Semiconductor quantum dots are promising candidates for preparing high-performance single photon sources.A basic requirement for this application is realizing the controlled growth of high-quality semiconductor quantu...Semiconductor quantum dots are promising candidates for preparing high-performance single photon sources.A basic requirement for this application is realizing the controlled growth of high-quality semiconductor quantum dots.Here,we report the growth of embedded GaAs_(1−x)Sb_(x) quantum dots in GaAs nanowires by molecular-beam epitaxy.It is found that the size of the GaAs_(1−x)Sb_(x) quantum dot can be well-defined by the GaAs nanowire.Energy dispersive spectroscopy analyses show that the antimony content x can be up to 0.36 by tuning the growth temperature.All GaAs_(1−x)Sb_(x) quantum dots exhibit a pure zinc-blende phase.In addition,we have developed a new technology to grow GaAs passivation layers on the sidewalls of the GaAs_(1−x)Sb_(x) quantum dots.Different from the traditional growth process of the passivation layer,GaAs passivation layers can be grown simultaneously with the growth of the embedded GaAs_(1−x)Sb_(x) quantum dots.The spontaneous GaAs passivation layer shows a pure zinc-blende phase due to the strict epitaxial relationship between the quantum dot and the passivation layer.The successful fabrication of embedded high-quality GaAs_(1−x)Sb_(x) quantum dots lays the foundation for the realization of GaAs_(1−x)Sb_(x)-based single photon sources.展开更多
Z-scheme semiconductors are a promising class of photocatalysts for hydrogen generation.In this work,Z-scheme semiconductors composed of WO3-x quantum dots supported on TiO2（WO3-xQDS/TiO2） were fabricated by solvoth...Z-scheme semiconductors are a promising class of photocatalysts for hydrogen generation.In this work,Z-scheme semiconductors composed of WO3-x quantum dots supported on TiO2（WO3-xQDS/TiO2） were fabricated by solvothermal and hydrogen-reduction methods.Characterization by transmission electron microscopy and X-ray diffraction indicated that the amount and size of the WO3-x QDs could be tuned by modulating the addition of the W precursor.Evidence from X-ray photoelectron spectroscopy and photoluminescence spectroscopy suggested that the hydrogen reduction of the composite induced the formation of oxygen vacancy（W^5＋/Vo） defects in WO3.These defects led to ohmic contact between WO3-x and TiO2,which altered the charge-transfer pathway from type Ⅱ heterojunction to Z-scheme,and maintained the highly reductive and oxidative ability of TiO2 and WO3-x,respectively.Therefore,the Z-scheme sample showed 1.3-fold higher photoactivity than pure TiO2 in hydrogen generation.These results suggest that the formation of W^5＋/Vo defects at the interface is highly beneficial for the fabrication of Z-scheme photocatalysts.展开更多
Oxidized nanoporous g-C3N4(PCNO)decorated with graphene oxide quantum dots(ox-GQDs)was successfully prepared by a facile self-assembly method.As co-catalysts,the ultrasmall zero-dimensional(0 D)ox-GQDs can achieve uni...Oxidized nanoporous g-C3N4(PCNO)decorated with graphene oxide quantum dots(ox-GQDs)was successfully prepared by a facile self-assembly method.As co-catalysts,the ultrasmall zero-dimensional(0 D)ox-GQDs can achieve uniform dispersion on the surface/inner channels of PCNO,as well as intimate contact with PCNO through hydrogen bonding,π-π,and chemical bonding interactions.In contrast with PCNO,the ox-GQDs/PCNO composite photocatalysts possessed improved light-harvesting ability,higher charge-transfer efficiency,enhanced photooxidation capacity,and increased amounts of reactive species due to the upconversion properties,strong electron capturing ability,and peroxidase-like activity of the ox-GQDs.Therefore,the visible-light photocatalytic degradation and disinfection performances of the ox-GQDs/PCNO composite were significantly enhanced.Remarkably,the composite with a 0.2 wt.% deposited amount of ox-GQDs(ox-GQDs-0.2%/PCNO)exhibited optimum amaranth photodegradation activity,with a corresponding rate about 3.1 times as high as that of PCNO.In addition,ox-GQDs-0.2%/PCNO could inactivate about 99.6%of Escherichia coli(E.coli)cells after 4 h of visible light irradiation,whereas only^31.9% of E.coli cells were killed by PCNO.Furthermore,h+,·O2-,and·OH were determined to be the reactive species generated in the photocatalytic process of the ox-GQDs/PCNO system;these species can thoroughly mineralize azo dyes and effectively inactivate pathogenic bacteria.展开更多
