While photoreduction of CO_(2) to CH 4 is an effective means of producing value-added fuels,common pho-tocatalysts have poor activity and low selectivity in photocatalytic CO_(2)-reduction processes.Even though creati...While photoreduction of CO_(2) to CH 4 is an effective means of producing value-added fuels,common pho-tocatalysts have poor activity and low selectivity in photocatalytic CO_(2)-reduction processes.Even though creating defects is an effective photocatalyst fabrication route to improve photocatalytic activity,there are some challenges with the facile photocatalyst synthesis method.In this work,an O element is in-troduced into a graphitic carbon nitride(CN)skeleton through a precursory ultraviolet light irradiation pretreatment to increase the visible light absorption and enhance the carrier density of this modified non-metal CN photocatalyst;the charge transfer dynamics thereof are also studied through electrochem-ical tests,photoluminescence spectroscopy,and nanosecond transient absorption.We verify that the op-timized sample exhibits lower charge recombination and a suppressed 84 ns electron-trapping lifetime,compared to the 103 ns electron-trapping lifetime of the CN counterpart,and thereby contributes to ro-bust detrapping and a fast transfer of active electrons.Through density functional theory calculations,we find that the improved light absorption and increased electron density are ascribed to O-element doping,which enhances the CO_(2) adsorption energy and improves the CO_(2)-to-CH 4 photoreduction activity;it be-comes 17 times higher than that of the bare CN,and the selectivity is 3.8 times higher than that of CN.Moreover,the optimized sample demonstrates excellent cyclic stability in a 24-hour cycle test.展开更多
The strategy of a reliable transition temperature control of vanadium dioxide(VO2)is reported.Rectangular VO2 nanobeams were synthesized by a thermal chemical vapor deposition(TCVD)system.The metal-insulator transitio...The strategy of a reliable transition temperature control of vanadium dioxide(VO2)is reported.Rectangular VO2 nanobeams were synthesized by a thermal chemical vapor deposition(TCVD)system.The metal-insulator transition(MIT)temperature increases to above 380K when the TiO2 ratio of the source is 5 at.%,although the Ti source is not physically doped into VO2 nanobeams.The XPS spectra of the V 2p orbital reveal the excessive oxidation of V after the TCVD processes with a higher TiO2 ratio,indicating that the TiO2 precursor is important in the O-doping of the surface V O bonds when forming volatile Ti-O gas species.Thus,TiO2 reactants can be used as a VO2 surface chemical modifier to manipulate the MIT transition temperature and maintain a homogenous VO2 phase,which is useful for a Mott device application with a record on/off switching ratio>104 and Mott transition temperature>380 K.展开更多
Organic semiconductors(OSCs)are showing great promise in large-area wearable devices,optoelectronic displays,logic circuits,and next-generation optoelectronic applications[1-9].Examples include organic field-effect tr...Organic semiconductors(OSCs)are showing great promise in large-area wearable devices,optoelectronic displays,logic circuits,and next-generation optoelectronic applications[1-9].Examples include organic field-effect transistors(OFETs),organic light-emitting diodes(OLEDs),organic photovoltaic cells(OPVs),and sensing devices.However,OSCs encounter significant challenges in widespread commercialization[10-13].Compared with their inorganic counterparts connected by strong covalent bonds,the structural characteristics of OSCs films are predominantly governed by van der Waals interactions[14-19],rendering their optoelectronic properties typically dependent on the synergistic effects between intrinsic properties and extrinsic effects,such as impurities and defects[20-26].展开更多
The enhancement of the photocatalytic activity of graphitic carbon nitride(g-C_(3)N_(4))depends on the rational design of its visible-light harvesting and charge separation/migration properties.Herein,an oxygen doping...The enhancement of the photocatalytic activity of graphitic carbon nitride(g-C_(3)N_(4))depends on the rational design of its visible-light harvesting and charge separation/migration properties.Herein,an oxygen doping-induced intramolecular electron acceptor system enabling n→π^(*)electronic transitions in red g-C_(3)N_(4)nanosheets(Eg∼1.89 eV)was prepared via copolymerization with nitrilotriacetic acid(NTA)and urea.The n→π^(*)electronic transition can be controllably tuned,thus broadening the absorption spectrum of the system to∼750 nm.Simultaneously,doping with oxygen which acts as an electron acceptor,accelerates in-plane charge separation and migration.Moreover,this strategy was confirmed experimentally to be scalable for industrial mass production.Experiments and theoretical calculations demonstrated that the oxygen doping could continuously modulate the band gap(from∼2.65 to∼1.32 eV),resulting in the formation of an intramolecular electron acceptor system which enhances charge separation/migration kinetics.The optimized sample exhibited remarkable photocatalytic H_(2)and H_(2)O_(2)production rates of∼144.8µmol/h and∼539.76µM/h,respectively,which are higher than those for currently available g-C_(3)N_(4)-based photocatalysts.Significantly,the sample exhibited H_(2)and H_(2)O_(2)photocatalytic yields∼37.3 and∼30.1 times those of pristine g-C_(3)N_(4)under long-wavelength excitation(λ=520 nm).This study developed an effective and scalable strategy for the design and synthesis of full-spectrum photocatalysts for a broad range of applications.展开更多
Heteroatom doping and defect engineering have been proposed as effective ways to modulate the energy band structure and improve the photocatalytic activity of g-C_(3)N_(4). In this work, ultrathin defective g-C_(3)N_(...Heteroatom doping and defect engineering have been proposed as effective ways to modulate the energy band structure and improve the photocatalytic activity of g-C_(3)N_(4). In this work, ultrathin defective g-C_(3)N_(4) was successfully prepared using cold plasma. Plasma exfoliation reduces the thickness of g-C_(3)N_(4) from 10 nm to 3 nm, while simultaneously introducing a large number of nitrogen defects and oxygen atoms into g-C_(3)N_(4). The amount of doped O was regulated by varying the time and power of the plasma treatment. Due to N vacancies, O atoms formed strong bonds with C atoms, resulting in O doping in g-C_(3)N_(4). The mechanism of plasma treatment involves oxygen etching and gas expansion. Photocatalytic experiments demonstrated that appropriate amount of O doping improved the photocatalytic degradation of rhodamine B compared with pure g-C_(3)N_(4). The introduction of O optimized the energy band structure and photoelectric properties of g-C_(3)N_(4). Active species trapping experiments revealed ·O_(2)^(–) as the main active species during the degradation.展开更多
