We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in...We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.展开更多
Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and t...Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and the low photoluminescence quantum yield(PLQY)restrict their performance and potential use,especially in ultraviolet(UV)wavelength light ranges.Quantum dots(QD)derived from 2D materials(2D/QD)provide efficient light absorption and emission of which energy can be tuned for desirable light wavelength.In this study,we greatly enhanced the photon absorption and PLQY of monolayer(1L)tungsten disulfide(WS_(2))in the UV range via hybridization with 2D/QD,particularly titanium nitride MXene QD(Ti_(2)N MQD)and graphitic carbon nitride QD(GCNQD).With the hybridization of MQD or GCNQD,1LWS_(2)showed a maximum PL enhancement by 15 times with 300 nm wavelength excitation,while no noticeable enhancement was observed when the excitation photon energy was less than the bandgap of the QD,indicating that UV absorption by the QD played a crucial role in enhancing the light emission of 1L-WS_(2)in our 0D/2D hybrid system.Our findings present a convenient method for enhancing the photo-response of 1L-WS_(2)to UV light and offer exciting possibilities for harvesting UV energy using 1L-TMD.展开更多
Heterojunction engineering is recognized as a promising strategy to modulate the photocatalytic properties of semiconductors.Herein,lead-free Cs_(2)CuBr_(4)perovskite quantum dots(PQDs)were confined in a mesoporous Cu...Heterojunction engineering is recognized as a promising strategy to modulate the photocatalytic properties of semiconductors.Herein,lead-free Cs_(2)CuBr_(4)perovskite quantum dots(PQDs)were confined in a mesoporous CuO framework and a p-n type S-scheme heterojunction of Cs_(2)CuBr_(4)/CuO(CCB/CuO)photocatalyst was fabricated.Experimental characterizations confirmed the effective confinement of the Cs_(2)CuBr_(4)PQDs in the mesoporous CuO framework,which enabled intimate contact in the interface of CCB/CuO heterojunction,thus facilitating the interfacial charge migration and separation between p-type CuO and n-type Cs_(2)CuBr_(4).Owing to the outstanding charge transport property and CO_(2)adsorption capacity,the developed CCB/CuO heterojunction exhibited remarkably enhanced photocatalytic CO_(2)conversion efficiency with an electron consumption rate(R_(electron))of 281.1μmol g^(-1)h^(-1),which was approximately2.8 times higher than that of pristine Cs_(2)CuBr_(4).These findings provide some insights into the rational engineering design of lead-free perovskite-based heterostructures for efficient photocatalytic CO_(2)conversion.展开更多
SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish ...SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.展开更多
The performance of the photodetector is significantly impacted by the inherent surface faults in GaAs nanowires(NWs).We combined three-dimensional(3D)gallium arsenide nanowires with zero-dimensional(0D)WS_(2) quantum ...The performance of the photodetector is significantly impacted by the inherent surface faults in GaAs nanowires(NWs).We combined three-dimensional(3D)gallium arsenide nanowires with zero-dimensional(0D)WS_(2) quantum dot(QDs)materials in a simple and convenient way to form a heterogeneous structure.Various performance enhancements have been realized through the formation of typeⅡenergy bands in heterostructures,opening up new research directions for the future development of photodetector devices.This work successfully fabricated a high-sensitivity photodetector based on WS_(2)QDs/GaAs NWs heterostructure.Under 660 nm laser excitation,the photodetector exhibits a responsivity of 368.07 A/W,a detectivity of 2.7×10^(12)Jones,an external quantum efficiency of 6.47×10^(2)%,a low-noise equivalent power of 2.27×10^(-17)W·Hz^(-1/2),a response time of 0.3 s,and a recovery time of 2.12 s.This study provides a new solution for the preparation of high-performance GaAs detectors and promotes the development of optoelectronic devices for GaAs NWs.展开更多