Energy band structure and interfacial compatibility of heterojunctions are crucial for photocatalysts in promoting photogene rated charge separation and transfer.Here,a combined strategy of vacancy engineering and qua...Energy band structure and interfacial compatibility of heterojunctions are crucial for photocatalysts in promoting photogene rated charge separation and transfer.Here,a combined strategy of vacancy engineering and quantum effect via a facile phosphating process is reported,for the first time,to modulate the energy band structure and the interface of Zn_(x)Cd_(1-x)S/CoP quantum dots(ZCS_(v)/CoP QDs)heterojunction.The combined experimental and theoretical investigation revealed that phosphating process transformed CoO_(x) QDs to CoP QDs,and more importantly,generated considerable amount of sulfur vacancies in ZCS_(v).As a result,a TypeⅡZCS_(v)/CoP QDs heterojunction with compatible interfaces was constructed via in-situ generated P-Zn,P-Cd and S-Co bonds,which facilitated the separation and transfer of the photogenerated charge and thus resulted in a high ability towards hydrogen evolution under visible light(17.53 mmol g^(-1) h^(-1)).This work provides an effective and adaptable strategy to modulate band structure and interfacial compatibility of heterojunctions via vacancy engineering and quantum effect.展开更多
We investigate the nonlinear optical rectification(NOR) of spherical quantum dots(QDs) under Hulthén plus Hellmann confining potential with the external tuning elements. Energy and wavefunction are determined by ...We investigate the nonlinear optical rectification(NOR) of spherical quantum dots(QDs) under Hulthén plus Hellmann confining potential with the external tuning elements. Energy and wavefunction are determined by using the Nikiforov–Uvarov method. Expression for the NOR coefficient is derived by the density matrix theory. The results show that the applied external elements and internal parameters of this system have a strong influence on intraband nonlinear optical properties. It is hopeful that this tuning of the nonlinear optical properties of GaAs/Ga_(1-x)Al_(x)As QDs can make a greater contribution to preparation of new functional optical devices.展开更多
The effects of indium composition in InGaAs interlayer and on optical properties of GaSb/InGaAs QD material on morphology of GaSb/InGaAs quantum dots （QDs） system are studied. AFM images show that the change of the ...The effects of indium composition in InGaAs interlayer and on optical properties of GaSb/InGaAs QD material on morphology of GaSb/InGaAs quantum dots （QDs） system are studied. AFM images show that the change of the indium composition in InGaAs interlayer can alter the GaSb QD morphology. It is found that low indium composition in InGaAs interlayer can promote the formation of QDs, while high indium composition can inhibit the formation of QDs. The photoluminescence （PL） spectra of GaSb/InGaAs QDs at 8 K under low excitation power indicate that the third root of the excitation power is linear with the peak position, which provides a direct evidence for their luminescence belonging to type-Ⅱ material optical transition. The PL spectra at 8 K under an excitation power of 90row show that the optical properties of GaSb/InGaAs QD material system can be affected by the indium composition in the InGaAs interlayer, and the PL peak position is linear with the indium composition. The optical properties of GaSb/InGaAs QDs can be improved by adjusting the indium composition in the InGaAs interlayer.展开更多
