Novel silver/silver molybdate(Ag/Ag2MoO4) composites with surface plasmon resonance(SPR)-enhanced photocatalytic performance were successfully fabricated via a facile one-pot hydrothermal route with the presence o...Novel silver/silver molybdate(Ag/Ag2MoO4) composites with surface plasmon resonance(SPR)-enhanced photocatalytic performance were successfully fabricated via a facile one-pot hydrothermal route with the presence of sodium dodecyl sulfate(SDS) in this study.The as prepared silver/silver molybdate(Ag/Ag2MoO4) composites were systematically characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM) and ultraviolet-visible diffuse reflectance absorption spectroscopy(DRS) in order to investigate their crystal structure,morphology and optical property as well.The photocatalytic activities of the composites were subsequently evaluated by their ability to degrade rhodamine B(RhB) under visible-light irradiation.Varies of controlled experiments were then carefully operated to gain a deep insight into the assembling of Ag/Ag2MoO4composites.It was found that preparation conditions such as pH,reaction time,and the amount of surfactant played important roles in the formation of composites with octahedral microstructures.And the composite obtained at 160 ℃ using 0.5 g of sodium dodecyl sulfate exhibited the highest photocatalytic performance under visible-light irradiation.Capture experiments were also conducted to clarify the function of different active species generated on the surface of Ag/Ag2MoO4during the photocatalytic process,in which both holes and ·OH radicals were found to play crucial role in photocatalytic removal of RhB under visible light irradiation.A possible photocatalytic mechanism of Ag/Ag2MoO4 was finally proposed on the basis of all the results to explain the higher photocatalytic activity of the octahedral Ag/Ag2MoO4 composites.It was inferred that the photoinduced "hot" electrons can quickly transfer from the Ag NPs to the conduction band of Ag2MoO4 and react with oxygen and H2O to generate a large quality of active radicals such as ·OH and ·O2^- because of the SPR effects.Besides,this SPR effects of Ag nanoparticles deposited on the surface of Ag2MoO4 can not only dramatically amplify its light absorption,especially in the visible region,but also promote the separation of photoexcited electron-hole pairs and effectively decrease electron-hole recombination.展开更多
Monodisperse ZnxCd1-xS spheres were successfully fabricated with a high yield by a facile hydrothermal route.The as-prepared samples were characterized by X-ray diffractometry,scanning electron microscopy and UV-vis d...Monodisperse ZnxCd1-xS spheres were successfully fabricated with a high yield by a facile hydrothermal route.The as-prepared samples were characterized by X-ray diffractometry,scanning electron microscopy and UV-vis diffusion reflectance spectroscopy.The results indicate that all the prepared samples have the same hexagonal wurtzite phase and exhibit good size uniformity and regularity.Degradation of rhodamine-B(RhB) was used to evaluate the photocatalytic activities of ZnxCd1-xS samples.Zn0.4Cd0.6S possessed the best photocatalytic activity and exhibited high stability during the reaction.展开更多
The photocatalytic activity of cobalt octakis(butylthio) porphyrazine(CoPz(BuS)8) was assessed through photodegradation of the dye rhodamine B(RhB) in water under irradiation with a Xe lamp and aerated conditi...The photocatalytic activity of cobalt octakis(butylthio) porphyrazine(CoPz(BuS)8) was assessed through photodegradation of the dye rhodamine B(RhB) in water under irradiation with a Xe lamp and aerated conditions.The photocatalytic activity of CoPz(BuS)8 loaded on Al2O3 or SiO2@Fe3O4nanoparticles or coordinated with an axial azide ligand was also investigated.The results demonstrated that the photocatalytic activity of CoPz(BuS)8 loaded on Al2O3 was higher than that loaded on SiO2@Fe3O4.The kinetic curves of RhB degradation in aqueous solutions at different pH indicated the pseudo first-order kinetics of the reaction.The highest degradation rate for CoPz(BuS)8 loaded Al2O3 at pH = 4 after 160 min was 84.6%.However,the advantages of easier separation and recycling as well as the ability to terminate the reaction at any time for the CoPz(BuS)8 loaded SiO2@Fe3O4 cannot be ignored.When electron-rich NaN3 was coordinated with CoPz(BuS)8 as an axial ligand and loaded on Al2O3,the resulting catalyst produced more active oxygen species such as O2^- and HO· to promote the quicker degradation of RhB than that by the other catalysts.For the N3-coordinated CoPz(BuS)8 loaded on Al2O3,the reactions at pH = 4 and 7 distinctly deviated from first-order kinetics,and the degradation rate reached 77.6%after 80 min at pH = 4.展开更多
