Al/Co co-doped α-Ni（OH）2 samples were prepared by either ultrasonic co-precipitation method （Sample B） or co-precipitation method （Sample A）. The crystal structure and particle size distribution of the prepared...Al/Co co-doped α-Ni（OH）2 samples were prepared by either ultrasonic co-precipitation method （Sample B） or co-precipitation method （Sample A）. The crystal structure and particle size distribution of the prepared samples were examined by X-ray diffraction （XRD） and laser particle size analyzer, respectively. The results show that Sample B has more crystalline defects and smaller average diameter than Sample A. The cyclic voltammetry and electrochemical impedance spectroscopy measurements indicate that Sample B has better electrochemical performance than Sample A, such as better reaction reversibility, lower charge-transfer resistance and better cyclic stability. Proton diffusion coefficient of Sample B is 1.96×10-10cm2/s, which is two times as large as that （9.78×10-11cm2/s） of Sample A. The charge-discharge tests show that the discharge capacity （308 mA·h/g） of Sample B is 25 mA·h/g higher than that of Sample A （283 mA·h/g）.展开更多
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
Electronic structure and optical properties of neutral and charged low band gap alternating copolyfluorenes （Green 1, which is based on alternating repeating units consisting of alkyl-substituted fluorene and a thiop...Electronic structure and optical properties of neutral and charged low band gap alternating copolyfluorenes （Green 1, which is based on alternating repeating units consisting of alkyl-substituted fluorene and a thiophene-[1,2,5]thiadiazolo-[3,4]quinoxaline-thiophene （T-TDQ-T） unit were investigated theoretically with time-dependent density functional theory （TD-DFT） method, and their excited state properties were further analyzed with 2D site and 3D cube representations. For neutral Green 1, the band gap, binding energy, exciton binding energy, and nuclear relaxation energy were obtained. The transition dipole moments of neutral and charged Green 1 are compared using 3D transition density, which reveals the orientation and strength of transition dipole moments. The charge redistribution of neutral and charged Green 1 upon excitation are displayed and compared with 3D charge difference density. The electron-hole coherences of neutral and charged Green 1 upon excitation are investigated with 2D site representation （transition density matrix）. The excited state properties of neutral Green 1 calculated with TD-DFT method are compared with that calculated with ZINDO method, which reveals the importance of electron-electron interaction （in TD-DFT） in the excited state properties.展开更多
Low optical absorption and photocorrosion are two crucial issues limiting the practical applications of zinc oxide(ZnO)-based photocatalysts.In this paper,we report the fabrication of graphitic-carbon-mediated ZnO nan...Low optical absorption and photocorrosion are two crucial issues limiting the practical applications of zinc oxide(ZnO)-based photocatalysts.In this paper,we report the fabrication of graphitic-carbon-mediated ZnO nanorod arrays(NRAs)with enhanced photocatalytic activity and photostability for CO2 reduction under visible light irradiation.ZnO NRA/C-x(x=005,01,02,and 03)nanohybrids are prepared by calcining pre-synthesized ZnO NRAs with different amounts of glucose(0.05,0.1,0.2,and 0.3 g)as a carbon source via a hydrothermal method.X-ray photoelectron spectroscopy reveals that the obtained ZnO NRA/C-x nanohybrids are imparted with the effects of both carbon doping and carbon coating,as evidenced by the detected C-O-Zn bond and the C-C,C-O and C=O bonds,respectively.While the basic structure of ZnO remains unchanged,the UV-Vis absorption spectra show increased absorbance owing to the carbon doping effect in the ZnO NRA/C-x nanohybrids.The photoluminescence(PL)intensities of ZnO NRA/C-x nanohybrids are lower than that of bare ZnO NRA,indicating that the graphitic carbon layer coated on the surface of the ZnO NRA significantly enhances the charge carrier separation and transport,which in turn enhances the photoelectrochemical property and photocatalytic activity of the ZnO NRA/C-x nanohybrids for CO2 reduction.More importantly,a long-term reaction of photocatalytic CO2 reduction demonstrates that the photostability of ZnO NRA/C-x nanohybrids is significantly increased in comparison with the bare ZnO NRA.展开更多