A novel flash memory cell with stacked structure （Si substrate/SiGe quantum dots/tunneling oxide/polySi floating gate） is proposed and demonstrated to achieve enhanced F-N tunneling for both programming and erasing....A novel flash memory cell with stacked structure （Si substrate/SiGe quantum dots/tunneling oxide/polySi floating gate） is proposed and demonstrated to achieve enhanced F-N tunneling for both programming and erasing. Simulation results indicate the new structure provides high speed and reliability. Experimental results show that the operation voltage can be as much as 4V less than that of conventional full F-N tunneling NAND memory cells. Memory cells with the proposed structure can achieve higher speed, lower voltage, and higher reliability.展开更多
Photocatalytic water splitting is a promising method for hydrogen production.Numerous efficient photocatalysts have been synthesized and utilized.However,photocatalysts without a noble metal as the co-catalyst have be...Photocatalytic water splitting is a promising method for hydrogen production.Numerous efficient photocatalysts have been synthesized and utilized.However,photocatalysts without a noble metal as the co-catalyst have been rarely reported.Herein,a CoP co-catalyst-modified graphitic-C3N4(g-C3N4/CoP)is investigated for photocatalytic water splitting to produce H2.The g-C3N4/CoP composite is synthesized in two steps.The first step is related to thermal decomposition,and the second step involves an electroless plating technique.The photocatalytic activity for hydrogen evolution reactions of g-C3N4 is distinctly increased by loading the appropriate amount of CoP quantum dots(QDs).Among the as-synthesized samples,the optimized one(g-C3N4/CoP-4%)shows exceptional photocatalytic activity as compared with pristine g-C3N4,generating H2 at a rate of 936μmol g^-1 h^-1,even higher than that of g-C3N4 with 4 wt%Pt(665μmol g^-1 h^-1).The UV-visible and optical absorption behavior confirms that g-C3N4 has an absorption edge at 451 nm,but after being composited with CoP,g-C3N4/CoP-4%has an absorption edge at 497 nm.Furthermore,photoluminescence and photocurrent measurements confirm that loading CoP QDs to pristine g-C3N4 not only enhances the charge separation,but also improves the transfer of photogenerated e--h+pairs,thus improving the photocatalytic performance of the catalyst to generate H2.This work demonstrates a feasible strategy for the synthesis of highly efficient metal phosphide-loaded g-C3N4 for hydrogen generation.展开更多
Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples w...Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.展开更多
Graphite‐like carbon nitride(g‐C3N4)‐based compounds have attracted considerable attention because of their excellent photocatalytic performance.In this work,a novel direct Z‐scheme system constructed from two‐di...Graphite‐like carbon nitride(g‐C3N4)‐based compounds have attracted considerable attention because of their excellent photocatalytic performance.In this work,a novel direct Z‐scheme system constructed from two‐dimensional(2D)g‐C3N4nanoplates and zero‐dimensional(0D)MoS2quantum dots(QDs)was prepared through the combination of a hydrothermal process and microemulsion preparation.The morphologies,structures,and optical properties of the as‐prepared photocatalysts were characterized by X‐ray diffraction,X‐ray photoelectron spectroscopy,atomic force microscopy,transmission electron microscopy,and UV‐vis diffuse reflectance spectroscopy.In addition,the photocatalytic performances of the prepared2D/0D hybrid composites were evaluated based on the photodegradation of rhodamine B under visible‐light irradiation.The results demonstrated that the introduction of MoS2QDs to g‐C3N4greatly enhanced the photocatalytic efficiency.For the optimum7%MoS2QD/g‐C3N4photocatalyst,the degradation rate constant was8.8times greater than that of pure g‐C3N4under visible‐light irradiation.Photocurrent and electrochemical impedance spectroscopy results further demonstrated that the MoS2QD/g‐C3N4composites exhibited higher photocurrent density and lower chargetransfer resistance than those of the pure g‐C3N4or MoS2QDs.Active species trapping,terephthalic acid photoluminescence,and nitro blue tetrazolium transformation experiments were performed to investigate the evolution of reactive oxygen species,including hydroxyl radicals and superoxide radicals.The possible enhanced photocatalytic mechanism was attributed to a direct Z‐scheme system,which not only can increase the separation efficiency of photogenerated electron‐hole pairs but also possesses excellent oxidation and reduction ability for high photocatalytic performances.This work provides an effective synthesis approach and insight to help develop other C3N4‐based direct Z‐scheme photocatalytic systems for environmental purification and energy conversion.展开更多