Graphitic carbon nitride(g-C3N4,CN)exhibits inefficient charge separation,deficient CO2 adsorption and activation sites,and sluggish surface reaction kinetics,which have been recognized as the main barriers to its app...Graphitic carbon nitride(g-C3N4,CN)exhibits inefficient charge separation,deficient CO2 adsorption and activation sites,and sluggish surface reaction kinetics,which have been recognized as the main barriers to its application in CO2 photocatalytic reduction.In this work,carbon quantum dot(CQD)decoration and oxygen atom doping were applied to CN by a facile one-step hydrothermal method.The incorporated CQDs not only facilitate charge transfer and separation,but also provide alternative CO2 adsorption and activation sites.Further,the oxygen-atom-doped CN(OCN),in which oxygen doping is accompanied by the formation of nitrogen defects,proves to be a sustainable H^+ provider by facilitating the water dissociation and oxidation half-reactions.Because of the synergistic effect of the hybridized binary CQDs/OCN addressing the three challenging issues of the CN based materials,the performance of CO2 photocatalytic conversion to CH4 over CQDs/OCN-x(x represents the volume ratio of laboratory-used H2O2(30 wt.%)in the mixed solution)is dramatically improved by 11 times at least.The hybrid photocatalyst design and mechanism proposed in this work could inspire more rational design and fabrication of effective photocatalysts for CO2 photocatalytic conversion with a high CH4 selectivity.展开更多
Engineering the electronic properties of semiconductor-based photocatalysts using elemental doping is an effective approach to improve their catalytic activity.Nevertheless,there still remain contradictions regarding ...Engineering the electronic properties of semiconductor-based photocatalysts using elemental doping is an effective approach to improve their catalytic activity.Nevertheless,there still remain contradictions regarding the role of the dopants played in photocatalysis.Herein,ultrathin ZnIn_(2)S_(4)(ZIS) nanosheets with oxygen doping were synthesized by a one-pot solvothermal method.XRD,XPS and Raman spectral measurements support the presence of lattice oxygen in the oxygen-doped ZIS(O-ZIS) sample.With optimum doping of oxygen,the ultrathin O-ZIS nanosheets show enhanced CO_(2)-to-CO conversion activity with a CO_(2)-evolving rate of 1680 μmol h^(-1) g^(-1) under visible light irradiation,which is about 7 times higher than that of the pristine ZIS.First-principle calculations support that doping of oxygen in the lattice of ZnIn_(2)S_(4) nanosheets plays a key role in tuning its electronic properties.The remarkable photocatalytic performance of O-ZIS can be assigned to a synergistic consequence of a unique ultrathin-layered structure and an upward shift of the conduction band minimum(CBM) caused by the oxygen doping into ZIS and the quantum confinement effect(QCE) induced by the decreased particle size after doping as well as to the improved charge separation efficiency.The present work offers a simple elemental doping method to promote charge separation at atomic level and illustrates the roles played by oxygen doping in photocatalysis,giving new insights into highly efficient artificial photosynthesis.展开更多
The influence of oxygen doping on resistive-switching characteristics of Ag/a-Si/p^＋-c-Si device was investigated. By oxygen doping in the growth process of amorphous silicon, the device resistive-switching performan...The influence of oxygen doping on resistive-switching characteristics of Ag/a-Si/p^＋-c-Si device was investigated. By oxygen doping in the growth process of amorphous silicon, the device resistive-switching performances, such as the ON/OFF resistance ratios, yield and stability were improved, which may be ascribed to the significant reduction of defect density because of oxygen incorporation. The device I-V characteristics are strongly dependent on the oxygen doping concentration. As the oxygen doping concentration increases, the Si-rich device gradually transforms to an oxygen-rich device, and the device yield, switching characteristics, and stability may be improved for silver/oxygen-doped a-Si/p^＋-c-Si device. Finally, the device resistive-switching mechanism was ana- lyzed. Key words： amorphous silicon; resistive switching; oxygen doping展开更多
Both sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)are considered as promising candidates in grid-level energy storage devices.Unfortunately,the larger ionic radii of K+and Na+induce poor diffusion kineti...Both sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)are considered as promising candidates in grid-level energy storage devices.Unfortunately,the larger ionic radii of K+and Na+induce poor diffusion kinetics and cycling stability of carbon anode materials.Pore structure regulation is an ideal strategy to promote the diffusion kinetics and cyclic stability of carbon materials by facilitating electrolyte infiltration,increasing the transport channels,and alleviating the volume change.However,traditional pore-forming agent-assisted methods considerably increase the difficulty of synthesis and limit practical applications of porous carbon materials.Herein,porous carbon materials(Ca-PC/Na-PC/K-PC)with different pore structures have been prepared with gluconates as the precursors,and the amorphous structure,abundant micropores,and oxygen-doping active sites endow the Ca-PC anode with excellent potassium and sodium storage performance.For PIBs,the capacitive contribution ratio of Ca-PC is 82%at 5.0 mV s^(-1) due to the introduction of micropores and high oxygen-doping content,while a high reversible capacity of 121.4 mAh g^(-1) can be reached at 5 A g^(-1) after 2000 cycles.For SIBs,stable sodium storage capacity of 101.4 mAh g^(-1) can be achieved at 2 A g^(-1) after 8000 cycles with a very low decay rate of 0.65%for per cycle.This work may provide an avenue for the application of porous carbon materials in the energy storage field.展开更多
Heteroatom-doped meso/micro-porous carbon materials are conventionally produced by harsh carbonization under an inert atmosphere involving specific precursors,hard/soft templates,and heteroatom-containing agents.Herei...Heteroatom-doped meso/micro-porous carbon materials are conventionally produced by harsh carbonization under an inert atmosphere involving specific precursors,hard/soft templates,and heteroatom-containing agents.Herein,we report a facile synthesis of N and O co-doped meso/micro-porous carbon(NOMC)by template-free carbonization of a small-molecule precursor in a semi-closed system.The semi-closed carbonizaiton process yields hydrophilic NOMCs with large surface area in a high yield.The porous structure as well as the elemental composition of NOMCs can be modulated by changing the holding time at a particular temperature.NOMCs as metal-free heterogeneous catalysts can selectively oxidize benzyl alcohol and its derivatives into aldehydes/ketones with>85%conversion in aqueous solution,which is much higher than that of the control sample obtained in tube furnace(21%conversion),mainly due to their high N content,high percentage of pyridinic N,and large surface area.The presence of O-containing moieties also helps to improve the hydrophilicity and dispersion ability of catalysts and thus facilitates the mass transfer process during aqueous oxidation.The NOMC catalysts also dispayed excellent activity for a wide range of substrates with a selectivity of>99%.展开更多