The synergistic effect of high voltage discharge non‐thermal plasma(NTP)and photocatalysts on contaminant removal has repeatedly confirmed by plenty of researches.Most previous plasma‐photocatalyst synergistic syste...The synergistic effect of high voltage discharge non‐thermal plasma(NTP)and photocatalysts on contaminant removal has repeatedly confirmed by plenty of researches.Most previous plasma‐photocatalyst synergistic systems focused on the utilization of the ultraviolet light but ignored the visible light generated by high voltage discharge.Graphitic carbon nitride(g‐C3N4),a metal‐free semiconductor that exhibits high chemical stability,can utilize both the ultraviolet and visible light from high voltage discharge.However,the synergistic system of NTP and g‐C3N4 has been researched little.In this paper,the effect of NTP generated by dielectric barrier discharge(DBD)on g‐C3N4 is studied by comparing the photocatalytic activities,the surface physical structure and the surface chemical characteristics of pristine and plasma treated g‐C3N4.Experimental results indicate that the DBD plasma can change the physical structure and the chemical characteristics and to further affect the photocatalytic activity of g‐C3N4.The effect of NTP on g‐C3N4 is associated with the discharge intensity and the discharge time.For a long time scale,the effect of NTP on g‐C3N4 photocatalysts presents a periodic change trend.展开更多
Pyropia yezoensis, an intertidal seaweed, experiences regular dehydration and rehydration with the tides. In this study, the responses of P. yezoensis to dehydration and rehydration under high and low CO2 concentratio...Pyropia yezoensis, an intertidal seaweed, experiences regular dehydration and rehydration with the tides. In this study, the responses of P. yezoensis to dehydration and rehydration under high and low CO2 concentrations ((600-700)×10^-6 and (40-80)×10^-6, named Group I and Group II respectively) were investigated. The thalli of Group I had a significantly higher effective photosystem II quantum yield than the thalli of Group II at 71% absolute water content (AWC). There was little difference between thalli morphology, total Rubisco activity and total protein content at 100% and 71% AWC, which might be the basis for the normal performance of photosynthesis during moderate dehydration. A higher effective photosystem I quantum yield was observed in the thalli subjected to a low CO2 concentration during moderate dehydration, which might be caused by the enhancement of cyclic electron flow. These results suggested that P. yezoensis can directly utilize COz in ambient air during moderate dehydration.展开更多
A new MeTAMP (thiazolylazo dye ligand 2-[2-(5-methyl thiazolyl)azo]-4-methoxy phenol) was prepared by coupling reaction between 5-methyl thiazolylazonium chloride with 4-methoxy phenol in alkaline alcoholic soluti...A new MeTAMP (thiazolylazo dye ligand 2-[2-(5-methyl thiazolyl)azo]-4-methoxy phenol) was prepared by coupling reaction between 5-methyl thiazolylazonium chloride with 4-methoxy phenol in alkaline alcoholic solution. The structure of azo dye ligand has been characterized by available technique such as 1H-NMR, mass spectrum, FT-IR, UV-vis and elemental analysis. Eight new chelate complexes of Cr(III), Mn(II), Fe(II), Fe(III), Co(III), Ni(II), Cu(II) and Zn(II) ions were prepared and identified by elemental analysis, atomic absorption, magnetic susceptibility, molar conductance measurements, FT-IR and electronic spectra. The spectral and analytical data show that the ligand a tridentate and coordinating with metal ions through the phenolate O, azo N atom which is the farthest of thiazole molecule and with thiazole N atom. The molar ratio (M:L) was also studied which was found 1:1 for Zn(II) and 1:2 for the rest metal ions. Conductivity measurements for prepared complexes showed 1:1 electrolyte for Cr(III), Fe(IlI), and Co(llI) complexes and non-electrolyte for rest complexes. Stability constants of complexes were calculated by spectrophotometry. Octahedral configuration suggested for Cr(III), Mn(II), Fe(II), Fe(III), Co(III), Ni(II) and Cu(II) but tetrahedral for Zn(IlI) complex. The solid complexes are found to have the general formula IML2]Cl H2O where M = Cr(III), Fe(III) and Co(IIl) and [ML2] H2O where M = Mn(II), Fe(II), Ni(II) and Cu(II) while [MLCI].H20 for Zn(II)-complex. The biological activity of ligand and its complexes against five types of bacteria, Strepto coccus and Staphylococcus aureus as example of gram positive, Pseudomonas, Proteus and Esherichia coli as example of gram negative bacteria by agar plate different technique was studied. The activity was also assayed on molecular level by using PCR in an attempt to monitor DNA banding pattern.展开更多