According to the well-established light-to-electricity conversion theory,resonant excited carriers in the quantum dots will relax to the ground states and cannot escape from the quantum dots to form photocurrent,which...According to the well-established light-to-electricity conversion theory,resonant excited carriers in the quantum dots will relax to the ground states and cannot escape from the quantum dots to form photocurrent,which have been observed in quantum dots without a p–n junction at an external bias.Here,we experimentally observed more than 88% of the resonantly excited photo carriers escaping from In As quantum dots embedded in a short-circuited p–n junction to form photocurrent.The phenomenon cannot be explained by thermionic emission,tunneling process,and intermediate-band theories.A new mechanism is suggested that the photo carriers escape directly from the quantum dots to form photocurrent rather than relax to the ground state of quantum dots induced by a p–n junction.The finding is important for understanding the low-dimensional semiconductor physics and applications in solar cells and photodiode detectors.展开更多
We report on fabrication and photovoltaic characteristics of InxGa1-xN/GaN multiple quantum well solar cells with different indium compositions and barrier thicknesses. The as-grown samples are characterized by high- ...We report on fabrication and photovoltaic characteristics of InxGa1-xN/GaN multiple quantum well solar cells with different indium compositions and barrier thicknesses. The as-grown samples are characterized by high- resolution x-ray diffraction and reciprocal space mapping. The results show that the sample with a thick barrier thickness （lO.Onm） and high indium composition （0.23） has better crystalline quality. In addition, the dark current density-voltage （J-V） measurement of this device shows a significant decrease of leakage current, which leads to high open-circuit voltage Vow. Through the J-V characteristics under an Air Mass 1.5 Global （AM 1.5 G） illumination, this device exhibits a Voc of 1.89 V, a short-circuit current density Ysc of 3.92mA/cm2 and a fill factor of 50.96%. As a result, the conversion efficiency （77） is enhanced to be 3.77% in comparison with other devices.展开更多
Metallic Sn has provoked tremendous progress as an anode material for sodium-ion batteries(SIBs).However,Sn anodes suffer from a dramatic capacity fading,owing to pulverization induced by drastic volume expansion duri...Metallic Sn has provoked tremendous progress as an anode material for sodium-ion batteries(SIBs).However,Sn anodes suffer from a dramatic capacity fading,owing to pulverization induced by drastic volume expansion during cycling.Herein,a flexible three-dimensional(3D)hierarchical conductive network electrode is designed by constructing Sn quantum dots(QDs)encapsulated in one-dimensional N,S codoped carbon nanofibers(NS-CNFs)sheathed within two-dimensional(2D)reduced graphene oxide(rGO)scrolls.In this ingenious strategy,1D NS-CNFs are regarded as building blocks to prevent the aggregation and pulverization of Sn QDs during sodiation/desodiation,2D rGO acts as electrical roads and“bridges”among NS-CNFs to improve the conductivity of the electrode and enlarge the contact area with electrolyte.Because of the unique structural merits,the flexible 3D hierarchical conductive network was directly used as binder-and current collectorfree anode for SIBs,exhibiting ultra-long cycling life(373 mAh g?1 after 5000 cycles at 1 A g?1),and excellent high-rate capability(189 mAh g?1 at 10 A g?1).This work provides a facile and efficient engineering method to construct 3D hierarchical conductive electrodes for other flexible energy storage devices.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.12374459)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB0460000)support from Youth Innovation Promotion Association,Chinese Academy of Sciences(Grant Nos.2017156 and Y2021043).