Oxygen atoms usually co-exist in the lattice of hexagonal boron nitride(h-BN). The understanding of interactions between the oxygen atoms and the adsorbate, however, is still ambiguous on improving adsorptive desulfur...Oxygen atoms usually co-exist in the lattice of hexagonal boron nitride(h-BN). The understanding of interactions between the oxygen atoms and the adsorbate, however, is still ambiguous on improving adsorptive desulfurization performance. Herein, simultaneously oxygen atom-scale interior substitution and edge hydroxylation in BN structure were constructed via a polymer-based synthetic strategy.Experimental results indicated that the dual oxygen modified BN(BN–2O) exhibited an impressively increased adsorptive capacity about 12% higher than that of the edge hydroxylated BN(BN–OH) fabricated via a traditional method. The dibenzothiophene(DBT) was investigated to undergo multimolecular layer type coverage on the BN–2O uneven surface via π–π interaction, which was enhanced by the increased oxygen doping at the edges of BN–2O. The density functional theory calculations also unveiled that the oxygen atoms confined in BN interior structure could polarize the adsorbate, thereby resulting in a dipole interaction between the adsorbate and BN–2O. This effect endowed BN–2O with the ability to selectively adsorb DBT from the aromatic-rich fuel, thereafter leading to an impressive prospect for the adsorptive desulfurization performance of the fuel. The adsorptive result was in good accordance with Freundlich and pseudo-second-order adsorption kinetics model results. Therefore, the designing of a polymer-based strategy could be also extended to other heteroatom doping systems to enhance adsorptive performance.展开更多
Highly efficient photon-to-electron conversion is crucial for achieving photocatalytic conversion.In this study,oxygen-doped carbon nitride nanocages(O@CNNCs)were engineered via dual strategies of morphology-controlle...Highly efficient photon-to-electron conversion is crucial for achieving photocatalytic conversion.In this study,oxygen-doped carbon nitride nanocages(O@CNNCs)were engineered via dual strategies of morphology-controlled heteroatom doping,which was successfully used in the photocatalytic selective oxidation of xylose/xylan to xylonic acid.The nanocage-shaped O@CNNCs had a larger surface area,which was 4.02 times of carbon nitride(CN).Furthermore,with the assistance of morphology regulation and O-doping,O@CNNCs exhibit highly efficient photon-to-electron conversion,enhanced visible-light utilization,high photocurrent,low resistance,and fast separation/migration of electron-hole pairs.Correspondingly,the photocatalytic oxidation of xylose to xylonic acid using O@CNNCs was successfully achieved under mild reaction conditions with a yield of 83.4%.O@CNNCs have excellent recyclability,in which the yield of xylonic acid in the 5th cycle was 98.2%of its initial use.The O@CNNC photocatalytic system was also suitable for macromolecular xylan,and a xylonic acid yield of 77.34 mg was obtained when 100 mg xylan was used.The oxidation-active species captured experiments indicated that holes were crucial for the selective oxidation of xylose to xylonic acid.Overall,this study provides a new strategy for the preparation of photocatalysts with excellent photon-to-electron conversion and selective oxidation of biomass-derived feedstocks to xylonic acid.展开更多
Transition-metal chalcogenides with hollow nanostructure,especially cobalt sulfides,are considered as the most pro mising non-precious metal catalysts for oxygen evolution reactio n.However,it is difficult to synthesi...Transition-metal chalcogenides with hollow nanostructure,especially cobalt sulfides,are considered as the most pro mising non-precious metal catalysts for oxygen evolution reactio n.However,it is difficult to synthesize oxygen-containing cobalt sulphides with hollow structure due to the different physical/chemical properties between metal sulfides and metal cobalts.Herein,we report a novel oxygencontaining amorphous cobalt sulfide ball-in-ball hollow sphere s(Co-S-O BBHS) synthesized by an anion exchange method.Taking advantage of the ball-in-ball hollow structure,the amorphous Co-S-O BBHS shows supe rior oxygen evolution reaction(OER) electrocatalytic performance with a low overpotentiat of285 mV at 10 mA/cm2,small Tafel slope of 49.67 mV/dec,high Faraday efficiency of 96%,and satisfied durability.Experiments and DFT calculations demonstrate that the introduction of oxygen and sulfur modulates the electronic structure of Co-S-O BBHS,thus enhancing the adsorption of *0(adsorbed 0 species on catalyst surface) intermediate,which greatly boosts the catalytic activity towards OER.This work provides a new strategy for controllable synthe sis of complex hollow structures of transition-metal chalcogenides for OER.展开更多
In recent decade, Au nanoclusters of atomic precision （AunLm, where L= organic ligand： thiolate andphosphine） have been shown as a new promising nanogold catalyst. The well-defined AunLm catalystspossess unique ele...In recent decade, Au nanoclusters of atomic precision （AunLm, where L= organic ligand： thiolate andphosphine） have been shown as a new promising nanogold catalyst. The well-defined AunLm catalystspossess unique electronic properties and frameworks, providing an excellent opportunity to correlate theintrinsic catalytic behavior with the cluster＇s framework as well as to study the catalytic mechanismsover gold nanoclusters. In this review, we only demonstrate the important roles of the gold nanoclustersin the oxygen activation （e.g., 302 to 102） and their selective oxidations in the presence of oxygen （e.g., COto C02, sulfides to sulfoxides, alcohol to aldehyde, styrene to styrene epoxide, amines to imines, andglucose to gluconic acid）. The size-specificity （Au25 （1.3 nm）, Au38 （].5 nm）, Au144 （1.9 nm）, etc.）, ligandengineering （e.g., aromatic vs aliphatic）, and doping effects （e.g., copper, silver, palladium, and platinum）are discussed in details. Finally, the proposed reactions＇ mechanism and the relationships of clusters＇structure and activity at the atomic level also are presented.展开更多
The presence of excess Ta in high-temperature protective coatings can compromise the integrity of the Al_(2)O_(3)scale on the surface,which has a negative impact on the oxidation behavior and reduces the service life....The presence of excess Ta in high-temperature protective coatings can compromise the integrity of the Al_(2)O_(3)scale on the surface,which has a negative impact on the oxidation behavior and reduces the service life.The effects of oxygen doping on the isothermal oxidation of three sputtered nanocrystalline coatings were investigated at 1100°C.The results indicated that oxygen doping inhibited the diffusion of Ta from the coating to the oxide scale,which was primarily attributed to the preferential oxidation of the Al in the coating.However,excess oxygen doping decreased the amount of Al available for the formation of the Al_(2)O_(3)scale on the coating,thus reducing the inhibitory effect on Ta oxidation.Moreover,doping with excess O caused spalling of the oxide scale.Therefore,the right balance in O doping is crucial for suppressing Ta oxidation while maintaining the integrity of the oxide scale.展开更多