A novel method combining dual wavelength fluorescent ratiometry with scanning near-field optical microscopy (SNOM) is proposed and developed to measure the concentration and distribution of protons in the vicinity of ...A novel method combining dual wavelength fluorescent ratiometry with scanning near-field optical microscopy (SNOM) is proposed and developed to measure the concentration and distribution of protons in the vicinity of biological samples. This method involves immersing mitochondria in a pH-sensitive fluorescent dye solution instead of injecting the dye into the surface of the mitochondrial membrane. It uses a dual emission pH-sensitive dye and SNOM with a thermally pulled and metal-coated optical fiber probe to improve the spatial resolution. The time dependence of the fluorescence intensity ratio (FIR) under acid addition and the response of mitochondria to nutritional supplementation were studied by using this method. Activation of mitochondria and a distance-dependent delay in the FIR response were observed. The results confirmed that mitochondrial activity could be observed by using this method.展开更多
Molybdenum ditelluride (MoTe2) has been demonstrated great potential in electronic and optoelectronic applications. However, the reported effective hole mobility remains far below its theoretical value. Herein, taki...Molybdenum ditelluride (MoTe2) has been demonstrated great potential in electronic and optoelectronic applications. However, the reported effective hole mobility remains far below its theoretical value. Herein, taking advantage of high-κ screening effect, we have fabricated back-gated MoTe2 transistors on an Al2O3 high-κ dielectric and systematically investigated the electronic and optoelectronic proper- ties. A high current on/off ratio exceeding 106 is achieved in the Al2O3-based MoTe2 transistors, and the hole mobility is demonstrated to be 150 cm2 V^-1 s^-1, compared to 0.2-20 cm^2 V^-1 s^-1 ever obtained from back-gated MoTe2 transistors in the literatures. Moreover, a considerable hole concentration of 1.2 × 10^13 cm 2 is attained in our Al2O3-based MoTe2 transistors owing to the strong gate control capa- bility, leading to a high on-state hole current of 6.1 μA μm^-1. After optimization, our Al2O3-based MoTe2 phototransistor exhibits outstanding photodetective performance, with a high responsivity of 543 AW^-1 and a high photogain of 1,662 at 405 nm light illumination, which are boosted around 419 times compared to the referential SiO2-based control devices. The mechanisms of photoconductivity in the Al2O3-based MoTe2 phototransistors have been analyzed in detail, and the photogating effect is considered to play an important role. This work may provide useful insight to improve carrier mobility in two-dimensional layered semiconductors and open opportunities to facilitate the development of high-performance photodetectors in the future.展开更多
Quantum chemical computations have been performed to evaluate the first and second hyperpolarizability quantities of the interference term, linear in the external static electric field, that appear in the electric fie...Quantum chemical computations have been performed to evaluate the first and second hyperpolarizability quantities of the interference term, linear in the external static electric field, that appear in the electric field-induced sum-frequency generation signal of chiral liquids. These are performed at the time-dependent Hartree-Fock level on the prototypical 1,1′-bi-2-naphtol chiral species.展开更多
Desymmetrization of prochiral 3-substituted glutaronitriles offers a new approach to access (S)-Pregabalin and (R)-Baclofen. A number of nitrilases from diverse sources were screened with 3-isobutylglutaronitriles...Desymmetrization of prochiral 3-substituted glutaronitriles offers a new approach to access (S)-Pregabalin and (R)-Baclofen. A number of nitrilases from diverse sources were screened with 3-isobutylglutaronitriles (1a) or 3-(4'-chlorophenyl)glutaronitriles (1b) as the substrate. Some nitrilases were found to catalyze the desymmetric hydrolysis of la and lb to form optically active 3-(cyanomethyl)-5-methylhexanoic acid (2a) and 3-(4'-chlorophenyl)-4-cyanobutanoic acid (2b) with high enantiomeric excesse (ee), respectively. This cannot be achieved using traditional chemical hydrolysis. Among them, AtNIT3 generated (R)-2b whereas BjNIT6402 and HsN1T produced the opposite (S)-enantiomer with high conversions and ee values. Not only the nitrilases showed different activities and stereoselectivities toward these 3-substituted glutaronitriles, the 3-substitueut of the substrates also exerted great effect on the enzyme activity and stereoselectivity. (S)-2a and (S)-2b were prepared with high yields and ee values using BjNIT6402 and HsNIT as the biocatalysts, respectively. A straightforward Curtius rearrangement of (S)-2a and (S)-2b, followed by the acidic hydrolysis, afforded (S)-Pregabalin and (R)-Baclofen. This offers a new platform methodology for the synthesis of optically active β-substituted T-amino acids of pharmaceutical importance.展开更多