文摘Semiconductor quantum dots are promising candidates for preparing high-performance single photon sources.A basic requirement for this application is realizing the controlled growth of high-quality semiconductor quantum dots.Here,we report the growth of embedded GaAs_(1−x)Sb_(x) quantum dots in GaAs nanowires by molecular-beam epitaxy.It is found that the size of the GaAs_(1−x)Sb_(x) quantum dot can be well-defined by the GaAs nanowire.Energy dispersive spectroscopy analyses show that the antimony content x can be up to 0.36 by tuning the growth temperature.All GaAs_(1−x)Sb_(x) quantum dots exhibit a pure zinc-blende phase.In addition,we have developed a new technology to grow GaAs passivation layers on the sidewalls of the GaAs_(1−x)Sb_(x) quantum dots.Different from the traditional growth process of the passivation layer,GaAs passivation layers can be grown simultaneously with the growth of the embedded GaAs_(1−x)Sb_(x) quantum dots.The spontaneous GaAs passivation layer shows a pure zinc-blende phase due to the strict epitaxial relationship between the quantum dot and the passivation layer.The successful fabrication of embedded high-quality GaAs_(1−x)Sb_(x) quantum dots lays the foundation for the realization of GaAs_(1−x)Sb_(x)-based single photon sources.
基金supported by the National Natural Science Foundation of China (21506156, 21676193)the Tianjin Municipal Natural Science Foundation (15JCZDJC37300, 16JCQNJC05200)~~
文摘Z-scheme semiconductors are a promising class of photocatalysts for hydrogen generation.In this work,Z-scheme semiconductors composed of WO3-x quantum dots supported on TiO2（WO3-xQDS/TiO2） were fabricated by solvothermal and hydrogen-reduction methods.Characterization by transmission electron microscopy and X-ray diffraction indicated that the amount and size of the WO3-x QDs could be tuned by modulating the addition of the W precursor.Evidence from X-ray photoelectron spectroscopy and photoluminescence spectroscopy suggested that the hydrogen reduction of the composite induced the formation of oxygen vacancy（W^5＋/Vo） defects in WO3.These defects led to ohmic contact between WO3-x and TiO2,which altered the charge-transfer pathway from type Ⅱ heterojunction to Z-scheme,and maintained the highly reductive and oxidative ability of TiO2 and WO3-x,respectively.Therefore,the Z-scheme sample showed 1.3-fold higher photoactivity than pure TiO2 in hydrogen generation.These results suggest that the formation of W^5＋/Vo defects at the interface is highly beneficial for the fabrication of Z-scheme photocatalysts.
基金supported by the National Natural Science Foundation of China(21707052)Jiangsu Agriculture Science and Technology Innovation Fund(CX(18)2025)+1 种基金Fundamental Research Funds for the Central Universities(JUSRP11905 and JUSRP51714B)Key Research and Development Program of Jiangsu Province(BE2017623)~~
文摘Oxidized nanoporous g-C3N4(PCNO)decorated with graphene oxide quantum dots(ox-GQDs)was successfully prepared by a facile self-assembly method.As co-catalysts,the ultrasmall zero-dimensional(0 D)ox-GQDs can achieve uniform dispersion on the surface/inner channels of PCNO,as well as intimate contact with PCNO through hydrogen bonding,π-π,and chemical bonding interactions.In contrast with PCNO,the ox-GQDs/PCNO composite photocatalysts possessed improved light-harvesting ability,higher charge-transfer efficiency,enhanced photooxidation capacity,and increased amounts of reactive species due to the upconversion properties,strong electron capturing ability,and peroxidase-like activity of the ox-GQDs.Therefore,the visible-light photocatalytic degradation and disinfection performances of the ox-GQDs/PCNO composite were significantly enhanced.Remarkably,the composite with a 0.2 wt.% deposited amount of ox-GQDs(ox-GQDs-0.2%/PCNO)exhibited optimum amaranth photodegradation activity,with a corresponding rate about 3.1 times as high as that of PCNO.In addition,ox-GQDs-0.2%/PCNO could inactivate about 99.6%of Escherichia coli(E.coli)cells after 4 h of visible light irradiation,whereas only^31.9% of E.coli cells were killed by PCNO.Furthermore,h+,·O2-,and·OH were determined to be the reactive species generated in the photocatalytic process of the ox-GQDs/PCNO system;these species can thoroughly mineralize azo dyes and effectively inactivate pathogenic bacteria.