Refractory multi-principal element alloys(RMPEAs)have garnered attention for their potential in high-temperature applications.Additive manufacturing(AM)provides opportunities to tailor RMPEAs’microstructures to enhan...Refractory multi-principal element alloys(RMPEAs)have garnered attention for their potential in high-temperature applications.Additive manufacturing(AM)provides opportunities to tailor RMPEAs’microstructures to enhance these properties.However,controlling defects and addressing the challenges posed by the complex thermal history during the AM process are crucial for optimizing RMPEAs’performance.This study aims to fabricate a high-quality oxygen-doped NbTiZr alloys using laser powder bed fusion and investigate their microstructure and mechanical properties.Our analysis reveals refined grain sizes and a periodic combination of fine near-equiaxed and columnar grain morphologies in the AM-fabricated alloy.Its substructure is characterized by the coexistence of loosely defined cellular dislocation networks and elemental segregation.Compared to its cast counterpart,the additively manufactured alloy exhibits a combination of high yield strength,excellent tensile ductility,and enhanced work hardening.These attributes make the AM-fabricated oxygen-doped NbTiZr alloy a promising candidate for applications required balanced mechanical properties.Understanding the specific effects of different crystal structures and deformation mechanisms is essential for optimizing AM processes to tailor the microstructure and achieve the desired mechanical performance in various engineering applications.展开更多
To realize the continuous production of hydrogen energy,the efficient photocatalysts are required in the heterogeneous reaction for water splitting.Herein,we reported a surface modulation strategy,via doping oxygen at...To realize the continuous production of hydrogen energy,the efficient photocatalysts are required in the heterogeneous reaction for water splitting.Herein,we reported a surface modulation strategy,via doping oxygen atoms to tune the surface state of ZnIn_(2)S_(4)nanosheets with cocatalyst MoS_(2)modification,to enhance water adsorption and surface catalytic reaction for boosting the photocatalytic activity.Consequently,MoS_(2)/O-ZnIn_(2)S_(4)photocatalysts showed a remarkably superior photocatalytic H_(2)production performance of 4.002 mmol g^(-1)h^(-1)and an apparent quantum yield(AQY)of~2.53%,5.4 folds higher than ZnIn_(2)S_(4).Using operando infrared spectroscopy and DFT calculation,we revealed the dynamic structural evolution,as well as the active sites for water adsorption and the catalytic reaction at the MoS_(2)/O ZnIn_(2)S_(4)interface.This work reveals the effect of surface modulation on the photocatalytic activity for MoS_(2)/O-ZnIn_(2)S_(4)and offers a feasible method to devise excellent nanomaterial photocatalysts for H_(2)production.展开更多
Exposure to oxygen alters the physical and chemical properties of two-dimensional(2D)transition metal dichalcogenides(TMDs).In particular,oxygen in the ambient may influence the device stability of 2D TMDs over time.E...Exposure to oxygen alters the physical and chemical properties of two-dimensional(2D)transition metal dichalcogenides(TMDs).In particular,oxygen in the ambient may influence the device stability of 2D TMDs over time.Engineering the doping of 2D TMDs,especially hole doping is highly desirable towards their device function.Herein,controllable oxygen-induced p-type doping in a range of hexagonal(MoTe2,WSe2,MoSe2 and PtSe2)and pentagonal(PdSe2)2D TMDs are demonstrated.Scanning tunneling microscopy,electrical transport and X-ray photoelectron spectroscopy are used to probe the origin of oxygen-derived hole doping.Three mechanisms are postulated that contribute to the hole doping in 2D TMDs,namely charge transfer from absorbed oxygen molecules,surface oxides,and chalcogen atom substitution.This work provides insights into the doping effects of oxygen,enabling the engineering of 2D TMDs properties for nanoelectronic applications.展开更多
Photocatalytic H2 production and CO2 reduction have attracted considerable attention for clean energy development.In this work,we designed an efficient photocatalyst by integrating lamellar oxygen-doped carbon nitride...Photocatalytic H2 production and CO2 reduction have attracted considerable attention for clean energy development.In this work,we designed an efficient photocatalyst by integrating lamellar oxygen-doped carbon nitride(CNO)nanosheets into ZnIn2S4(ZIS)microflowers by a one-step hydrothermal method.A well-fitted 2D hierarchical hybrid heterostructure was fabricated.Under visible light irradiation,the ZIS@CNO composite with 40 wt%CNO(ZC 40%)showed the highest hydrogen evolution rate from water(188.4μmol·h-1),which was approximately 2.1 times higher than those of CNO and ZIS(88.6 and 90.2μmol·h-1,respectively).Furthermore,the selective CO production rates of ZC 40%(12.69μmol·h-1)were 2.2 and 14.0 times higher than those of ZIS(5.85μmol·h-1)and CNO(0.91μmol·h-1),respectively,and the CH4 production rate of ZC 40%was 1.18μmol·h-1.This enhanced photocatalytic activity of CNO@ZIS is due mainly to the formation of a heterostructure that can promote the transfer of photoinduced electrons and holes between CNO and ZIS,thereby efficiently avoiding recombination of electron-hole pairs.展开更多
Femtosecond laser ablation-driven periodic surface structuring offers a promising method for large-scale and high-throughput nanolithography technique.However,the self-organized periodic structures typically manifest ...Femtosecond laser ablation-driven periodic surface structuring offers a promising method for large-scale and high-throughput nanolithography technique.However,the self-organized periodic structures typically manifest constraints in terms of tunable period and depth,as well as suboptimal regularity,which restricts their broader application potential.Here,in terms of a rarely explored laser-induced photochemical mechanism for nonablative structuring,we demonstrate manufacturing of sub-wavelength oxidative grating structures on silicon films with active structural modulation.In this scenario,the plasmonic field plays a pivotal role in dragging oxygen ions from surface into the silicon,greatly speeding up oxidation rates.While high oxygen doping levels can already be achieved with single-pulse exposure,far superior results are obtained with the application of 40-MHz burst mode pulse trains,mitigating the formation of excessively large nanocrystallites.Furthermore,it is revealed that the periodicity and modulation depth of laser-writing nanograting are both dependent on the number of pulse per burst.This offers a convenient scheme for actively controlling laser plasmonic lithography.展开更多
文摘While photoreduction of CO_(2) to CH 4 is an effective means of producing value-added fuels,common pho-tocatalysts have poor activity and low selectivity in photocatalytic CO_(2)-reduction processes.Even though creating defects is an effective photocatalyst fabrication route to improve photocatalytic activity,there are some challenges with the facile photocatalyst synthesis method.In this work,an O element is in-troduced into a graphitic carbon nitride(CN)skeleton through a precursory ultraviolet light irradiation pretreatment to increase the visible light absorption and enhance the carrier density of this modified non-metal CN photocatalyst;the charge transfer dynamics thereof are also studied through electrochem-ical tests,photoluminescence spectroscopy,and nanosecond transient absorption.We verify that the op-timized sample exhibits lower charge recombination and a suppressed 84 ns electron-trapping lifetime,compared to the 103 ns electron-trapping lifetime of the CN counterpart,and thereby contributes to ro-bust detrapping and a fast transfer of active electrons.Through density functional theory calculations,we find that the improved light absorption and increased electron density are ascribed to O-element doping,which enhances the CO_(2) adsorption energy and improves the CO_(2)-to-CH 4 photoreduction activity;it be-comes 17 times higher than that of the bare CN,and the selectivity is 3.8 times higher than that of CN.Moreover,the optimized sample demonstrates excellent cyclic stability in a 24-hour cycle test.
