficient.The cycle test also revealed that the TiNT-TEPA adsorbent is fairly stable,with only a 5% drop in the adsorption capacity after 10 adsorption/desorption cycles.In addition,the CO2 adsorption behavior was investigated with the deactivation model,and which showed an excellent prediction for the TiNT-TEPA breakthrough curves.展开更多
The efficiency of photo-electrocatalytic（PECa） devices for the production of solar fuels depends on several limiting factors such as light harvesting, charge recombination and mass transport diffusion. We analyse he...The efficiency of photo-electrocatalytic（PECa） devices for the production of solar fuels depends on several limiting factors such as light harvesting, charge recombination and mass transport diffusion. We analyse here how they influence the performances in PECa cells having a photo-anode based on Au-modified TiOnanotube（TNT） arrays, with the aim of developing design criteria to optimize the photo-anode and the PECa cell configuration for water photo-electrolysis（splitting） and ethanol photo-reforming processes.The TNT samples were prepared by controlled anodic oxidation of Ti foils and then decorated with gold nanoparticles using different techniques to enhance the visible light response through heterojunction and plasmonic effects. The activity tests were made in a gas-phase reactor, as well as in a PECa cell without applied bias. Results were analysed in terms of photo-generated current, Hproduction rate and photoconversion efficiency. Particularly, a solar-to-hydrogen efficiency of 0.83% and a Faradaic efficiency of 91%were obtained without adding sacrificial reagents.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.51672249,51802282,and 11804301)the Zhejiang Provincial Natural Science Foundation of China(Grant Nos.LQ17F040004 and LY17E020001)Fundamental Research Funds of Zhejiang Sci-Tech University(No.2019Q062)。
文摘Two-dimensional (2D) ultrathin MoS2-modified black Ti^3+-TiO2 nanotubes were fabricated using an electrospinning-hydrothermal treatment-reduction method.Bare TiO2 nanotubes were fabricated via electrospinning.Then,2D MoS2 lamellae were grown on the surface of the nanotubes and Ti^3+/Ov ions were introduced by reduction.The photocatalytic performance of the 2D MoS2/Ti^3+-TiO2 nanotubes was^15 times better than that of TiO2.The HER enhancement of the MoS2/Ti^3+-TiO2 nanotubes can be attributed to the Pt-like behavior of 2D MoS2 and the presence of Ti^3+-ions,which facilitated the quick diffusion of the photogenerated electrons to water,reducing the H2 activation barrier.The presence of Ov ions in the nanotubes and their hollow structure increased their solar utilization.
文摘Low‐temperature selective catalytic reduction(SCR)of NO with NH3 was tested over Ho‐doped Mn–Ce/TiO2 catalysts prepared by the impregnation method.The obtained catalysts with different Ho doping ratios were characterized by Brunauer‐Emmett‐Teller(BET),X‐ray diffraction(XRD),temperature‐programmed reduction(H2‐TPR),temperature‐programmed desorption of NH3(NH3‐TPD),X‐ray photoelectron spectroscopy(XPS),and scanning electron microscopy(SEM).The catalytic activities were tested on a fixed bed.Their results indicated that the proper doping amount of Ho could effectively improve the low‐temperature denitrification performance and the SO2 resistance of Mn–Ce/TiO2 catalyst.The catalyst with Ho/Ti of 0.1 presented excellent catalytic activity,with a conversion of more than 90%in the temperature window of 140–220°C.The characterization results showed that the improved SCR activity of the Mn–Ce/TiO2 catalyst caused by Ho doping was due to the increase of the specific surface area,higher concentration of chemisorbed oxygen,higher surface Mn4+/Mn3+ratio,and higher acidity.The SO2 resistance test showed that the deactivating influence of SO2 on the catalyst was irreversible.The XRD and XPS results showed that the main reason for the catalyst deactivation was sulfates that had formed on the catalyst surface and that Ho doping could inhibit the sulfation to some extent.