基金financially supported by the Taishan Scholar Program of Shandong Province(ts201712046)the Key Research and Development Programme of Shandong Province(2019JZZY010905)+2 种基金the Natural Science Foundation of Shandong Province(ZR2020QB132)the Liaoning BaiQianWan Talents Programthe Royal Society and the Newton Fund(NAF\R1\191294)。
文摘Energy band structure and interfacial compatibility of heterojunctions are crucial for photocatalysts in promoting photogene rated charge separation and transfer.Here,a combined strategy of vacancy engineering and quantum effect via a facile phosphating process is reported,for the first time,to modulate the energy band structure and the interface of Zn_(x)Cd_(1-x)S/CoP quantum dots(ZCS_(v)/CoP QDs)heterojunction.The combined experimental and theoretical investigation revealed that phosphating process transformed CoO_(x) QDs to CoP QDs,and more importantly,generated considerable amount of sulfur vacancies in ZCS_(v).As a result,a TypeⅡZCS_(v)/CoP QDs heterojunction with compatible interfaces was constructed via in-situ generated P-Zn,P-Cd and S-Co bonds,which facilitated the separation and transfer of the photogenerated charge and thus resulted in a high ability towards hydrogen evolution under visible light(17.53 mmol g^(-1) h^(-1)).This work provides an effective and adaptable strategy to modulate band structure and interfacial compatibility of heterojunctions via vacancy engineering and quantum effect.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.51702003,61775087,11674312,52174161,and 12174161)。
文摘We investigate the nonlinear optical rectification(NOR) of spherical quantum dots(QDs) under Hulthén plus Hellmann confining potential with the external tuning elements. Energy and wavefunction are determined by using the Nikiforov–Uvarov method. Expression for the NOR coefficient is derived by the density matrix theory. The results show that the applied external elements and internal parameters of this system have a strong influence on intraband nonlinear optical properties. It is hopeful that this tuning of the nonlinear optical properties of GaAs/Ga_(1-x)Al_(x)As QDs can make a greater contribution to preparation of new functional optical devices.
基金Supported by the Science and Technology Planning Projects of Guangdong Province under Grant Nos 2014B050505020,2015B010114007 and 2014B090904045the Research Fund for the Doctoral Program of Higher Education of China under Grant No 20134407110008+1 种基金the Guangzhou Science and Technology Project of Guangdong Province under Grant No 2016201604030027the Zhongshan Science and Technology Project of Guangdong Province under Grant No 2013B3FC0003
文摘The effects of indium composition in InGaAs interlayer and on optical properties of GaSb/InGaAs QD material on morphology of GaSb/InGaAs quantum dots （QDs） system are studied. AFM images show that the change of the indium composition in InGaAs interlayer can alter the GaSb QD morphology. It is found that low indium composition in InGaAs interlayer can promote the formation of QDs, while high indium composition can inhibit the formation of QDs. The photoluminescence （PL） spectra of GaSb/InGaAs QDs at 8 K under low excitation power indicate that the third root of the excitation power is linear with the peak position, which provides a direct evidence for their luminescence belonging to type-Ⅱ material optical transition. The PL spectra at 8 K under an excitation power of 90row show that the optical properties of GaSb/InGaAs QD material system can be affected by the indium composition in the InGaAs interlayer, and the PL peak position is linear with the indium composition. The optical properties of GaSb/InGaAs QDs can be improved by adjusting the indium composition in the InGaAs interlayer.
文摘A novel flash memory cell with stacked structure （Si substrate/SiGe quantum dots/tunneling oxide/polySi floating gate） is proposed and demonstrated to achieve enhanced F-N tunneling for both programming and erasing. Simulation results indicate the new structure provides high speed and reliability. Experimental results show that the operation voltage can be as much as 4V less than that of conventional full F-N tunneling NAND memory cells. Memory cells with the proposed structure can achieve higher speed, lower voltage, and higher reliability.