Solar-driven photocatalytic CO_(2) reduction to produce valuable chemicals and fuels offers an attractive strategy in alleviating the energy crisis.Pt quantum dots(PtQDs)with TiO_(2) nanowire(TiO_(2)NW)/Ti_(3)C_(2) MX...Solar-driven photocatalytic CO_(2) reduction to produce valuable chemicals and fuels offers an attractive strategy in alleviating the energy crisis.Pt quantum dots(PtQDs)with TiO_(2) nanowire(TiO_(2)NW)/Ti_(3)C_(2) MXene heterostructures(Pt-TiO_(2)NW/Ti_(3)C_(2)) with tight interfacial contacts between the various components were prepared at room temperature via oxidation reactions.The incorporated PtQDs played crucial roles as electron conduction bridges supported by the cocatalyst effect,effectively enhancing the separation efficiencies of photoinduced electron/hole pairs and improving CO_(2) reduction under simulated solar light irradiation.The Pt-TiO_(2)NW/Ti_(3)C_(2) heterostructures exhibited remarkable carbon monoxide(CO)and methane(CH_(4)) production at respective rates of 38.14 and 36.15μmol g^(-1)after 10 h of simulated solar light irradiation,an apparent quantum yield of 1.68%,and 79.2%selectivity for CH4.The photocatalytic activities of the Pt-TiO_(2) NW/Ti_(3)C_(2) heterostructures for CO_(2) reduction were significantly enhanced compared to those of TiO_(2)NW/Ti_(3)C_(2) and the single-component photocatalysts,and they exhibited remarkable stabilities even after five cycles.In addition,the densities of states and electronic characteristics of Ti_(3)C_(2) MXene and Pt-TiO_(2)NW/Ti_(3)C_(2) were studied using density functional theory,and a synergistic mechanism of the improvement in CO_(2) photoreduction is proposed.展开更多
Pressure induced insulator to metal transition followed by the appearance of superconductivity has been observed recently in inorganic quantum spin liquid candidate NaYbSe_(2).In this paper,we study the properties of ...Pressure induced insulator to metal transition followed by the appearance of superconductivity has been observed recently in inorganic quantum spin liquid candidate NaYbSe_(2).In this paper,we study the properties of isostructural compound NaYbS_(2)under pressure.It is found that the resistance of Na YbS_(2)single crystal exhibits an insulating state below 82.9 GPa,but with a drop of more than six orders of magnitude at room temperature.Then a minimum of resistance is observed at about 100.1 GPa and it moves to lower temperature with further compression.Finally,a metallic state in the whole temperature range is observed at about 130.3 GPa accompanied by a non-Fermi liquid behavior below 100 K.The insulator to metal transition,non-monotonic resistance feature and non-Fermi liquid behavior of NaYbS_(2)under pressure are similar to those of NaYbSe_(2),suggesting that these phenomena might be the universal properties in NaLnCh_(2)(Ln=rare earth,Ch=O,S,Se)system.展开更多
The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determi...The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determined to be~0.59 eV in height.It is found that the electron transfer from the copper substrate to H_(2) plays a key role in the activation and breaking of the H–H bond,and the formation of the Cu–H bonds.Two stationary states are identified at around the critical height of bond breaking,corresponding to the molecular and the dissociative states,respectively.Using the transfer matrix method,we also investigate the role of quantum tunneling in the dissociation process along the minimum energy pathway(MEP),which is found to be significant at or below room temperature.At a given temperature,the tunneling contributions due to the translational and the vibrational motions of H_(2) are quantified for the dissociation process.Within a wide range of temperature,the effects of quantum tunneling on the effective barriers of dissociation and the rate constants are observed.The deduced energetic parameters associated with the thermal equilibrium and non-equilibrium(molecular beam)conditions are comparable to experimental data.In the low-temperature region,the crossover from classical to quantum regime is identified.展开更多
This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2) quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size ...This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2) quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size increased with longer annealing,reducing catalytic activity.UV–vis,XRD,TEM,and FTIR analyses probed optical structural,morphological,and vibrational features.XRD confirmed NiS2's anorthic structure,with crystallite size growing from 6.53 to 7.81 nm during extended annealing.UV–Vis exhibited a bathochromic shift,reflecting reduced band gap energy(Eg)in NiS_(2).TEM revealed NiS_(2)QD formation,with agglomerated QD average size increasing from 7.13 to 9.65 nm with prolonged annealing.Pure NiS_(2) showed significant MB decolorization(89.85%)in acidic conditions.Annealed NiS_(2) QDs demonstrated notable antibacterial activity,yielding a 6.15mm inhibition zone against Escherichia coli(E.coli)compared to Ciprofloxacin.First-principles computation supported a robust interaction between MB and NiS_(2),evidenced by obtained adsorption energies.This study highlights the nuanced relationship between annealing duration,structural changes,and functional properties in NiS_(2)QDs,emphasizing their potential applications in catalysis and antibacterial interventions.展开更多
Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like cov...Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like covalent organic framework(COF)to form a step-scheme(S-scheme)photocata-lyst for H_(2)O_(2)production.The as-prepared S-scheme photocatalyst exhibits a broad light absorption range with an edge at 810 nm owing to the synergistic effect between the ZnSe QDs and COF.The S-scheme charge-carrier transfer mechanism is validated by performing Fermi level calculations and in-situ X-ray photoelectron and femtosecond transient absorption spectroscopies.Photolumi-nescence,time-resolved photoluminescence,photocurrent response,electrochemical impedance spectroscopy,and electron paramagnetic resonance results show that the S-scheme heterojunction not only promotes charge carrier separation but also boosts the redox ability,resulting in enhanced photocatalytic performance.Remarkably,a 10%-ZnSe QD/COF has excellent photocatalytic H_(2)O_(2)-production activity,and the optimal S-scheme composite with ethanol as the hole scavenger yields a H_(2)O_(2)-production rate of 1895 mol g^(-1)h^(-1).This study presents an example of a high-performance organic/inorganic S-scheme photocatalyst for H_(2)O_(2)production.展开更多
基金the Natural Science Foundation of China(11922415,12274471)Guangdong Basic and Applied Basic Research Foundation(2022A1515011168,2019A1515011718,2019A1515011337)the Key Research and Development Program of Guangdong Province,China(2019B110209003).
文摘We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
基金supported by National Research Foundation of Korea (NRF)funded by the Ministry of Education (2021R1A6A1A03039696,2022R1A2C2009412)
文摘Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and the low photoluminescence quantum yield(PLQY)restrict their performance and potential use,especially in ultraviolet(UV)wavelength light ranges.Quantum dots(QD)derived from 2D materials(2D/QD)provide efficient light absorption and emission of which energy can be tuned for desirable light wavelength.In this study,we greatly enhanced the photon absorption and PLQY of monolayer(1L)tungsten disulfide(WS_(2))in the UV range via hybridization with 2D/QD,particularly titanium nitride MXene QD(Ti_(2)N MQD)and graphitic carbon nitride QD(GCNQD).With the hybridization of MQD or GCNQD,1LWS_(2)showed a maximum PL enhancement by 15 times with 300 nm wavelength excitation,while no noticeable enhancement was observed when the excitation photon energy was less than the bandgap of the QD,indicating that UV absorption by the QD played a crucial role in enhancing the light emission of 1L-WS_(2)in our 0D/2D hybrid system.Our findings present a convenient method for enhancing the photo-response of 1L-WS_(2)to UV light and offer exciting possibilities for harvesting UV energy using 1L-TMD.
基金financially supported by Natural Science Foundation of Shanghai(No.22ZR1460700)Shanghai Institute of Technology(No.XTCX2022-28)。
文摘Heterojunction engineering is recognized as a promising strategy to modulate the photocatalytic properties of semiconductors.Herein,lead-free Cs_(2)CuBr_(4)perovskite quantum dots(PQDs)were confined in a mesoporous CuO framework and a p-n type S-scheme heterojunction of Cs_(2)CuBr_(4)/CuO(CCB/CuO)photocatalyst was fabricated.Experimental characterizations confirmed the effective confinement of the Cs_(2)CuBr_(4)PQDs in the mesoporous CuO framework,which enabled intimate contact in the interface of CCB/CuO heterojunction,thus facilitating the interfacial charge migration and separation between p-type CuO and n-type Cs_(2)CuBr_(4).Owing to the outstanding charge transport property and CO_(2)adsorption capacity,the developed CCB/CuO heterojunction exhibited remarkably enhanced photocatalytic CO_(2)conversion efficiency with an electron consumption rate(R_(electron))of 281.1μmol g^(-1)h^(-1),which was approximately2.8 times higher than that of pristine Cs_(2)CuBr_(4).These findings provide some insights into the rational engineering design of lead-free perovskite-based heterostructures for efficient photocatalytic CO_(2)conversion.