基金This study was supported through the National Research Foundation of Korea[NRF-2019M3F3A1A03079739 and NRF-2019R1A2C2003804]of the Ministry of Science and ICT,Republic of Korea.This study was partially supported by Leaders in Industryuniversity Cooperation+Project,supported by the Ministry of Education,Republic of Korea and by Ajou University.Minhwan Ko and Sang Yeon Lee contributed equally to this study.
文摘The strategy of a reliable transition temperature control of vanadium dioxide(VO2)is reported.Rectangular VO2 nanobeams were synthesized by a thermal chemical vapor deposition(TCVD)system.The metal-insulator transition(MIT)temperature increases to above 380K when the TiO2 ratio of the source is 5 at.%,although the Ti source is not physically doped into VO2 nanobeams.The XPS spectra of the V 2p orbital reveal the excessive oxidation of V after the TCVD processes with a higher TiO2 ratio,indicating that the TiO2 precursor is important in the O-doping of the surface V O bonds when forming volatile Ti-O gas species.Thus,TiO2 reactants can be used as a VO2 surface chemical modifier to manipulate the MIT transition temperature and maintain a homogenous VO2 phase,which is useful for a Mott device application with a record on/off switching ratio>104 and Mott transition temperature>380 K.
基金supported by the National Key Research and Development Program of China(2024YFA1209600 to Li L)the National Natural Science Foundation of China(52225304 and 52073210 to Li L,52403243 to Huang Y)。
文摘Organic semiconductors(OSCs)are showing great promise in large-area wearable devices,optoelectronic displays,logic circuits,and next-generation optoelectronic applications[1-9].Examples include organic field-effect transistors(OFETs),organic light-emitting diodes(OLEDs),organic photovoltaic cells(OPVs),and sensing devices.However,OSCs encounter significant challenges in widespread commercialization[10-13].Compared with their inorganic counterparts connected by strong covalent bonds,the structural characteristics of OSCs films are predominantly governed by van der Waals interactions[14-19],rendering their optoelectronic properties typically dependent on the synergistic effects between intrinsic properties and extrinsic effects,such as impurities and defects[20-26].
基金supported by the Natural Science Foundation of Shandong Province(Grant No.ZR2021ME143,ZR2020MA076).
文摘The enhancement of the photocatalytic activity of graphitic carbon nitride(g-C_(3)N_(4))depends on the rational design of its visible-light harvesting and charge separation/migration properties.Herein,an oxygen doping-induced intramolecular electron acceptor system enabling n→π^(*)electronic transitions in red g-C_(3)N_(4)nanosheets(Eg∼1.89 eV)was prepared via copolymerization with nitrilotriacetic acid(NTA)and urea.The n→π^(*)electronic transition can be controllably tuned,thus broadening the absorption spectrum of the system to∼750 nm.Simultaneously,doping with oxygen which acts as an electron acceptor,accelerates in-plane charge separation and migration.Moreover,this strategy was confirmed experimentally to be scalable for industrial mass production.Experiments and theoretical calculations demonstrated that the oxygen doping could continuously modulate the band gap(from∼2.65 to∼1.32 eV),resulting in the formation of an intramolecular electron acceptor system which enhances charge separation/migration kinetics.The optimized sample exhibited remarkable photocatalytic H_(2)and H_(2)O_(2)production rates of∼144.8µmol/h and∼539.76µM/h,respectively,which are higher than those for currently available g-C_(3)N_(4)-based photocatalysts.Significantly,the sample exhibited H_(2)and H_(2)O_(2)photocatalytic yields∼37.3 and∼30.1 times those of pristine g-C_(3)N_(4)under long-wavelength excitation(λ=520 nm).This study developed an effective and scalable strategy for the design and synthesis of full-spectrum photocatalysts for a broad range of applications.
基金supported by National Natural Science Foundation of China(Grant No.22278316).
文摘Heteroatom doping and defect engineering have been proposed as effective ways to modulate the energy band structure and improve the photocatalytic activity of g-C_(3)N_(4). In this work, ultrathin defective g-C_(3)N_(4) was successfully prepared using cold plasma. Plasma exfoliation reduces the thickness of g-C_(3)N_(4) from 10 nm to 3 nm, while simultaneously introducing a large number of nitrogen defects and oxygen atoms into g-C_(3)N_(4). The amount of doped O was regulated by varying the time and power of the plasma treatment. Due to N vacancies, O atoms formed strong bonds with C atoms, resulting in O doping in g-C_(3)N_(4). The mechanism of plasma treatment involves oxygen etching and gas expansion. Photocatalytic experiments demonstrated that appropriate amount of O doping improved the photocatalytic degradation of rhodamine B compared with pure g-C_(3)N_(4). The introduction of O optimized the energy band structure and photoelectric properties of g-C_(3)N_(4). Active species trapping experiments revealed ·O_(2)^(–) as the main active species during the degradation.
基金the National Natural Science Foundation of China(No.51578488)Zhejiang Provincial “151” Talents Program,the Program for Zhejiang Leading Team of S&T Innovation(No.2013TD07)Changjiang Scholar Incentive Program(Ministry of Education,China,2009)。
文摘Graphitic carbon nitride(g-C3N4,CN)exhibits inefficient charge separation,deficient CO2 adsorption and activation sites,and sluggish surface reaction kinetics,which have been recognized as the main barriers to its application in CO2 photocatalytic reduction.In this work,carbon quantum dot(CQD)decoration and oxygen atom doping were applied to CN by a facile one-step hydrothermal method.The incorporated CQDs not only facilitate charge transfer and separation,but also provide alternative CO2 adsorption and activation sites.Further,the oxygen-atom-doped CN(OCN),in which oxygen doping is accompanied by the formation of nitrogen defects,proves to be a sustainable H^+ provider by facilitating the water dissociation and oxidation half-reactions.Because of the synergistic effect of the hybridized binary CQDs/OCN addressing the three challenging issues of the CN based materials,the performance of CO2 photocatalytic conversion to CH4 over CQDs/OCN-x(x represents the volume ratio of laboratory-used H2O2(30 wt.%)in the mixed solution)is dramatically improved by 11 times at least.The hybrid photocatalyst design and mechanism proposed in this work could inspire more rational design and fabrication of effective photocatalysts for CO2 photocatalytic conversion with a high CH4 selectivity.