The excited-state symmetry-breaking charge transfer (SBCT) dynamics in quadrupolar or octupolar molecules without clear infrared markers is usually hard to be tracked directly. In this work, on the basis of the evolut...The excited-state symmetry-breaking charge transfer (SBCT) dynamics in quadrupolar or octupolar molecules without clear infrared markers is usually hard to be tracked directly. In this work, on the basis of the evolution of instantaneous emission dipole moment obtained by femtosecond transient fluorescence spectroscopy, we presented a real-time characterization of the solvent-induced SBCT dynamics in an octupolar triphenylamine derivative. While the emission dipole moment of the octupolar trimer in weakly polar toluene changes little during the excited-state relaxation, it exhibits a fast reduction in a few picoseconds in strongly polar tetrahydrofuran. In comparison with the uorescence dynamics of dipolar monomer, we deduced that the emitting state of the octupolar trimer in strongly polar solvent, which undergoes solvent-induced structural uctuation, changes from exciton-coupled octupolar to excitation localized dipolar symmetry. In weakly polar solvent, the octupolar symmetry of the trimer is largely preserved during the solvation stabilization.展开更多
Metal-free indoline dyes for dye-sensitized solar cells were studied by employing quantum chemistry methods. Comparative study of the properties of both ground and excited states of metal-free indoline dyes for dye-se...Metal-free indoline dyes for dye-sensitized solar cells were studied by employing quantum chemistry methods. Comparative study of the properties of both ground and excited states of metal-free indoline dyes for dye-sensitized solar cells revealed： （i） as the number of rhodanine rings increases, the energy difference between HOMO and LUMO decreases and there is a red shift in the absorption spectrum with the binding energy increased, and the transition dipole moment decreased; （ii） Based on an analysis of charge differential density, we observed that the charge and energy are transfered from the phenylethenyl to the indoline and rhodanine rings; （iii） The electron-hole coherences are mainly on the indoline and rhodanine rings, and the exciton sizes are 30 and 40 atoms for indoline dyes with one and two rhodanline rings, respectively. These results serve as a good example of computer-aided design in metal-free indoline dyes for dye-sensitized solar cells.展开更多
Low-cost, highly efficient catalysts for hydrogen evolution reaction(HER) are very important to advance energy economy based on clean hydrogen gas. Intensive studies on two-dimensional molybdenum disulfides(2 D Mo S2)...Low-cost, highly efficient catalysts for hydrogen evolution reaction(HER) are very important to advance energy economy based on clean hydrogen gas. Intensive studies on two-dimensional molybdenum disulfides(2 D Mo S2) have been conducted due to their remarkable catalytic properties.However, most of the reported syntheses are time consuming,complicated and less efficient. The present work demonstrates the production of Mo S2/graphene catalyst via an ultra-fast(60 s) microwave-initiated approach. High specific surface area and conductivity of graphene delivers a favorable conductive network for the growth of Mo S2 nanosheets, along with rapid charge transfer kinetics. As-produced Mo S2/graphene nanocomposites exhibit superior electrocatalytic activity for the HER in acidic medium, with a low onset potential of62 m V, high cathodic currents and a Tafel slope of43.3 m V/decade. Beyond excellent catalytic activity, Mo S2/graphene reveals long cycling stability with a very high cathodic current density of around 1000 m A cm^-2 at an overpotential of 250 m V. Moreover, the Mo S2/graphene-catalyst exhibits outstanding HER activities in a temperature range of 30 to 120°C with low activation energy of36.51 k J mol^-1, providing the opportunity of practical scalable processing.展开更多
A non-sulfur chemosensor based on an easy to prepare double naphthalene Schiff base is reported for the colorimetric and fluorometric dual-channel sensing of Hg2+ ions by taking advantage of the twisted intramolecular...A non-sulfur chemosensor based on an easy to prepare double naphthalene Schiff base is reported for the colorimetric and fluorometric dual-channel sensing of Hg2+ ions by taking advantage of the twisted intramolecular charge transfer (TICT) mechanism. This work provides a novel approach for the selective recognition of mercury ions. Moreover, this sensor serves as a potential recyclable component in sensing materials and the complex L-Hg2+ (L = 1-[(2-naphthalenylimino)methyl]-2-naphthalenol) can therefore be used as a fluorescent sensor for iodine anions. Notably, the color changes are very significant and all the recognition and recycling processes can be observed by the naked eye.展开更多