文摘A series of phosphorus-modified titanium dioxide samples with varying P/Ti atomic ratio were conveniently prepared via a conventional solgel route. The effects of phosphorus content and calcination temperature on the crystalline structure, grain growth, surface area, and the photocatalytic activity of P-modified TiO2 were investigated. The XRD results showed that P species slow down the particle growth of anatase and increase the anatase-to-rutile phase transformation temperature to more than 900°C. Kinetic studies on the P-modified TiO2 to degraded 4-chlorophenol had found that the TP5500 prepared by adopting a P/Ti atomic ratio equal to 0.05 and calcined at 500°C had an apparent rate constant equal to 0.0075 min 1, which is superior to the performance of a commercial photocatalyst Degussa P25 Kapp = 0.0045 min 1 and of unmodified TiO2 （TP0500） Kapp = 0.0022 min 1. From HPLC analyses, various hydroxylated intermediates formed during oxidation had been identified, including hydroquinone （HQ）, benzoquinone （BQ） and （4CC） 4-chlorocatechol as main products. Phytotoxicity was assessed before and after irradiation against seed germination of tomato （Lycopersicon esculentum） whereas acute toxicity was assessed by using Folsomia candida as the test organism. Intermediates products were all less toxic than 4-chlorophenol and a significant removal of the overall toxicity was accomplished
文摘Adding a small amount of nanocrystalline TiO2@C （TiO2 supported on nano- porous carbon） composite dramatically decreases the operating temperatures and improves the reaction kinetics for hydrogen storage in NaAlH4. The nano- crystalline TiO2@C composite synthesized at 900 ℃ （referred as TiO2@C-900） exhibits superior catalytic activity to other catalyst-containing samples. The onset dehydrogenation temperature of the TiO2@C-900-containing sample is lowered to 90 ℃; this is 65 ℃ lower than that of the pristine sample. The dehydrogenated sample is completely hydrogenated at 115 ℃ and 100 bar of hydrogen pressure with a hydrogen capacity of 4.5 wt.%. Structural analyses reveal that the Ti undergoes a reduction process of Ti^4＋→Ti^3＋→Ti^2＋→Ti during the ball milling and heating processes, and further converts to Ti hydrides or forms Ti-Al species after rehydrogenation. The catalytic activities of Ti-based catalytic species decrease in the order Al-Ti-species 〉 TiH0.71 〉 TiH2 〉 TiO2. This understanding guides further improvement in hydrogen storage properties of metal alanates using nanocrvstalline transition metal-based additives.
基金financially supported by the National Natural Science Foundation of China(No.51472177)the China-EU Science and Technology Cooperation Project(No.SQ2013ZOA100006)
文摘Carbon and few-layer MoS2 nanosheets co- modified TiO2 nanocomposites （defined as MoS2-C@TiO2） were prepared through a facile one-step pyrolysis reaction technique. In this unique nanostructure, the TiO2 nanosh- eets with stable structure serve as the backbones, and carbon coating and few-layer MoS2 tightly adhere onto the surface of the TiO2. It needs to be pointed out that the carbon coating improves the overall electronic conductivity and the few-layer MoS2 facilitates the diffusion of lithium ions and offers more active sites for lithium-ion storage. As a result, when evaluated as lithium-ion battery anodes, the MoS2-C@TiO2 nanocomposites exhibit markedly enhanced lithium storage capability compared with pure TiO2. A high specific capacity of 180 mA.h.g-1 has been achieved during the preliminary cycles, and the specific capacity can maintain 160 mA.h.g-1 at a high current density of 1C （1C=167 mA.g-1） even after 300 discharge/ charge cycles, indicating the great potential of the MoS2- C@TiO2 on energy storage.
基金Supported by the Major National Science and Technology Special Project on Treatment and Control of Water Pollution(2009ZX07425-006)the State Key laboratory of Environmental Simulation and Pollution Control (09K04ESPCT)
文摘The adsorption equilibrium of a fluoride solution on 1-2 mm granular activated alumina modified by Fe2(SO4)3 solution was investigated.The experiments were conducted using a wide range of initial fluoride concentrations(0.5 to 180 mg·L-1 at pH～7.0) and an adsorbent dose of 1.0 g·L-1.The application of Langmuir and Freundlich adsorption isotherm models(linear and nonlinear forms) generally showed that a single Langmuir or Freundlich equation cannot fit the entire concentration gap.Experimental data on low equilibrium concentrations(0.1 to 5.0 mg·L-1) was in line with both Langmuir and Freundlich isotherm models,whereas that of high equilibrium concentrations(5.0 to 150 mg·L-1) was more in line with the Freundlich isotherm model.A new LangmuirFreundlich function was used for the entire concentration gap,as well as for low and high concentrations.