基金National Natural Science Foundation of China,Grant/Award Number:51971065Innovation Program of Shanghai Municipal Education Commission,Grant/Award Number:2019-01-07-00-07-E00028。
文摘SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.
文摘The performance of the photodetector is significantly impacted by the inherent surface faults in GaAs nanowires(NWs).We combined three-dimensional(3D)gallium arsenide nanowires with zero-dimensional(0D)WS_(2) quantum dot(QDs)materials in a simple and convenient way to form a heterogeneous structure.Various performance enhancements have been realized through the formation of typeⅡenergy bands in heterostructures,opening up new research directions for the future development of photodetector devices.This work successfully fabricated a high-sensitivity photodetector based on WS_(2)QDs/GaAs NWs heterostructure.Under 660 nm laser excitation,the photodetector exhibits a responsivity of 368.07 A/W,a detectivity of 2.7×10^(12)Jones,an external quantum efficiency of 6.47×10^(2)%,a low-noise equivalent power of 2.27×10^(-17)W·Hz^(-1/2),a response time of 0.3 s,and a recovery time of 2.12 s.This study provides a new solution for the preparation of high-performance GaAs detectors and promotes the development of optoelectronic devices for GaAs NWs.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the South Korean Ministries of Education(NRF-2021R1I1A3059469,NRF2018R1A6A1A03024962)Science and ICT(NRF-2020R1A2C2100746)。
文摘Solar-driven photocatalytic CO_(2) reduction to produce valuable chemicals and fuels offers an attractive strategy in alleviating the energy crisis.Pt quantum dots(PtQDs)with TiO_(2) nanowire(TiO_(2)NW)/Ti_(3)C_(2) MXene heterostructures(Pt-TiO_(2)NW/Ti_(3)C_(2)) with tight interfacial contacts between the various components were prepared at room temperature via oxidation reactions.The incorporated PtQDs played crucial roles as electron conduction bridges supported by the cocatalyst effect,effectively enhancing the separation efficiencies of photoinduced electron/hole pairs and improving CO_(2) reduction under simulated solar light irradiation.The Pt-TiO_(2)NW/Ti_(3)C_(2) heterostructures exhibited remarkable carbon monoxide(CO)and methane(CH_(4)) production at respective rates of 38.14 and 36.15μmol g^(-1)after 10 h of simulated solar light irradiation,an apparent quantum yield of 1.68%,and 79.2%selectivity for CH4.The photocatalytic activities of the Pt-TiO_(2) NW/Ti_(3)C_(2) heterostructures for CO_(2) reduction were significantly enhanced compared to those of TiO_(2)NW/Ti_(3)C_(2) and the single-component photocatalysts,and they exhibited remarkable stabilities even after five cycles.In addition,the densities of states and electronic characteristics of Ti_(3)C_(2) MXene and Pt-TiO_(2)NW/Ti_(3)C_(2) were studied using density functional theory,and a synergistic mechanism of the improvement in CO_(2) photoreduction is proposed.