A series of Eu3+ -incorporated ETS-10 samples were successfully prepared based on the traditional ion exchange method. The relationship between photogenerated charge behaviors and luminescent properties has been inves...A series of Eu3+ -incorporated ETS-10 samples were successfully prepared based on the traditional ion exchange method. The relationship between photogenerated charge behaviors and luminescent properties has been investigated in detail. It has been demonstrated that as a result of the charge transfer from the titanate quantum wires to Eu3+ crystal field states, the host matrix ETS-10 functions as the sensitizer of Eu3+ to enhance the red luminescence, while Eu3+ cations contribute to the recombination of photogenerated charges. The behavior of photogenerated charges has significant impact on the luminescent properties of Eu3+ -incorporated ETS-10 materials.展开更多
MXene is a variety of new two-dimensional(2D)materials with early transition metal carbides,nitrides,and carbonitrides.Quantum chemical studies have been carried out on the geometries,electronic structures,stability a...MXene is a variety of new two-dimensional(2D)materials with early transition metal carbides,nitrides,and carbonitrides.Quantum chemical studies have been carried out on the geometries,electronic structures,stability and catalytic properties of a non-noble metal single-atom catalyst(SAC)with single Co atom anchored on MXene materials of Mo_(2)CS_(2).The Co adatom anchored on top of the Mo atom of this MXene is found to be rather stable,and this SAC is appropriate for CO oxidation.The charge transfers from the surface to the adsorbed CO and O2 play a significant role in the activation of these molecules on Co_(1)/Mo_(2)CS_(2).With this catalyst,the Eley-Rideal(ER),Langmuir-Hinshelwood(LH),and Termolecular Eley-Rideal(TER)mechanisms are explored for CO oxidation.We find that,while all the three mechanisms are feasible at low temperature,Co_(1)/Mo_(2)CS_(2) possesses higher catalytic activity for CO oxidation through the TER mechanism that features an intriguing OC(OO)CO intermediate(IM)adsorbed on Co single atom.The calculated activation energy barriers of the rate-limiting step are 0.67 eV(TER),0.78 eV(LH)and 0.88 eV(ER),respectively.The present study illustrates that it is promising to develop and design low-cost,non-noble metal SACs using MXene types of 2D materials.展开更多
In this paper,poly(pyridine-imide)s,PI-Ph and PI-Naphth,were successfully synthesised and fabricated for use as memory devices.The Al/PI-Ph/indium tin oxide(ITO)device showed dynamic random access memory characteristi...In this paper,poly(pyridine-imide)s,PI-Ph and PI-Naphth,were successfully synthesised and fabricated for use as memory devices.The Al/PI-Ph/indium tin oxide(ITO)device showed dynamic random access memory characteristics,whereas Al/PI-Naphth/ITO showed rewritable(FLASH)memory characteristics.Characterisation of their UV,cyclic voltammograms,and density functional theory,were used to illustrate the different memory behaviours.The results show that the stability of electric-field-induced-charge-transfer complexes can affect memory performance.展开更多
Molecular-based conducting magnet or magnetic conductor, is an overlap of organic conductor and molecular magnet. Due to the existence of ferromagnetism, antiferromagnetism and quantum magnetism in insulated charge-tr...Molecular-based conducting magnet or magnetic conductor, is an overlap of organic conductor and molecular magnet. Due to the existence of ferromagnetism, antiferromagnetism and quantum magnetism in insulated charge-transfer salt, it becomes a common sense that magnetism is not good for conductivity. After the discovery of first molecular-based metallic ferromagnet, molecular-based conducting magnet with n-unit from organic conductor and magnetism from coordination counterion became a hot area. The metallic ferromagnet, semiconductor room-temperature ferrimagnet, metallic weak ferromagnet and supercon- ducting antiferromagnet have been discovered. The new molecular-based conducting magnet with higher conductivity and higher magnetic ordering temperature is expected.展开更多