基金supported by the National Natural Science Foundation of China(51602207)the Doctoral Scientific Research Foundation of Liaoning Province(20170520011)+3 种基金the Program for Liaoning Excellent Talents in Universities(LR2017074)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(SKLPEE-201810)Fuzhou University,the Scientific Research Project of the Educational Department of Liaoning Province(LQN201712)Shenyang Excellent Talents in Universities(RC180211)~~
文摘Photocatalytic water splitting is a promising method for hydrogen production.Numerous efficient photocatalysts have been synthesized and utilized.However,photocatalysts without a noble metal as the co-catalyst have been rarely reported.Herein,a CoP co-catalyst-modified graphitic-C3N4(g-C3N4/CoP)is investigated for photocatalytic water splitting to produce H2.The g-C3N4/CoP composite is synthesized in two steps.The first step is related to thermal decomposition,and the second step involves an electroless plating technique.The photocatalytic activity for hydrogen evolution reactions of g-C3N4 is distinctly increased by loading the appropriate amount of CoP quantum dots(QDs).Among the as-synthesized samples,the optimized one(g-C3N4/CoP-4%)shows exceptional photocatalytic activity as compared with pristine g-C3N4,generating H2 at a rate of 936μmol g^-1 h^-1,even higher than that of g-C3N4 with 4 wt%Pt(665μmol g^-1 h^-1).The UV-visible and optical absorption behavior confirms that g-C3N4 has an absorption edge at 451 nm,but after being composited with CoP,g-C3N4/CoP-4%has an absorption edge at 497 nm.Furthermore,photoluminescence and photocurrent measurements confirm that loading CoP QDs to pristine g-C3N4 not only enhances the charge separation,but also improves the transfer of photogenerated e--h+pairs,thus improving the photocatalytic performance of the catalyst to generate H2.This work demonstrates a feasible strategy for the synthesis of highly efficient metal phosphide-loaded g-C3N4 for hydrogen generation.
文摘Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.
基金supported by National Natural Science Foundation of China(51672113)Six Talent Peaks Project in Jiangsu Province(2015-XCL-026)+3 种基金Natural Science Foundation of Jiangsu Province(BK20171299)State Key Laboratory of Photocatalysis on Energy and Environment(SKLPEE-KF201705),Fuzhou UniversityState Key Laboratory of Advanced Technology for Materials Synthesis and Processing(2016-KF-10),Wuhan University of Technologythe Qing Lan Project Foundation of Jiangsu Province~~
文摘Graphite‐like carbon nitride(g‐C3N4)‐based compounds have attracted considerable attention because of their excellent photocatalytic performance.In this work,a novel direct Z‐scheme system constructed from two‐dimensional(2D)g‐C3N4nanoplates and zero‐dimensional(0D)MoS2quantum dots(QDs)was prepared through the combination of a hydrothermal process and microemulsion preparation.The morphologies,structures,and optical properties of the as‐prepared photocatalysts were characterized by X‐ray diffraction,X‐ray photoelectron spectroscopy,atomic force microscopy,transmission electron microscopy,and UV‐vis diffuse reflectance spectroscopy.In addition,the photocatalytic performances of the prepared2D/0D hybrid composites were evaluated based on the photodegradation of rhodamine B under visible‐light irradiation.The results demonstrated that the introduction of MoS2QDs to g‐C3N4greatly enhanced the photocatalytic efficiency.For the optimum7%MoS2QD/g‐C3N4photocatalyst,the degradation rate constant was8.8times greater than that of pure g‐C3N4under visible‐light irradiation.Photocurrent and electrochemical impedance spectroscopy results further demonstrated that the MoS2QD/g‐C3N4composites exhibited higher photocurrent density and lower chargetransfer resistance than those of the pure g‐C3N4or MoS2QDs.Active species trapping,terephthalic acid photoluminescence,and nitro blue tetrazolium transformation experiments were performed to investigate the evolution of reactive oxygen species,including hydroxyl radicals and superoxide radicals.The possible enhanced photocatalytic mechanism was attributed to a direct Z‐scheme system,which not only can increase the separation efficiency of photogenerated electron‐hole pairs but also possesses excellent oxidation and reduction ability for high photocatalytic performances.This work provides an effective synthesis approach and insight to help develop other C3N4‐based direct Z‐scheme photocatalytic systems for environmental purification and energy conversion.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11574362,61210014,11374340,and 11474205)the Innovative Clean-Energy Research and Application Program of Beijing Municipal Science and Technology Commission,China(Grant No.Z151100003515001)
文摘According to the well-established light-to-electricity conversion theory,resonant excited carriers in the quantum dots will relax to the ground states and cannot escape from the quantum dots to form photocurrent,which have been observed in quantum dots without a p–n junction at an external bias.Here,we experimentally observed more than 88% of the resonantly excited photo carriers escaping from In As quantum dots embedded in a short-circuited p–n junction to form photocurrent.The phenomenon cannot be explained by thermionic emission,tunneling process,and intermediate-band theories.A new mechanism is suggested that the photo carriers escape directly from the quantum dots to form photocurrent rather than relax to the ground state of quantum dots induced by a p–n junction.The finding is important for understanding the low-dimensional semiconductor physics and applications in solar cells and photodiode detectors.