基金financially supported by the National Natural Science Foundation of China(Grants Nos.21976116 and 21902095)Shaanxi Science and Technology Program(2020KWZ005)+3 种基金SAFEA of China(High-end foreign expert project # G20190241013)Natural Foundation of Shaanxi Province(No.2020JQ-711)Group Linkage Program of Alexander-vonHumboldt Foundation of Germanythe scientific research startup fund of Shannxi University of Science and Technology。
文摘Engineering the electronic properties of semiconductor-based photocatalysts using elemental doping is an effective approach to improve their catalytic activity.Nevertheless,there still remain contradictions regarding the role of the dopants played in photocatalysis.Herein,ultrathin ZnIn_(2)S_(4)(ZIS) nanosheets with oxygen doping were synthesized by a one-pot solvothermal method.XRD,XPS and Raman spectral measurements support the presence of lattice oxygen in the oxygen-doped ZIS(O-ZIS) sample.With optimum doping of oxygen,the ultrathin O-ZIS nanosheets show enhanced CO_(2)-to-CO conversion activity with a CO_(2)-evolving rate of 1680 μmol h^(-1) g^(-1) under visible light irradiation,which is about 7 times higher than that of the pristine ZIS.First-principle calculations support that doping of oxygen in the lattice of ZnIn_(2)S_(4) nanosheets plays a key role in tuning its electronic properties.The remarkable photocatalytic performance of O-ZIS can be assigned to a synergistic consequence of a unique ultrathin-layered structure and an upward shift of the conduction band minimum(CBM) caused by the oxygen doping into ZIS and the quantum confinement effect(QCE) induced by the decreased particle size after doping as well as to the improved charge separation efficiency.The present work offers a simple elemental doping method to promote charge separation at atomic level and illustrates the roles played by oxygen doping in photocatalysis,giving new insights into highly efficient artificial photosynthesis.
基金Project supported by the Zhejiang Provincial Natural Science Foundation of China(No.LY17F040001)the Open Project Program of Surface Physics Laboratory(National Key Laboratory)of Fudan University(No.KF2015_02)+2 种基金the Open Project Program of National Laboratory for Infrared Physics,Chinese Academy of Sciences(No.M201503)the Zhejiang Provincial Science and Technology Key Innovation Team(No.2011R50012)the Zhejiang Provincial Key Laboratory(No.2013E10022)
文摘The influence of oxygen doping on resistive-switching characteristics of Ag/a-Si/p^＋-c-Si device was investigated. By oxygen doping in the growth process of amorphous silicon, the device resistive-switching performances, such as the ON/OFF resistance ratios, yield and stability were improved, which may be ascribed to the significant reduction of defect density because of oxygen incorporation. The device I-V characteristics are strongly dependent on the oxygen doping concentration. As the oxygen doping concentration increases, the Si-rich device gradually transforms to an oxygen-rich device, and the device yield, switching characteristics, and stability may be improved for silver/oxygen-doped a-Si/p^＋-c-Si device. Finally, the device resistive-switching mechanism was ana- lyzed. Key words： amorphous silicon; resistive switching; oxygen doping
基金The authors are grateful for the financial support provided by the National Natural Science Foundation of China(52362010,52304326,22305055,and 52274297)the Start-up Research Foundation of Hainan University(KYQD(ZR)-23069,20008,23067,and 23073)the specific research fund of the Innovation Platform for Academicians of Hainan Province(YSPTZX202315).
文摘Both sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)are considered as promising candidates in grid-level energy storage devices.Unfortunately,the larger ionic radii of K+and Na+induce poor diffusion kinetics and cycling stability of carbon anode materials.Pore structure regulation is an ideal strategy to promote the diffusion kinetics and cyclic stability of carbon materials by facilitating electrolyte infiltration,increasing the transport channels,and alleviating the volume change.However,traditional pore-forming agent-assisted methods considerably increase the difficulty of synthesis and limit practical applications of porous carbon materials.Herein,porous carbon materials(Ca-PC/Na-PC/K-PC)with different pore structures have been prepared with gluconates as the precursors,and the amorphous structure,abundant micropores,and oxygen-doping active sites endow the Ca-PC anode with excellent potassium and sodium storage performance.For PIBs,the capacitive contribution ratio of Ca-PC is 82%at 5.0 mV s^(-1) due to the introduction of micropores and high oxygen-doping content,while a high reversible capacity of 121.4 mAh g^(-1) can be reached at 5 A g^(-1) after 2000 cycles.For SIBs,stable sodium storage capacity of 101.4 mAh g^(-1) can be achieved at 2 A g^(-1) after 8000 cycles with a very low decay rate of 0.65%for per cycle.This work may provide an avenue for the application of porous carbon materials in the energy storage field.
基金supported by National Natural Science Foundation of China(Grant No.51772089 and 21872046)the Youth 1000 Talent Program of China+3 种基金the Outstanding Youth Scientist Foundation of Hunan Province(Grant No.2018JJ1009)the Natural Science Foundation of Hunan Province(Grant No.2020JJ4174)Provincial Science and Technology Innovation Platform and Talent Plan-Changsha,Zhuzhou and Xiangtan High-level Talents Accumulation Project(Grant No.2017XK2023)Research and Development Plan of Key Areas in Hunan Province(Grant No.2019GK2235)
文摘Heteroatom-doped meso/micro-porous carbon materials are conventionally produced by harsh carbonization under an inert atmosphere involving specific precursors,hard/soft templates,and heteroatom-containing agents.Herein,we report a facile synthesis of N and O co-doped meso/micro-porous carbon(NOMC)by template-free carbonization of a small-molecule precursor in a semi-closed system.The semi-closed carbonizaiton process yields hydrophilic NOMCs with large surface area in a high yield.The porous structure as well as the elemental composition of NOMCs can be modulated by changing the holding time at a particular temperature.NOMCs as metal-free heterogeneous catalysts can selectively oxidize benzyl alcohol and its derivatives into aldehydes/ketones with>85%conversion in aqueous solution,which is much higher than that of the control sample obtained in tube furnace(21%conversion),mainly due to their high N content,high percentage of pyridinic N,and large surface area.The presence of O-containing moieties also helps to improve the hydrophilicity and dispersion ability of catalysts and thus facilitates the mass transfer process during aqueous oxidation.The NOMC catalysts also dispayed excellent activity for a wide range of substrates with a selectivity of>99%.