基金supported by the National Natural Science Foundation of China (No.61774073)Open Project of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University (No. 2016-25)Science and Technology Development Program of Jilin province (No. 20170101086JC)
文摘TiO2 nanotube arrays were prepared by means of an electrochemical anodization technique in an organic electrolyte solution doped with polyvinyl pyrrolidone (PVP) and were subsequently modified with phosphomolybdic acid (PMoA) to obtain PMoA/TiO2 nanotube arrays. The microstructure and photochromic properties were investigated via X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), ultraviolet-visible spectroscopy (UV-vis), and X-ray photoelectron spectroscopy (XPS). The results indicated that the Keggin structure of PMoA and the nanotube structure of TiO2 were not destroyed, and there was a strong degree of interaction between PMoA and TiO2 at the biphasic interface with lattice interlacing during the compositing process. The XPS results further indicated that there was a change in the chemical microenvironment during the formation process of the composite, and a new charge transfer bridge was formed through the Mo-O-Ti bond. Under visible light irradiation, the colorless PMoA/TiO2 nanotube array quickly turned blue and exhibited a photochromic response together with reversible photochromism in the presence of H2O2. After visible light irradiation for 60s, the appearance of Mo^5+ species in the XPS spectra indicated a photoreduction process in accordance with a photoinduced electron transfer mechanism.
基金the National Natural Science Foundation of China(51602179,21333006,21573135,11374190)the National Basic Research Program of China(973 Program,2013CB632401)~~
文摘In this study,CuBi2O4 photocathodes were prepared using a simple electrodeposition method for photoelectrochemical(PEC)hydrogen production.The prepared photocathodes were modified with amorphous TiO2 and a Pt co‐catalyst,which resulted in the formation of CuBi2O4/TiO2 p‐n heterojunctions,and enhanced the activities of the as‐prepared photocathodes.The novel Pt/TiO2/CuBi2O4 photocathode exhibited a photocurrent of 0.35 mA/cm2 at 0.60 V vs.Reversible Hydrogen Electrode(RHE),which was nearly twice that of the Pt/CuBi2O4 photocathode.The present study provides a facile method for increasing the efficiency of photocathodes and provides meaningful guidance for the preparation of high‐performance CuBi2O4 photocathodes.
基金Project supported by the Beijing Nova Program(Z181100006218030)Major State Research Development Program of Hebei province(20374202D)。
文摘As the oxygen redox ability shows great effects on the catalytic performances of ceria-zirconia based materials,many strategies have been utilized to improve the oxygen storage capacity.Here in this study,we report a simple and facile approach to prepare a SO_(4)^(2-)-modified La,Y-doped ceria-zirconia material(SO/CZLY-f)with high oxygen storage capacity.Due to the additional redox process between SO_(4)^(2-)and S^(2-),oxygen storage capacity of SO/CZLY-f(745.3μmol O_(2)/g)is about 1.6 times higher than that of La,Ydoped ceria-zirconia material without SO_(4)^(2-)modification.Moreover,the catalytic activities and stability of the corresponding Pd-only three-way catalyst were measured.Compared to that of Pd@CZLY-f,the operation window of CO,full conversion temperature of HC and NO over Pd@SO/CZLY-f are obviously widened and lowered,respectively.After aging treatment at 1100℃for 4 h,the superiority of aged Pdloading composite is still maintained.
基金supported by the Major State Basic Research Development Program of China (No.2006CB202605)the National Natural Science Foundation of China (No.50473055)
文摘The ZnO-modified TiO2 electrode was prepared by adding Zn（CH3COO）2·2H2O to the TiO2 colloid during the sol-gel production process, and was used in dye-sensitized solar cells （DSCs）. The open circuit voltage （Voc） and fill factor （if） of the cells were improved sig- nificantly. The performances of the ZnO-modified TiO2 electrode such as dark current, transient photocurrent, impedance, absorption spectra, and fiat band potential （Vfb） were investigated. It is found that the interface charge recombination impedance increases and Vfb shifts about 200 mV toward the cathodic potential. The effect mechanism of ZnO modification on the performance of DSCs may be that ZnO occupies the surface states of the TiO2 film.
文摘Exploring low-cost and highly active photocatalysts is very urgent to accomplish complete removal of phenolic contaminants and overcome the limitations of the existing photocatalysts.In this study,we designed and synthesized noble metal-free TiO2 photocatalysts by introducing bismuth nanoparticles as modifiers of a TiO2 single crystal(Bi-SCTiO2).The Bi-SCTiO2 can make full use of the synergistic effect of a small band overlap and low charge carrier density(Bi)with a high conductivity(single crystal),significantly boosting the separation and migration of the photogenerated charge pairs.Therefore,the Bi-SCTiO2 photocatalyst exhibits a significantly enhanced degradation rate(12 times faster)of 4-nitrophenol than a TiO2 single crystal under simulated sunlight irradiation.Notably,the complete removal of phenolic contaminants is achieved in various water matrices,which not only successfully overcomes the incomplete degradation in many reported photocatalytic systems,but also manifests a significant practical potential for sewage disposal.Therefore,this work presents a new insight in designing and constructing noble metal-free decorated semiconductor single-crystal photocatalysts with excellent activity and cyclability.