This article summarized the recent advance on the structural design and synthetic strategies of intramolec- ular charge-transfer compounds as well as their potential ap- plications in two-photon absorption chromophore...This article summarized the recent advance on the structural design and synthetic strategies of intramolec- ular charge-transfer compounds as well as their potential ap- plications in two-photon absorption chromophores, organic photovoltaics and organic light-emitting diodes.展开更多
Light absorption plays an important role in improving the power conversion efficiency(PCE)of quantum dot-sensitized solar cells(QDSSCs).In this study,a multifunctional long-persistence phosphor(LPP)layer was introduce...Light absorption plays an important role in improving the power conversion efficiency(PCE)of quantum dot-sensitized solar cells(QDSSCs).In this study,a multifunctional long-persistence phosphor(LPP)layer was introduced into the CdS/CdSe QDSSCs via a simple doctor blade method.The LPP layer can simultaneously improve the light harvesting and photo charge transfer in CdS/CdSe QDSSCs.As a result,their short-circuit current and corresponding PCE are effectively enhanced.The PCE can reach up to 5.07%,which is about 24%larger than that of the conventional CdS/CdSe QDSSCs without LPP layer.The solar cells can work in dark for a while due to the long-lasting fluorescence of the LPP layer.This research provides an effective way to improve the PCE of QDSSCs,and finds the possibility for all-weather QDSSCs.展开更多
The organic single-crystal field-effect transistors using anthracene derivative, H-Ant as an active layer with source/drain electrodes decorated by metal charge transfer salt(Cu TCNQ) were fabricated. We demonstrated ...The organic single-crystal field-effect transistors using anthracene derivative, H-Ant as an active layer with source/drain electrodes decorated by metal charge transfer salt(Cu TCNQ) were fabricated. We demonstrated that this bottom-contact structure displayed an obvious improvement in the electrical characteristics relative to their pristine copper and top-contact gold electrode counterparts. This observation could be ascribed to the lower contact resistance resulting from the energetic match between electrodes and semiconductor.展开更多
Though several theoretical models have been proposed to design electronic flat-bands, the definite experimental realization in two-dimensional atomic crystal is still lacking. Here we propose a novel and realistic fla...Though several theoretical models have been proposed to design electronic flat-bands, the definite experimental realization in two-dimensional atomic crystal is still lacking. Here we propose a novel and realistic flat-band model based on threefold degenerate p-orbitals in two-dimensional ionic materials. Our theoretical analysis and first-principles calculations show that the proposed flat-band can be realized in 1 T layered materials of alkali-metal chalogenides and metal-carbon group compounds. Some of the former are theoretically predicted to be stable as layered materials(e.g., K2 S), and some of the latter have been experimentally fabricated in previous works(e.g., Gd2 CCl2). More interestingly, the flat-band is partially filled in the heterostructure of a K2 S monolayer and graphene layers. The spin polarized nearly flatband can be realized in the ferromagnetic state of a Gd2 CCl2 monolayer, which has been fabricated in experiments. Our theoretical model together with the material predictions provide a realistic platform for the study of flat-bands and related exotic quantum phases.展开更多
基金Project (10774030) supported by the National Natural Science Foundation of ChinaProject (2008J1-C161) supported by the Science and Technology Program of Guangzhou City of China
文摘Al/Co co-doped α-Ni（OH）2 samples were prepared by either ultrasonic co-precipitation method （Sample B） or co-precipitation method （Sample A）. The crystal structure and particle size distribution of the prepared samples were examined by X-ray diffraction （XRD） and laser particle size analyzer, respectively. The results show that Sample B has more crystalline defects and smaller average diameter than Sample A. The cyclic voltammetry and electrochemical impedance spectroscopy measurements indicate that Sample B has better electrochemical performance than Sample A, such as better reaction reversibility, lower charge-transfer resistance and better cyclic stability. Proton diffusion coefficient of Sample B is 1.96×10-10cm2/s, which is two times as large as that （9.78×10-11cm2/s） of Sample A. The charge-discharge tests show that the discharge capacity （308 mA·h/g） of Sample B is 25 mA·h/g higher than that of Sample A （283 mA·h/g）.