Low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O nanopowders(NPs)would determine their practical application in purifying wastewater.In this contribution,ZnO NPs were scala...Low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O nanopowders(NPs)would determine their practical application in purifying wastewater.In this contribution,ZnO NPs were scalably synthesized via the simple reaction of Zn powder with H_2O vapor in autoclave.The structural,morphological and optical properties of the samples were systematically characterized by X-ray diffraction,scanning electron microscopy,Fourier transform infrared spectra,transmission electron microscopy,Micro-Raman,photoluminescence,and ultraviolet-visible spectroscopy.The as-prepared Zn O NPs are composed of nanoparticles with 100–150 nm in diameter,and have a small Brunauer-Emmett-Teller surface area of 6.85 m^2/g.The formation of Zn O nanoparticles is relative to the peeling of H_2 release.Furthermore,the product has big strain-stress leading to the red-shift in the band gap of product,and shows a strong green emission centered at 515 nm revealing enough atomic defects in Zn O NPs.As a comparison with P25,the obtained dust gray Zn O NPs have a strong absorbance in the region of 200–700 nm,suggesting the wide wave-band utilization in sunlight.Based on the traits above,the Zn O NPs show excellent photocatalytic activity on the degradation of rhodamine B(Rh-B)under solar light irradiation,close to that under UV irradiation.Importantly,the Zn O NPs could be well recycled in water due to the quick sedimentation in themselves in solution.The low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O NPs endow themselves with promising application in purifying wastewater.展开更多
基金supported by Fundamental Research Funds for the Central Universities (2662014BQ061, 2015PY120, 2015PY047, 2016PY088)the National Natural Science Foundation of China (51572101, 21502059, 21607047)~~
文摘Novel silver/silver molybdate(Ag/Ag2MoO4) composites with surface plasmon resonance(SPR)-enhanced photocatalytic performance were successfully fabricated via a facile one-pot hydrothermal route with the presence of sodium dodecyl sulfate(SDS) in this study.The as prepared silver/silver molybdate(Ag/Ag2MoO4) composites were systematically characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM) and ultraviolet-visible diffuse reflectance absorption spectroscopy(DRS) in order to investigate their crystal structure,morphology and optical property as well.The photocatalytic activities of the composites were subsequently evaluated by their ability to degrade rhodamine B(RhB) under visible-light irradiation.Varies of controlled experiments were then carefully operated to gain a deep insight into the assembling of Ag/Ag2MoO4composites.It was found that preparation conditions such as pH,reaction time,and the amount of surfactant played important roles in the formation of composites with octahedral microstructures.And the composite obtained at 160 ℃ using 0.5 g of sodium dodecyl sulfate exhibited the highest photocatalytic performance under visible-light irradiation.Capture experiments were also conducted to clarify the function of different active species generated on the surface of Ag/Ag2MoO4during the photocatalytic process,in which both holes and ·OH radicals were found to play crucial role in photocatalytic removal of RhB under visible light irradiation.A possible photocatalytic mechanism of Ag/Ag2MoO4 was finally proposed on the basis of all the results to explain the higher photocatalytic activity of the octahedral Ag/Ag2MoO4 composites.It was inferred that the photoinduced "hot" electrons can quickly transfer from the Ag NPs to the conduction band of Ag2MoO4 and react with oxygen and H2O to generate a large quality of active radicals such as ·OH and ·O2^- because of the SPR effects.Besides,this SPR effects of Ag nanoparticles deposited on the surface of Ag2MoO4 can not only dramatically amplify its light absorption,especially in the visible region,but also promote the separation of photoexcited electron-hole pairs and effectively decrease electron-hole recombination.