基金the U.S. EPA/Pegasus contract (contract number EP-C-11-006) for financial support of this work through the scholarship to Siva Nagi Reddy Inturi
文摘A novel rapid and continuous process has developed for the synthesis of nitrogen-doped TiO2（N-TiO2）with flame spray pyrolysis（FSP） method. The nitrogen incorporation into TiO2 was achieved by a facile modification（addition of dilute nitric acid） in the precursor for the synthesis. The catalysts were characterized by X-ray diffraction, Raman spectroscopy, transmission electron microscopy, diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy. The doping of nitrogen into the TiO2 was confirmed by X-ray photoelectron spectroscopy（XPS） and energy dispersive X-ray（EDX） spectroscopy. The UV-vis spectra of the modified catalysts（with primary N source） exhibited band-gap narrowing for 4 N-TiO2 with band gap energy of 2.89 eV, which may be due to the presence of nitrogen in TiO2 structure. The introduction of secondary N-source（urea） into TiO2 crystal lattice results in additional reduction of the band gap energy to 2.68 eV and shows a significant improvement of visible light absorption. The N-TiO2 nanoparticles modified by using secondary N-source showed significant photocatalytic activity under visible light much higher than TiO2. The higher activity is attributed to the synergetic interaction of nitrogen with the TiO2 lattice. The lowering of the band-gap energy for the flame made N-doped TiO2 materials implies that the nitrogen doping in TiO2 by aerosol method is highly effective in extending the optical response of TiO2 in the visible region. The nitrogen atomic percentage has increased monotonically（0.09%-0.15%）with the increase in primary nitrogen source（nitric acid）, and significantly boosted to 0.97% when secondary nitrogen source（urea） was introduced. The highest rate of phenol degradation was obtained for catalysts with secondary N source due to increase in N content in the catalyst.
基金supported by the Industry-Academia Cooperation Innovation Fund Projects of Jiangsu Province(No.BY2012025)
文摘TiO2 nanotubes （TiNT） were prepared by a hydrothermal treatment and modified by three kinds of amines,namely ethylenediamine,polyetherimide and tetraethylenepentamine （TEPA）,to study their CO2 adsorption properties from gas streams.The resultant samples were characterized by X-ray diffraction,transmission electron microscopy,and infrared spectroscopy,as well as low temperature N 2 adsorption.CO2 capture was investigated in a dynamic packed column at 30℃.TEPA-modified TiO2 nanotubes showed the highest adsorption capacity of 167.64 mg/g because it had the highest amino-group content among the three amines.CO2 fixation on TiNT impregnated by TEPA was investigated at 30,50,and 70℃,and the adsorption capacity increased slightly with temperature.Following the adsorption step,the sorbents were regenerated by temperature programmed desorption,and the TiNT-TEPA sample,as CO2 sorbent,was found to be readily regenerated and energy-efficient.The cycle test also revealed that the TiNT-TEPA adsorbent is fairly stable,with only a 5% drop in the adsorption capacity after 10 adsorption/desorption cycles.In addition,the CO2 adsorption behavior was investigated with the deactivation model,and which showed an excellent prediction for the TiNT-TEPA breakthrough curves.
基金The TERRA(Tandem Electrocatalytic Reactor for energy/Resource efficiency and process intensification,H2020 project 677471)Eco~2CO_2(Eco-friendly biorefinery fine chemicals from CO_2 photo-catalytic reduction,FP7 project 309701)
文摘The efficiency of photo-electrocatalytic（PECa） devices for the production of solar fuels depends on several limiting factors such as light harvesting, charge recombination and mass transport diffusion. We analyse here how they influence the performances in PECa cells having a photo-anode based on Au-modified TiOnanotube（TNT） arrays, with the aim of developing design criteria to optimize the photo-anode and the PECa cell configuration for water photo-electrolysis（splitting） and ethanol photo-reforming processes.The TNT samples were prepared by controlled anodic oxidation of Ti foils and then decorated with gold nanoparticles using different techniques to enhance the visible light response through heterojunction and plasmonic effects. The activity tests were made in a gas-phase reactor, as well as in a PECa cell without applied bias. Results were analysed in terms of photo-generated current, Hproduction rate and photoconversion efficiency. Particularly, a solar-to-hydrogen efficiency of 0.83% and a Faradaic efficiency of 91%were obtained without adding sacrificial reagents.