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.
文摘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ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.10505001, No.10875055, No.10874234, and No.10703064） and the Educational Department of Liaoning Province （No.2008228）.
文摘Electronic structure and optical properties of neutral and charged low band gap alternating copolyfluorenes （Green 1, which is based on alternating repeating units consisting of alkyl-substituted fluorene and a thiophene-[1,2,5]thiadiazolo-[3,4]quinoxaline-thiophene （T-TDQ-T） unit were investigated theoretically with time-dependent density functional theory （TD-DFT） method, and their excited state properties were further analyzed with 2D site and 3D cube representations. For neutral Green 1, the band gap, binding energy, exciton binding energy, and nuclear relaxation energy were obtained. The transition dipole moments of neutral and charged Green 1 are compared using 3D transition density, which reveals the orientation and strength of transition dipole moments. The charge redistribution of neutral and charged Green 1 upon excitation are displayed and compared with 3D charge difference density. The electron-hole coherences of neutral and charged Green 1 upon excitation are investigated with 2D site representation （transition density matrix）. The excited state properties of neutral Green 1 calculated with TD-DFT method are compared with that calculated with ZINDO method, which reveals the importance of electron-electron interaction （in TD-DFT） in the excited state properties.
文摘Low optical absorption and photocorrosion are two crucial issues limiting the practical applications of zinc oxide(ZnO)-based photocatalysts.In this paper,we report the fabrication of graphitic-carbon-mediated ZnO nanorod arrays(NRAs)with enhanced photocatalytic activity and photostability for CO2 reduction under visible light irradiation.ZnO NRA/C-x(x=005,01,02,and 03)nanohybrids are prepared by calcining pre-synthesized ZnO NRAs with different amounts of glucose(0.05,0.1,0.2,and 0.3 g)as a carbon source via a hydrothermal method.X-ray photoelectron spectroscopy reveals that the obtained ZnO NRA/C-x nanohybrids are imparted with the effects of both carbon doping and carbon coating,as evidenced by the detected C-O-Zn bond and the C-C,C-O and C=O bonds,respectively.While the basic structure of ZnO remains unchanged,the UV-Vis absorption spectra show increased absorbance owing to the carbon doping effect in the ZnO NRA/C-x nanohybrids.The photoluminescence(PL)intensities of ZnO NRA/C-x nanohybrids are lower than that of bare ZnO NRA,indicating that the graphitic carbon layer coated on the surface of the ZnO NRA significantly enhances the charge carrier separation and transport,which in turn enhances the photoelectrochemical property and photocatalytic activity of the ZnO NRA/C-x nanohybrids for CO2 reduction.More importantly,a long-term reaction of photocatalytic CO2 reduction demonstrates that the photostability of ZnO NRA/C-x nanohybrids is significantly increased in comparison with the bare ZnO NRA.