基金financially supported by the National Key Research and Development Program of China (2017YFB0306504)the National Natural Science Foundation of China (22178154, 22108105, 21722604, and 21878133)+1 种基金the Postdoctoral Foundation of China (2017M611726)Graduate Education Innovation Project of Government of Jiangsu Province (KYCX20_3039)
文摘Oxygen atoms usually co-exist in the lattice of hexagonal boron nitride(h-BN). The understanding of interactions between the oxygen atoms and the adsorbate, however, is still ambiguous on improving adsorptive desulfurization performance. Herein, simultaneously oxygen atom-scale interior substitution and edge hydroxylation in BN structure were constructed via a polymer-based synthetic strategy.Experimental results indicated that the dual oxygen modified BN(BN–2O) exhibited an impressively increased adsorptive capacity about 12% higher than that of the edge hydroxylated BN(BN–OH) fabricated via a traditional method. The dibenzothiophene(DBT) was investigated to undergo multimolecular layer type coverage on the BN–2O uneven surface via π–π interaction, which was enhanced by the increased oxygen doping at the edges of BN–2O. The density functional theory calculations also unveiled that the oxygen atoms confined in BN interior structure could polarize the adsorbate, thereby resulting in a dipole interaction between the adsorbate and BN–2O. This effect endowed BN–2O with the ability to selectively adsorb DBT from the aromatic-rich fuel, thereafter leading to an impressive prospect for the adsorptive desulfurization performance of the fuel. The adsorptive result was in good accordance with Freundlich and pseudo-second-order adsorption kinetics model results. Therefore, the designing of a polymer-based strategy could be also extended to other heteroatom doping systems to enhance adsorptive performance.
基金supported by the National Natural Science Foundation of China(22008018)the China Postdoctoral Science Foundation(2020M670716).
文摘Highly efficient photon-to-electron conversion is crucial for achieving photocatalytic conversion.In this study,oxygen-doped carbon nitride nanocages(O@CNNCs)were engineered via dual strategies of morphology-controlled heteroatom doping,which was successfully used in the photocatalytic selective oxidation of xylose/xylan to xylonic acid.The nanocage-shaped O@CNNCs had a larger surface area,which was 4.02 times of carbon nitride(CN).Furthermore,with the assistance of morphology regulation and O-doping,O@CNNCs exhibit highly efficient photon-to-electron conversion,enhanced visible-light utilization,high photocurrent,low resistance,and fast separation/migration of electron-hole pairs.Correspondingly,the photocatalytic oxidation of xylose to xylonic acid using O@CNNCs was successfully achieved under mild reaction conditions with a yield of 83.4%.O@CNNCs have excellent recyclability,in which the yield of xylonic acid in the 5th cycle was 98.2%of its initial use.The O@CNNC photocatalytic system was also suitable for macromolecular xylan,and a xylonic acid yield of 77.34 mg was obtained when 100 mg xylan was used.The oxidation-active species captured experiments indicated that holes were crucial for the selective oxidation of xylose to xylonic acid.Overall,this study provides a new strategy for the preparation of photocatalysts with excellent photon-to-electron conversion and selective oxidation of biomass-derived feedstocks to xylonic acid.
基金supported by the National Natural Science Foundation of China (Nos.91741105,21173169)Chongqing Municipal Natural Science Foundation (No.cstc2018jcyjAX0625)。
文摘Transition-metal chalcogenides with hollow nanostructure,especially cobalt sulfides,are considered as the most pro mising non-precious metal catalysts for oxygen evolution reactio n.However,it is difficult to synthesize oxygen-containing cobalt sulphides with hollow structure due to the different physical/chemical properties between metal sulfides and metal cobalts.Herein,we report a novel oxygencontaining amorphous cobalt sulfide ball-in-ball hollow sphere s(Co-S-O BBHS) synthesized by an anion exchange method.Taking advantage of the ball-in-ball hollow structure,the amorphous Co-S-O BBHS shows supe rior oxygen evolution reaction(OER) electrocatalytic performance with a low overpotentiat of285 mV at 10 mA/cm2,small Tafel slope of 49.67 mV/dec,high Faraday efficiency of 96%,and satisfied durability.Experiments and DFT calculations demonstrate that the introduction of oxygen and sulfur modulates the electronic structure of Co-S-O BBHS,thus enhancing the adsorption of *0(adsorbed 0 species on catalyst surface) intermediate,which greatly boosts the catalytic activity towards OER.This work provides a new strategy for controllable synthe sis of complex hollow structures of transition-metal chalcogenides for OER.
基金financial support by the Program for the Outstanding Innovative Teams of Higher Learning Institutions of Shanxi(OIT)Shanxi Province Hundred Talent Project
文摘In recent decade, Au nanoclusters of atomic precision （AunLm, where L= organic ligand： thiolate andphosphine） have been shown as a new promising nanogold catalyst. The well-defined AunLm catalystspossess unique electronic properties and frameworks, providing an excellent opportunity to correlate theintrinsic catalytic behavior with the cluster＇s framework as well as to study the catalytic mechanismsover gold nanoclusters. In this review, we only demonstrate the important roles of the gold nanoclustersin the oxygen activation （e.g., 302 to 102） and their selective oxidations in the presence of oxygen （e.g., COto C02, sulfides to sulfoxides, alcohol to aldehyde, styrene to styrene epoxide, amines to imines, andglucose to gluconic acid）. The size-specificity （Au25 （1.3 nm）, Au38 （].5 nm）, Au144 （1.9 nm）, etc.）, ligandengineering （e.g., aromatic vs aliphatic）, and doping effects （e.g., copper, silver, palladium, and platinum）are discussed in details. Finally, the proposed reactions＇ mechanism and the relationships of clusters＇structure and activity at the atomic level also are presented.
基金supported by the National Natural Science Foundation of China under Grant Nos.51671053 and 51801021the Fundamental Research Funds for the Central Universities(No.N2302007)the Ministry of Industry and Information Technology Project(No.MJ-2017-J-99).
文摘The presence of excess Ta in high-temperature protective coatings can compromise the integrity of the Al_(2)O_(3)scale on the surface,which has a negative impact on the oxidation behavior and reduces the service life.The effects of oxygen doping on the isothermal oxidation of three sputtered nanocrystalline coatings were investigated at 1100°C.The results indicated that oxygen doping inhibited the diffusion of Ta from the coating to the oxide scale,which was primarily attributed to the preferential oxidation of the Al in the coating.However,excess oxygen doping decreased the amount of Al available for the formation of the Al_(2)O_(3)scale on the coating,thus reducing the inhibitory effect on Ta oxidation.Moreover,doping with excess O caused spalling of the oxide scale.Therefore,the right balance in O doping is crucial for suppressing Ta oxidation while maintaining the integrity of the oxide scale.
