Graphitic carbon nitride nanosheets(CNNs)become the most promising member in the carbon nitride family benefitted from their two-dimensional structural features.Recently,great endeavors have been made in the synthesis...Graphitic carbon nitride nanosheets(CNNs)become the most promising member in the carbon nitride family benefitted from their two-dimensional structural features.Recently,great endeavors have been made in the synthesis and modification of CNNs to improve their photocatalytic properties,and many exciting progresses have been gained.In order to elucidate the fundamentals of CNNs based catalysts and provide the insights into rational design of photocatalysis system,we describe recent progress made in CNNs preparation strategies and their applications in this review.Firstly,the physicochemical properties of CNNs are briefly introduced.Secondly,the synthesis approaches of CNNs are reviewed,including top-down stripping strategies(thermal,gas,liquid,and composite stripping)and bottom-up precursor molecules design strategies(solvothermal,template,and supramolecular self-assembly method).Subsequently,the modification strategies based on CNNs in recent years are discussed,including crystal structure design,doping,surface functionalization,constructing 2D heterojunction,and anchoring single-atom.Then the multifunctional applications of g-C_(3)N_(4) nanosheet based materials in photocatalysis including H_(2) evolution,O_(2) evolution,overall water splitting,H_(2)O_(2) production,CO_(2) reduction,N_(2) fixation,pollutant removal,organic synthesis,and sensing are highlighted.Finally,the opportunities and challenges for the development of high-performance CNNs photocatalytic systems are also prospected.展开更多
As electromagnetic technology advances and demand for electronic devices grows,concerns about electromagnetic pollution intensify.This has spurred focused research on innovative electromagnetic absorbers,particularly ...As electromagnetic technology advances and demand for electronic devices grows,concerns about electromagnetic pollution intensify.This has spurred focused research on innovative electromagnetic absorbers,particularly chalcogenides,noted for their superior absorption capabilities.In this study,we successfully synthesize 3R–TaS_(2)nanosheets using a straightforward calcination method for the first time.These nanosheets exhibit significant absorption capabilities in both the C-band(4–8 GHz)and Ku-band(12–18 GHz)frequency ranges.By optimizing the calcination process,the complex permittivity of TaS_(2)is enhanced,specifically for those synthesized at 1000℃for 24 h.The nanosheets possess dual-band absorption properties,with a notable minimum reflection loss(RLmin)of41.4 dB in the C-band,and an average absorption intensity exceeding 10 dB in C-and Ku-bands,in the absorbers with a thickness of 5.6 mm.Additionally,the 3R–TaS_(2)nanosheets are demonstrated to have an effective absorption bandwidth of 5.04 GHz(3.84–8.88 GHz)in the absorbers with thicknesses of 3.5–5.5 mm.The results highlight the multiple reflection effects in 3R–TaS_(2)as caused by their stacked structures,which could be promising low-frequency absorbers.展开更多
Lysine is one of the essential amino acids for human body,and its imbalance is a major cause to anemia,aging process,leukemia cell proliferation and tumor growth.Therefore,its monitoring is dominative to the preventio...Lysine is one of the essential amino acids for human body,and its imbalance is a major cause to anemia,aging process,leukemia cell proliferation and tumor growth.Therefore,its monitoring is dominative to the prevention the disease progress and guidance to the clinical treatment.However,traditional inhospital detection methods,such as colorimetry and fluorometric,often suffer the disadvantages of high cost and long time-consuming.These drawbacks show a difficulty in the home-in and dairy monitoring for the lysine regulation in body.In this study,we have proposed an ultrasensitive microchipbased portable device to achieve the onsite and precise determination of lysine within only 10 s.This microchip was functionalized through constructing a center-concave nanosheet of core-shell WO_(3)@Prussian blue(WO_(3)@PB)to remarkably strengthen the generation and transfer of the detection signal.In this special architecture,the core WO_(3)nanosheet can be exposed at the center region of this nanocomposite to effectively promote the enzymatic oxidation,while the PB shell enables to strongly reduce the H_(2)O_(2)produced by the enzymatic reaction.Under above synergetic effects,a handheld device was designed to support the plug-and-play microchip,which performed an outstanding accuracy for the lysine detection in blood.展开更多
A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride(g-C3N4)nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework(MOF)is proposed in th...A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride(g-C3N4)nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework(MOF)is proposed in this study.Specifically,Co-MOF as an electron donor is capable of transferring the photogenerated electrons in the lowest unoccupied molecular orbital(LUMO)to the conduction band of g-C3N4 to facilitate charge separation.As expected,the prepared Co-MOF/g-C3N4 nanocomposites display excellent visible-light-driven photocatalytic CO2 reduction activities.The CO production rate of 6.75μmol g–1 h–1 and CH4 evolution rate of 5.47μmol g–1 h–1 are obtained,which are approximately 2 times those obtained with the original g-C3N4 under the same conditions.Based on a series of analyses,it is shown that the introduction of Co-MOF not only broadens the range of visible-light absorption but also enhances the charge separation,which improves the photocatalytic activity of g-C3N4 to a higher level.In particular,the hydroxyl radical(·OH)experiment was operated under 590 nm(single-wavelength)irradiation,which further proved that the photogenerated electrons in the LUMO of Co-MOF can successfully migrate to g-C3N4.This work may provide an important strategy for the design of highly efficient g-C3N4-based photocatalysts for CO2 reduction.展开更多