基金supported by the National Natural Science Foundation of China (No.21673252, No.21333012, No.21672211, and No.21773252, No.21827803)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB12020200)
文摘The excited-state symmetry-breaking charge transfer (SBCT) dynamics in quadrupolar or octupolar molecules without clear infrared markers is usually hard to be tracked directly. In this work, on the basis of the evolution of instantaneous emission dipole moment obtained by femtosecond transient fluorescence spectroscopy, we presented a real-time characterization of the solvent-induced SBCT dynamics in an octupolar triphenylamine derivative. While the emission dipole moment of the octupolar trimer in weakly polar toluene changes little during the excited-state relaxation, it exhibits a fast reduction in a few picoseconds in strongly polar tetrahydrofuran. In comparison with the uorescence dynamics of dipolar monomer, we deduced that the emitting state of the octupolar trimer in strongly polar solvent, which undergoes solvent-induced structural uctuation, changes from exciton-coupled octupolar to excitation localized dipolar symmetry. In weakly polar solvent, the octupolar symmetry of the trimer is largely preserved during the solvation stabilization.
基金ACKN0WLEDGMENT This work was supported by the National Nature Science Foundation of China （No.10374040）.
文摘Metal-free indoline dyes for dye-sensitized solar cells were studied by employing quantum chemistry methods. Comparative study of the properties of both ground and excited states of metal-free indoline dyes for dye-sensitized solar cells revealed： （i） as the number of rhodanine rings increases, the energy difference between HOMO and LUMO decreases and there is a red shift in the absorption spectrum with the binding energy increased, and the transition dipole moment decreased; （ii） Based on an analysis of charge differential density, we observed that the charge and energy are transfered from the phenylethenyl to the indoline and rhodanine rings; （iii） The electron-hole coherences are mainly on the indoline and rhodanine rings, and the exciton sizes are 30 and 40 atoms for indoline dyes with one and two rhodanline rings, respectively. These results serve as a good example of computer-aided design in metal-free indoline dyes for dye-sensitized solar cells.
基金supported by Auburn UniversityIntramural Grants Program (AU-IGP)
文摘Low-cost, highly efficient catalysts for hydrogen evolution reaction(HER) are very important to advance energy economy based on clean hydrogen gas. Intensive studies on two-dimensional molybdenum disulfides(2 D Mo S2) have been conducted due to their remarkable catalytic properties.However, most of the reported syntheses are time consuming,complicated and less efficient. The present work demonstrates the production of Mo S2/graphene catalyst via an ultra-fast(60 s) microwave-initiated approach. High specific surface area and conductivity of graphene delivers a favorable conductive network for the growth of Mo S2 nanosheets, along with rapid charge transfer kinetics. As-produced Mo S2/graphene nanocomposites exhibit superior electrocatalytic activity for the HER in acidic medium, with a low onset potential of62 m V, high cathodic currents and a Tafel slope of43.3 m V/decade. Beyond excellent catalytic activity, Mo S2/graphene reveals long cycling stability with a very high cathodic current density of around 1000 m A cm^-2 at an overpotential of 250 m V. Moreover, the Mo S2/graphene-catalyst exhibits outstanding HER activities in a temperature range of 30 to 120°C with low activation energy of36.51 k J mol^-1, providing the opportunity of practical scalable processing.
基金supported by the National Natural Science Foundation of China (21064006, 21161018)the Natural Science Foundation of Gansu Province (1010RJZA018)the Program for Changjiang Scholars and Innovative Research Teams in Universities of the Ministry of Education of China (IRT1177)
文摘A non-sulfur chemosensor based on an easy to prepare double naphthalene Schiff base is reported for the colorimetric and fluorometric dual-channel sensing of Hg2+ ions by taking advantage of the twisted intramolecular charge transfer (TICT) mechanism. This work provides a novel approach for the selective recognition of mercury ions. Moreover, this sensor serves as a potential recyclable component in sensing materials and the complex L-Hg2+ (L = 1-[(2-naphthalenylimino)methyl]-2-naphthalenol) can therefore be used as a fluorescent sensor for iodine anions. Notably, the color changes are very significant and all the recognition and recycling processes can be observed by the naked eye.