基金Project (20776016) supported by the National Natural Science Foundation of ChinaProject (20876109) supported by Program for New Century Excellent Talents in University of China
文摘Monodisperse ZnxCd1-xS spheres were successfully fabricated with a high yield by a facile hydrothermal route.The as-prepared samples were characterized by X-ray diffractometry,scanning electron microscopy and UV-vis diffusion reflectance spectroscopy.The results indicate that all the prepared samples have the same hexagonal wurtzite phase and exhibit good size uniformity and regularity.Degradation of rhodamine-B(RhB) was used to evaluate the photocatalytic activities of ZnxCd1-xS samples.Zn0.4Cd0.6S possessed the best photocatalytic activity and exhibited high stability during the reaction.
基金supported by National Natural Science Foundation of China (20977115, 21272281)Natural Science Foundation of Hubei Province (2014CFB919)the Science and Technology Plan Innovation Team of Wuhan City (2015070504020220)~~
文摘The photocatalytic activity of cobalt octakis(butylthio) porphyrazine(CoPz(BuS)8) was assessed through photodegradation of the dye rhodamine B(RhB) in water under irradiation with a Xe lamp and aerated conditions.The photocatalytic activity of CoPz(BuS)8 loaded on Al2O3 or SiO2@Fe3O4nanoparticles or coordinated with an axial azide ligand was also investigated.The results demonstrated that the photocatalytic activity of CoPz(BuS)8 loaded on Al2O3 was higher than that loaded on SiO2@Fe3O4.The kinetic curves of RhB degradation in aqueous solutions at different pH indicated the pseudo first-order kinetics of the reaction.The highest degradation rate for CoPz(BuS)8 loaded Al2O3 at pH = 4 after 160 min was 84.6%.However,the advantages of easier separation and recycling as well as the ability to terminate the reaction at any time for the CoPz(BuS)8 loaded SiO2@Fe3O4 cannot be ignored.When electron-rich NaN3 was coordinated with CoPz(BuS)8 as an axial ligand and loaded on Al2O3,the resulting catalyst produced more active oxygen species such as O2^- and HO· to promote the quicker degradation of RhB than that by the other catalysts.For the N3-coordinated CoPz(BuS)8 loaded on Al2O3,the reactions at pH = 4 and 7 distinctly deviated from first-order kinetics,and the degradation rate reached 77.6%after 80 min at pH = 4.
文摘The synergistic effect of high voltage discharge non‐thermal plasma(NTP)and photocatalysts on contaminant removal has repeatedly confirmed by plenty of researches.Most previous plasma‐photocatalyst synergistic systems focused on the utilization of the ultraviolet light but ignored the visible light generated by high voltage discharge.Graphitic carbon nitride(g‐C3N4),a metal‐free semiconductor that exhibits high chemical stability,can utilize both the ultraviolet and visible light from high voltage discharge.However,the synergistic system of NTP and g‐C3N4 has been researched little.In this paper,the effect of NTP generated by dielectric barrier discharge(DBD)on g‐C3N4 is studied by comparing the photocatalytic activities,the surface physical structure and the surface chemical characteristics of pristine and plasma treated g‐C3N4.Experimental results indicate that the DBD plasma can change the physical structure and the chemical characteristics and to further affect the photocatalytic activity of g‐C3N4.The effect of NTP on g‐C3N4 is associated with the discharge intensity and the discharge time.For a long time scale,the effect of NTP on g‐C3N4 photocatalysts presents a periodic change trend.
基金Supported by the Science and Technology Strategic Pilot Program of Chinese Academy of Sciences(No.XDA11020404)the National High Technology Research and Development Program of China(863 Program)(No.2012AA100806)+1 种基金the Tianjin Natural Science Foundation(No.12JCZDJC22200)the Project for Developing Marine Economy by Science and Technology in Tianjin(No.KX2010-0005)
文摘Pyropia yezoensis, an intertidal seaweed, experiences regular dehydration and rehydration with the tides. In this study, the responses of P. yezoensis to dehydration and rehydration under high and low CO2 concentrations ((600-700)×10^-6 and (40-80)×10^-6, named Group I and Group II respectively) were investigated. The thalli of Group I had a significantly higher effective photosystem II quantum yield than the thalli of Group II at 71% absolute water content (AWC). There was little difference between thalli morphology, total Rubisco activity and total protein content at 100% and 71% AWC, which might be the basis for the normal performance of photosynthesis during moderate dehydration. A higher effective photosystem I quantum yield was observed in the thalli subjected to a low CO2 concentration during moderate dehydration, which might be caused by the enhancement of cyclic electron flow. These results suggested that P. yezoensis can directly utilize COz in ambient air during moderate dehydration.