基金Supported by the National Basic Research Program of China(No 2012CB619303)the National High-Technology Research and Development Program of China(No 2011AA050514)
文摘We report on fabrication and photovoltaic characteristics of InxGa1-xN/GaN multiple quantum well solar cells with different indium compositions and barrier thicknesses. The as-grown samples are characterized by high- resolution x-ray diffraction and reciprocal space mapping. The results show that the sample with a thick barrier thickness （lO.Onm） and high indium composition （0.23） has better crystalline quality. In addition, the dark current density-voltage （J-V） measurement of this device shows a significant decrease of leakage current, which leads to high open-circuit voltage Vow. Through the J-V characteristics under an Air Mass 1.5 Global （AM 1.5 G） illumination, this device exhibits a Voc of 1.89 V, a short-circuit current density Ysc of 3.92mA/cm2 and a fill factor of 50.96%. As a result, the conversion efficiency （77） is enhanced to be 3.77% in comparison with other devices.
基金Acknowledgements This work was supported by Key Project of Chinese National Programs for Fundamental Research and Development（Grant No. 2010CB631002）, National Natural Science Foundation of China （Grant No. 50771078, 50901057） and Xi＇ an Applied Materials Innovation Fund （XA-AM- 200904） . The authors thank Guo S W and Li Y H for their help with the HRTEM operation.
基金financially supported by the Natural Science Foundation of Shandong Province,China(ZR2018JL021,ZR2014EMQ011)the Applied Basic Research Foundation of Qingdao City(17-1-1-84-jch)+2 种基金the National Natural Science Foundation of China(51402160)supported by Taishan Scholar Program of Shandong Province,China,and National Demonstration Center for Experimental Applied Physics Education(Qingdao University)support from the China Postdoctoral Science Foundation Funded Project(2018M630747)and Qingdao Postdoctoral Applied Research Project.
文摘Metallic Sn has provoked tremendous progress as an anode material for sodium-ion batteries(SIBs).However,Sn anodes suffer from a dramatic capacity fading,owing to pulverization induced by drastic volume expansion during cycling.Herein,a flexible three-dimensional(3D)hierarchical conductive network electrode is designed by constructing Sn quantum dots(QDs)encapsulated in one-dimensional N,S codoped carbon nanofibers(NS-CNFs)sheathed within two-dimensional(2D)reduced graphene oxide(rGO)scrolls.In this ingenious strategy,1D NS-CNFs are regarded as building blocks to prevent the aggregation and pulverization of Sn QDs during sodiation/desodiation,2D rGO acts as electrical roads and“bridges”among NS-CNFs to improve the conductivity of the electrode and enlarge the contact area with electrolyte.Because of the unique structural merits,the flexible 3D hierarchical conductive network was directly used as binder-and current collectorfree anode for SIBs,exhibiting ultra-long cycling life(373 mAh g?1 after 5000 cycles at 1 A g?1),and excellent high-rate capability(189 mAh g?1 at 10 A g?1).This work provides a facile and efficient engineering method to construct 3D hierarchical conductive electrodes for other flexible energy storage devices.