基金supported by the National Natural Science Foundation of China (21201121, 21271128)the National Basic Research Program of China (2011CB808703)
文摘A series of Eu3+ -incorporated ETS-10 samples were successfully prepared based on the traditional ion exchange method. The relationship between photogenerated charge behaviors and luminescent properties has been investigated in detail. It has been demonstrated that as a result of the charge transfer from the titanate quantum wires to Eu3+ crystal field states, the host matrix ETS-10 functions as the sensitizer of Eu3+ to enhance the red luminescence, while Eu3+ cations contribute to the recombination of photogenerated charges. The behavior of photogenerated charges has significant impact on the luminescent properties of Eu3+ -incorporated ETS-10 materials.
基金the National Natural Science Foundation of China(21590792,91426302,and 21433005)Guangdong Provincial Key Laboratory of Catalysis(2020B121201002)+1 种基金the National Science Basic Research Program of Shaanxi Province(2019JM-226)the financial and technical support from the Research Center for Advanced Materials Science(RCAMS)at King Khalid University through the Grant(RCAMS/KKU/014-20)。
文摘MXene is a variety of new two-dimensional(2D)materials with early transition metal carbides,nitrides,and carbonitrides.Quantum chemical studies have been carried out on the geometries,electronic structures,stability and catalytic properties of a non-noble metal single-atom catalyst(SAC)with single Co atom anchored on MXene materials of Mo_(2)CS_(2).The Co adatom anchored on top of the Mo atom of this MXene is found to be rather stable,and this SAC is appropriate for CO oxidation.The charge transfers from the surface to the adsorbed CO and O2 play a significant role in the activation of these molecules on Co_(1)/Mo_(2)CS_(2).With this catalyst,the Eley-Rideal(ER),Langmuir-Hinshelwood(LH),and Termolecular Eley-Rideal(TER)mechanisms are explored for CO oxidation.We find that,while all the three mechanisms are feasible at low temperature,Co_(1)/Mo_(2)CS_(2) possesses higher catalytic activity for CO oxidation through the TER mechanism that features an intriguing OC(OO)CO intermediate(IM)adsorbed on Co single atom.The calculated activation energy barriers of the rate-limiting step are 0.67 eV(TER),0.78 eV(LH)and 0.88 eV(ER),respectively.The present study illustrates that it is promising to develop and design low-cost,non-noble metal SACs using MXene types of 2D materials.
基金supported by the National Natural Science Foundation of China(21336005,21371128)the major research project of Jiangsu Province Office of Education(15KJA150008)
文摘In this paper,poly(pyridine-imide)s,PI-Ph and PI-Naphth,were successfully synthesised and fabricated for use as memory devices.The Al/PI-Ph/indium tin oxide(ITO)device showed dynamic random access memory characteristics,whereas Al/PI-Naphth/ITO showed rewritable(FLASH)memory characteristics.Characterisation of their UV,cyclic voltammograms,and density functional theory,were used to illustrate the different memory behaviours.The results show that the stability of electric-field-induced-charge-transfer complexes can affect memory performance.
基金financially supported by the National Natural Science Foundation of China (21173230)MOST (2011CE93202)
文摘Molecular-based conducting magnet or magnetic conductor, is an overlap of organic conductor and molecular magnet. Due to the existence of ferromagnetism, antiferromagnetism and quantum magnetism in insulated charge-transfer salt, it becomes a common sense that magnetism is not good for conductivity. After the discovery of first molecular-based metallic ferromagnet, molecular-based conducting magnet with n-unit from organic conductor and magnetism from coordination counterion became a hot area. The metallic ferromagnet, semiconductor room-temperature ferrimagnet, metallic weak ferromagnet and supercon- ducting antiferromagnet have been discovered. The new molecular-based conducting magnet with higher conductivity and higher magnetic ordering temperature is expected.