基金supported by National Key R&D Program of China(Grant No.2023YFB3712002)E.M.acknowledge National Natural Science Foundation of China(Grant No.52231001).
文摘Refractory multi-principal element alloys(RMPEAs)have garnered attention for their potential in high-temperature applications.Additive manufacturing(AM)provides opportunities to tailor RMPEAs’microstructures to enhance these properties.However,controlling defects and addressing the challenges posed by the complex thermal history during the AM process are crucial for optimizing RMPEAs’performance.This study aims to fabricate a high-quality oxygen-doped NbTiZr alloys using laser powder bed fusion and investigate their microstructure and mechanical properties.Our analysis reveals refined grain sizes and a periodic combination of fine near-equiaxed and columnar grain morphologies in the AM-fabricated alloy.Its substructure is characterized by the coexistence of loosely defined cellular dislocation networks and elemental segregation.Compared to its cast counterpart,the additively manufactured alloy exhibits a combination of high yield strength,excellent tensile ductility,and enhanced work hardening.These attributes make the AM-fabricated oxygen-doped NbTiZr alloy a promising candidate for applications required balanced mechanical properties.Understanding the specific effects of different crystal structures and deformation mechanisms is essential for optimizing AM processes to tailor the microstructure and achieve the desired mechanical performance in various engineering applications.
基金supported by the National Natural Science Foundation of China(22005164)the Natural Science Foundation of Shandong Province(BS2015CL002)the Basic Research Project of Qingdao Source Innovation Program Fund(17-1-1-82-jch)。
文摘To realize the continuous production of hydrogen energy,the efficient photocatalysts are required in the heterogeneous reaction for water splitting.Herein,we reported a surface modulation strategy,via doping oxygen atoms to tune the surface state of ZnIn_(2)S_(4)nanosheets with cocatalyst MoS_(2)modification,to enhance water adsorption and surface catalytic reaction for boosting the photocatalytic activity.Consequently,MoS_(2)/O-ZnIn_(2)S_(4)photocatalysts showed a remarkably superior photocatalytic H_(2)production performance of 4.002 mmol g^(-1)h^(-1)and an apparent quantum yield(AQY)of~2.53%,5.4 folds higher than ZnIn_(2)S_(4).Using operando infrared spectroscopy and DFT calculation,we revealed the dynamic structural evolution,as well as the active sites for water adsorption and the catalytic reaction at the MoS_(2)/O ZnIn_(2)S_(4)interface.This work reveals the effect of surface modulation on the photocatalytic activity for MoS_(2)/O-ZnIn_(2)S_(4)and offers a feasible method to devise excellent nanomaterial photocatalysts for H_(2)production.
基金This work was financially supported by the National Natural Science Foundation of China(No.51472164)Shenzhen Peacock Plan(No.KQTD2016053112042971)+3 种基金the Educational Commission of Guangdong Province(Nos.2015KGJHZ006 and 2016KCXTD006)the Science and Technology Planning Project of Guangdong Province(No.2016B050501005)A.T.S.W.acknowledges funding support from MOE Tier 2 grant R 144-000-382-112,A*STAR Pharos Program(No.1527300025)facility support from the NUS Centre for Advanced 2D Materials(CA2DM).
文摘Exposure to oxygen alters the physical and chemical properties of two-dimensional(2D)transition metal dichalcogenides(TMDs).In particular,oxygen in the ambient may influence the device stability of 2D TMDs over time.Engineering the doping of 2D TMDs,especially hole doping is highly desirable towards their device function.Herein,controllable oxygen-induced p-type doping in a range of hexagonal(MoTe2,WSe2,MoSe2 and PtSe2)and pentagonal(PdSe2)2D TMDs are demonstrated.Scanning tunneling microscopy,electrical transport and X-ray photoelectron spectroscopy are used to probe the origin of oxygen-derived hole doping.Three mechanisms are postulated that contribute to the hole doping in 2D TMDs,namely charge transfer from absorbed oxygen molecules,surface oxides,and chalcogen atom substitution.This work provides insights into the doping effects of oxygen,enabling the engineering of 2D TMDs properties for nanoelectronic applications.
基金supported by the National Natural Science Foundation of China(21503096,21407067)the Natural Science Foundation of Educational Committee of Anhui Province(KJ2018A0387),ChinaProject of Anhui Province for Excellent Young Talents in Universities(gxyq2019029),China
文摘Photocatalytic H2 production and CO2 reduction have attracted considerable attention for clean energy development.In this work,we designed an efficient photocatalyst by integrating lamellar oxygen-doped carbon nitride(CNO)nanosheets into ZnIn2S4(ZIS)microflowers by a one-step hydrothermal method.A well-fitted 2D hierarchical hybrid heterostructure was fabricated.Under visible light irradiation,the ZIS@CNO composite with 40 wt%CNO(ZC 40%)showed the highest hydrogen evolution rate from water(188.4μmol·h-1),which was approximately 2.1 times higher than those of CNO and ZIS(88.6 and 90.2μmol·h-1,respectively).Furthermore,the selective CO production rates of ZC 40%(12.69μmol·h-1)were 2.2 and 14.0 times higher than those of ZIS(5.85μmol·h-1)and CNO(0.91μmol·h-1),respectively,and the CH4 production rate of ZC 40%was 1.18μmol·h-1.This enhanced photocatalytic activity of CNO@ZIS is due mainly to the formation of a heterostructure that can promote the transfer of photoinduced electrons and holes between CNO and ZIS,thereby efficiently avoiding recombination of electron-hole pairs.
基金supported by the National Natural Science Foundation of China(12474317 and 62105269).
文摘Femtosecond laser ablation-driven periodic surface structuring offers a promising method for large-scale and high-throughput nanolithography technique.However,the self-organized periodic structures typically manifest constraints in terms of tunable period and depth,as well as suboptimal regularity,which restricts their broader application potential.Here,in terms of a rarely explored laser-induced photochemical mechanism for nonablative structuring,we demonstrate manufacturing of sub-wavelength oxidative grating structures on silicon films with active structural modulation.In this scenario,the plasmonic field plays a pivotal role in dragging oxygen ions from surface into the silicon,greatly speeding up oxidation rates.While high oxygen doping levels can already be achieved with single-pulse exposure,far superior results are obtained with the application of 40-MHz burst mode pulse trains,mitigating the formation of excessively large nanocrystallites.Furthermore,it is revealed that the periodicity and modulation depth of laser-writing nanograting are both dependent on the number of pulse per burst.This offers a convenient scheme for actively controlling laser plasmonic lithography.