文摘A new MeTAMP (thiazolylazo dye ligand 2-[2-(5-methyl thiazolyl)azo]-4-methoxy phenol) was prepared by coupling reaction between 5-methyl thiazolylazonium chloride with 4-methoxy phenol in alkaline alcoholic solution. The structure of azo dye ligand has been characterized by available technique such as 1H-NMR, mass spectrum, FT-IR, UV-vis and elemental analysis. Eight new chelate complexes of Cr(III), Mn(II), Fe(II), Fe(III), Co(III), Ni(II), Cu(II) and Zn(II) ions were prepared and identified by elemental analysis, atomic absorption, magnetic susceptibility, molar conductance measurements, FT-IR and electronic spectra. The spectral and analytical data show that the ligand a tridentate and coordinating with metal ions through the phenolate O, azo N atom which is the farthest of thiazole molecule and with thiazole N atom. The molar ratio (M:L) was also studied which was found 1:1 for Zn(II) and 1:2 for the rest metal ions. Conductivity measurements for prepared complexes showed 1:1 electrolyte for Cr(III), Fe(IlI), and Co(llI) complexes and non-electrolyte for rest complexes. Stability constants of complexes were calculated by spectrophotometry. Octahedral configuration suggested for Cr(III), Mn(II), Fe(II), Fe(III), Co(III), Ni(II) and Cu(II) but tetrahedral for Zn(IlI) complex. The solid complexes are found to have the general formula IML2]Cl H2O where M = Cr(III), Fe(III) and Co(IIl) and [ML2] H2O where M = Mn(II), Fe(II), Ni(II) and Cu(II) while [MLCI].H20 for Zn(II)-complex. The biological activity of ligand and its complexes against five types of bacteria, Strepto coccus and Staphylococcus aureus as example of gram positive, Pseudomonas, Proteus and Esherichia coli as example of gram negative bacteria by agar plate different technique was studied. The activity was also assayed on molecular level by using PCR in an attempt to monitor DNA banding pattern.
基金supported by Grant-in-Aid for Scientific Research (B) (Grant No.22310078) from the Japan Society for the Promotion of Science (JSPS)
文摘A novel method combining dual wavelength fluorescent ratiometry with scanning near-field optical microscopy (SNOM) is proposed and developed to measure the concentration and distribution of protons in the vicinity of biological samples. This method involves immersing mitochondria in a pH-sensitive fluorescent dye solution instead of injecting the dye into the surface of the mitochondrial membrane. It uses a dual emission pH-sensitive dye and SNOM with a thermally pulled and metal-coated optical fiber probe to improve the spatial resolution. The time dependence of the fluorescence intensity ratio (FIR) under acid addition and the response of mitochondria to nutritional supplementation were studied by using this method. Activation of mitochondria and a distance-dependent delay in the FIR response were observed. The results confirmed that mitochondrial activity could be observed by using this method.
基金supported by the National Key Research and Development Program of China(2016YFA0302300,016YFA0200400)the National Science and Technology Major Project of China(2016ZX02301001)+1 种基金the National Natural Science Foundation of China(61306105)the Tsinghua University Initiative Scientific Research Program
文摘Molybdenum ditelluride (MoTe2) has been demonstrated great potential in electronic and optoelectronic applications. However, the reported effective hole mobility remains far below its theoretical value. Herein, taking advantage of high-κ screening effect, we have fabricated back-gated MoTe2 transistors on an Al2O3 high-κ dielectric and systematically investigated the electronic and optoelectronic proper- ties. A high current on/off ratio exceeding 106 is achieved in the Al2O3-based MoTe2 transistors, and the hole mobility is demonstrated to be 150 cm2 V^-1 s^-1, compared to 0.2-20 cm^2 V^-1 s^-1 ever obtained from back-gated MoTe2 transistors in the literatures. Moreover, a considerable hole concentration of 1.2 × 10^13 cm 2 is attained in our Al2O3-based MoTe2 transistors owing to the strong gate control capa- bility, leading to a high on-state hole current of 6.1 μA μm^-1. After optimization, our Al2O3-based MoTe2 phototransistor exhibits outstanding photodetective performance, with a high responsivity of 543 AW^-1 and a high photogain of 1,662 at 405 nm light illumination, which are boosted around 419 times compared to the referential SiO2-based control devices. The mechanisms of photoconductivity in the Al2O3-based MoTe2 phototransistors have been analyzed in detail, and the photogating effect is considered to play an important role. This work may provide useful insight to improve carrier mobility in two-dimensional layered semiconductors and open opportunities to facilitate the development of high-performance photodetectors in the future.