基金supported by AcRF Tier 1(RG 8/16,RG 133/14 and RG 13/15)from MOE,SingaporeSTU Scientific Research Foundation for Talents(NTF15005)+1 种基金STU Youth Research Fund(YR15001)the Foundation for Young Talents in Higher Education of Guangdong(2015KQNCX042)
文摘This article summarized the recent advance on the structural design and synthetic strategies of intramolec- ular charge-transfer compounds as well as their potential ap- plications in two-photon absorption chromophores, organic photovoltaics and organic light-emitting diodes.
基金financially supported by the National Natural Science Foundation of China (61376011, 51402141 and 61604086)Gansu Provincial Natural Science Foundation (17JR5RA198)+2 种基金the Fundamental Research Funds for the Central Universities (LZUJBKY-2018-119 and LZUJBKY-2018-CT08)Shenzhen Science and Technology Innovation Committee (JCYJ20170818155813437)the Key Areas Scientific and Technological Research Projects in Xinjiang Production and Construction Corps (2018AB004)
文摘Light absorption plays an important role in improving the power conversion efficiency(PCE)of quantum dot-sensitized solar cells(QDSSCs).In this study,a multifunctional long-persistence phosphor(LPP)layer was introduced into the CdS/CdSe QDSSCs via a simple doctor blade method.The LPP layer can simultaneously improve the light harvesting and photo charge transfer in CdS/CdSe QDSSCs.As a result,their short-circuit current and corresponding PCE are effectively enhanced.The PCE can reach up to 5.07%,which is about 24%larger than that of the conventional CdS/CdSe QDSSCs without LPP layer.The solar cells can work in dark for a while due to the long-lasting fluorescence of the LPP layer.This research provides an effective way to improve the PCE of QDSSCs,and finds the possibility for all-weather QDSSCs.
基金supported by the National Natural Science Foundation of China(20721061,51033006,51003107,91027043)the China-Denmark Co-project,TRR61(NSFC-DFG Transregio Project)the National Basic Research Program of China(2011CB808400,2011CB932300,2009CB930400)and Chinese Academy of Sciences
文摘The organic single-crystal field-effect transistors using anthracene derivative, H-Ant as an active layer with source/drain electrodes decorated by metal charge transfer salt(Cu TCNQ) were fabricated. We demonstrated that this bottom-contact structure displayed an obvious improvement in the electrical characteristics relative to their pristine copper and top-contact gold electrode counterparts. This observation could be ascribed to the lower contact resistance resulting from the energetic match between electrodes and semiconductor.
基金supported by the National Basic Research Program of China(2015CB921102 and 2019YFA0308403)the National Natural Science Foundation of China(11674028 and11822407)+1 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(XDB28000000)China Postdoctoral Science Foundation(2020M670011)。
文摘Though several theoretical models have been proposed to design electronic flat-bands, the definite experimental realization in two-dimensional atomic crystal is still lacking. Here we propose a novel and realistic flat-band model based on threefold degenerate p-orbitals in two-dimensional ionic materials. Our theoretical analysis and first-principles calculations show that the proposed flat-band can be realized in 1 T layered materials of alkali-metal chalogenides and metal-carbon group compounds. Some of the former are theoretically predicted to be stable as layered materials(e.g., K2 S), and some of the latter have been experimentally fabricated in previous works(e.g., Gd2 CCl2). More interestingly, the flat-band is partially filled in the heterostructure of a K2 S monolayer and graphene layers. The spin polarized nearly flatband can be realized in the ferromagnetic state of a Gd2 CCl2 monolayer, which has been fabricated in experiments. Our theoretical model together with the material predictions provide a realistic platform for the study of flat-bands and related exotic quantum phases.