基金the National Key Research and Development Program of China(Grant Nos.2018YFA0305700,2018YFE0202600,and 2022YFA1403800)the Beijing Natural Science Foundation(Grant Nos.2202059 and Z200005)+2 种基金the National Natural Science Foundation of China(Grant Nos.22171283 and 12274459)the Hebei Natural Science Foundation(Grant No.B2020205040)the Beijing National Laboratory for Condensed Matter Physics。
文摘Pressure induced insulator to metal transition followed by the appearance of superconductivity has been observed recently in inorganic quantum spin liquid candidate NaYbSe_(2).In this paper,we study the properties of isostructural compound NaYbS_(2)under pressure.It is found that the resistance of Na YbS_(2)single crystal exhibits an insulating state below 82.9 GPa,but with a drop of more than six orders of magnitude at room temperature.Then a minimum of resistance is observed at about 100.1 GPa and it moves to lower temperature with further compression.Finally,a metallic state in the whole temperature range is observed at about 130.3 GPa accompanied by a non-Fermi liquid behavior below 100 K.The insulator to metal transition,non-monotonic resistance feature and non-Fermi liquid behavior of NaYbS_(2)under pressure are similar to those of NaYbSe_(2),suggesting that these phenomena might be the universal properties in NaLnCh_(2)(Ln=rare earth,Ch=O,S,Se)system.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11474285 and 12074382)。
文摘The activation and dissociation of hydrogen molecules(H_(2))on the Cu(001)surface are studied theoretically.Using first-principles calculations,the activation barrier for the dissociation of H_(2) on Cu(001)is determined to be~0.59 eV in height.It is found that the electron transfer from the copper substrate to H_(2) plays a key role in the activation and breaking of the H–H bond,and the formation of the Cu–H bonds.Two stationary states are identified at around the critical height of bond breaking,corresponding to the molecular and the dissociative states,respectively.Using the transfer matrix method,we also investigate the role of quantum tunneling in the dissociation process along the minimum energy pathway(MEP),which is found to be significant at or below room temperature.At a given temperature,the tunneling contributions due to the translational and the vibrational motions of H_(2) are quantified for the dissociation process.Within a wide range of temperature,the effects of quantum tunneling on the effective barriers of dissociation and the rate constants are observed.The deduced energetic parameters associated with the thermal equilibrium and non-equilibrium(molecular beam)conditions are comparable to experimental data.In the low-temperature region,the crossover from classical to quantum regime is identified.
基金The authors thank the Deanship of Scientific Research at King Khalid University for funding this work through a large group Research Project under grant number(R.G.P.2/123/44).The author MBK would like to thank Prince Sultan University for their support.
文摘This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2) quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size increased with longer annealing,reducing catalytic activity.UV–vis,XRD,TEM,and FTIR analyses probed optical structural,morphological,and vibrational features.XRD confirmed NiS2's anorthic structure,with crystallite size growing from 6.53 to 7.81 nm during extended annealing.UV–Vis exhibited a bathochromic shift,reflecting reduced band gap energy(Eg)in NiS_(2).TEM revealed NiS_(2)QD formation,with agglomerated QD average size increasing from 7.13 to 9.65 nm with prolonged annealing.Pure NiS_(2) showed significant MB decolorization(89.85%)in acidic conditions.Annealed NiS_(2) QDs demonstrated notable antibacterial activity,yielding a 6.15mm inhibition zone against Escherichia coli(E.coli)compared to Ciprofloxacin.First-principles computation supported a robust interaction between MB and NiS_(2),evidenced by obtained adsorption energies.This study highlights the nuanced relationship between annealing duration,structural changes,and functional properties in NiS_(2)QDs,emphasizing their potential applications in catalysis and antibacterial interventions.
文摘Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like covalent organic framework(COF)to form a step-scheme(S-scheme)photocata-lyst for H_(2)O_(2)production.The as-prepared S-scheme photocatalyst exhibits a broad light absorption range with an edge at 810 nm owing to the synergistic effect between the ZnSe QDs and COF.The S-scheme charge-carrier transfer mechanism is validated by performing Fermi level calculations and in-situ X-ray photoelectron and femtosecond transient absorption spectroscopies.Photolumi-nescence,time-resolved photoluminescence,photocurrent response,electrochemical impedance spectroscopy,and electron paramagnetic resonance results show that the S-scheme heterojunction not only promotes charge carrier separation but also boosts the redox ability,resulting in enhanced photocatalytic performance.Remarkably,a 10%-ZnSe QD/COF has excellent photocatalytic H_(2)O_(2)-production activity,and the optimal S-scheme composite with ethanol as the hole scavenger yields a H_(2)O_(2)-production rate of 1895 mol g^(-1)h^(-1).This study presents an example of a high-performance organic/inorganic S-scheme photocatalyst for H_(2)O_(2)production.