基金The calculations were performed on the computing facilities of the Consortium deséquipements de Calcul Intensif(CéCI),in particular those of the Plateforme Technologique de Calcul Intensif(PTCI)installed in the University of Namur,for which we gratefully acknowledge financial support of the FNRS-FRFC(2.4.617.07.F,2.5020.11)
文摘Quantum chemical computations have been performed to evaluate the first and second hyperpolarizability quantities of the interference term, linear in the external static electric field, that appear in the electric field-induced sum-frequency generation signal of chiral liquids. These are performed at the time-dependent Hartree-Fock level on the prototypical 1,1′-bi-2-naphtol chiral species.
基金financially supported by the Chinese Academy of Sciences (KSZD-EW-Z-015)the CAS Agenda to Provide S&T Support and Services for the National Strategic Emerging Industries
文摘Desymmetrization of prochiral 3-substituted glutaronitriles offers a new approach to access (S)-Pregabalin and (R)-Baclofen. A number of nitrilases from diverse sources were screened with 3-isobutylglutaronitriles (1a) or 3-(4'-chlorophenyl)glutaronitriles (1b) as the substrate. Some nitrilases were found to catalyze the desymmetric hydrolysis of la and lb to form optically active 3-(cyanomethyl)-5-methylhexanoic acid (2a) and 3-(4'-chlorophenyl)-4-cyanobutanoic acid (2b) with high enantiomeric excesse (ee), respectively. This cannot be achieved using traditional chemical hydrolysis. Among them, AtNIT3 generated (R)-2b whereas BjNIT6402 and HsN1T produced the opposite (S)-enantiomer with high conversions and ee values. Not only the nitrilases showed different activities and stereoselectivities toward these 3-substituted glutaronitriles, the 3-substitueut of the substrates also exerted great effect on the enzyme activity and stereoselectivity. (S)-2a and (S)-2b were prepared with high yields and ee values using BjNIT6402 and HsNIT as the biocatalysts, respectively. A straightforward Curtius rearrangement of (S)-2a and (S)-2b, followed by the acidic hydrolysis, afforded (S)-Pregabalin and (R)-Baclofen. This offers a new platform methodology for the synthesis of optically active β-substituted T-amino acids of pharmaceutical importance.
基金the National Natural Science Foundation of China (21161016)the Natural Science Foundation of Jiangxi Province (20142BAB216013)+1 种基金Jiangxi Education Department Fund (KJLD14087, GJJ14714)Jiangxi Environmental Protection Department Fund ([2013]370)
文摘Low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O nanopowders(NPs)would determine their practical application in purifying wastewater.In this contribution,ZnO NPs were scalably synthesized via the simple reaction of Zn powder with H_2O vapor in autoclave.The structural,morphological and optical properties of the samples were systematically characterized by X-ray diffraction,scanning electron microscopy,Fourier transform infrared spectra,transmission electron microscopy,Micro-Raman,photoluminescence,and ultraviolet-visible spectroscopy.The as-prepared Zn O NPs are composed of nanoparticles with 100–150 nm in diameter,and have a small Brunauer-Emmett-Teller surface area of 6.85 m^2/g.The formation of Zn O nanoparticles is relative to the peeling of H_2 release.Furthermore,the product has big strain-stress leading to the red-shift in the band gap of product,and shows a strong green emission centered at 515 nm revealing enough atomic defects in Zn O NPs.As a comparison with P25,the obtained dust gray Zn O NPs have a strong absorbance in the region of 200–700 nm,suggesting the wide wave-band utilization in sunlight.Based on the traits above,the Zn O NPs show excellent photocatalytic activity on the degradation of rhodamine B(Rh-B)under solar light irradiation,close to that under UV irradiation.Importantly,the Zn O NPs could be well recycled in water due to the quick sedimentation in themselves in solution.The low-cost and scalable preparation,high photocatalytic activity,and convenient recycle of Zn O NPs endow themselves with promising application in purifying wastewater.