Wet chemistry methods,including hot-injection and precipitation methods,have emerged as major synthetic routes for high-quality perovskite nanocrystals in backlit display and scintillation applications.However,low che...Wet chemistry methods,including hot-injection and precipitation methods,have emerged as major synthetic routes for high-quality perovskite nanocrystals in backlit display and scintillation applications.However,low chemical yield hinders their upscale production for practical use.Meanwhile,the labile nature of halide-based perovskite poses a major challenge for long-term storage of perovskite nanocrystals.Herein,we report a green synthesis at room temperature for gram-scale production of CsPbBr3 nanosheets with minimum use of solvent,saving over 95% of the solvent for the unity mass nanocrystal production.The perovskite colloid exhibits record stability upon long-term storage for up to 8 months,preserving a photoluminescence quantum yield of 63% in solid state.Importantly,the colloidal nanosheets show self-assembly behavior upon slow solidification,generating a crack-free thin film in a large area.The uniform film was then demonstrated as an efficient scintillation screen for X-ray imaging.Our findings bring a scalable tool for synthesis of high-quality perovskite nanocrystals,which may inspire the industrial optoelectronic application of large-area perovskite film.展开更多
Constructing binary heterojunctions is an important strategy to improve the photocatalytic performance of graphitic carbon nitride(g‐C3N4).In this paper,a novel g‐C3N4 nanosheet‐based composite was constructed via ...Constructing binary heterojunctions is an important strategy to improve the photocatalytic performance of graphitic carbon nitride(g‐C3N4).In this paper,a novel g‐C3N4 nanosheet‐based composite was constructed via in situ growth of bismuth oxyiodide(BiOI)nanoplates on the surface of g‐C3N4 nanosheets.The crystal phase,microstructure,optical absorption and textural properties of the synthesized photocatalysts were analyzed by X‐ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),ultraviolet‐visible(UV‐vis)diffuse reflectance spectroscopy(DRS),and nitrogen adsorption‐desorption isotherm measurements.The BiOI/g‐C3N4 nanosheet composite showed high activity and recyclability for the photodegradation of the target pollutant rhodamine B(RhB).The conversion of RhB(20 mg L?1)by the photocatalyst was nearly 100%after 50 min under visible‐light irradiation.The high photoactivity of the BiOI/g‐C3N4 nanosheet composite can be attributed to the enhanced visible‐light absorption of the g‐C3N4 nanosheets sensitized by BiOI nanoplates as well as the high charge separation efficiency obtained by the establishment of an internal electric field between the n‐type g‐C3N4 and p‐type BiOI.Based on the characterization and experimental results,a double‐transfer mechanism of the photoinduced electrons in the BiOI/g‐C3N4 nanosheet composite was proposed to explain its activity.This work represents a new strategy to understand and realize the design and synthesis of g‐C3N4 nanosheet‐based heterojunctions that display highly efficient charge separation and transfer.展开更多
In this study, the effect of reduced graphene oxide(rGO) on interconnected Co_3O_4 nanosheets and the improved supercapacitive behaviors is reported. By optimizing the experimental parameters, we achieved a specific c...In this study, the effect of reduced graphene oxide(rGO) on interconnected Co_3O_4 nanosheets and the improved supercapacitive behaviors is reported. By optimizing the experimental parameters, we achieved a specific capacitance of ~1016.4 F g^(-1) for the Co_3O_4/rGO/NF(nickel foam) system at a current density of 1 A g^(-1). However, the Co_3O_4/NF structure without rGO only delivers a specific capacitance of ~520.0 F g^(-1)at the same current density. The stability test demonstrates that Co_3O_4/rGO/NF retains ~95.5% of the initial capacitance value even after 3000 charge–discharge cycles at a high current density of 7 A g^(-1). Further investigation reveals that capacitance improvement for the Co_3O_4/rGO/NF structure is mainly because of a higher specific surface area(~87.8 m^2g^(-1))and a more optimal mesoporous size(4–15 nm) compared to the corresponding values of 67.1 m^2g^(-1) and 6–25 nm,respectively, for the Co_3O_4/NF structure. rGO and the thinner Co_3O_4 nanosheets benefit from the strain relaxation during the charge and discharge processes, improving the cycling stability of Co_3O_4/rGO/NF.展开更多
PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution o...PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g^–1 h^–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g^–1 h^–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.展开更多
Searching for advanced anode materials with excellent electrochemical properties in sodium-ion battery is essential and imperative for next-generation energy storage system to solve the energy shortage problem.In this...Searching for advanced anode materials with excellent electrochemical properties in sodium-ion battery is essential and imperative for next-generation energy storage system to solve the energy shortage problem.In this work,two-dimensional(2D)ultrathin FePS3 nanosheets,a typical ternary metal phosphosulfide,are first prepared by ultrasonic exfoliation.The novel 2D/2D heterojunction of FePS3 nanosheets@MXene composite is then successfully synthesized by in situ mixing ultrathin MXene nanosheets with FePS3 nanosheets.The resultant FePS3 nanosheets@MXene hybrids can increase the electronic conductivity and specific surface area,assuring excellent surface and interfacial charge transfer abilities.Furthermore,the unique heterojunction endows FePS3 nanosheets@MXene composite to promote the diffusion of Na^+ and alleviate the drastic change in volume in the cyclic process,enhancing the sodium storage capability.Consequently,the few-layered FePS3 nanosheets uniformly coated by ultrathin MXene provide an exceptional reversible capacity of 676.1 mAh g^−1 at the current of 100 mA g^−1 after 90 cycles,which is equivalent to around 90.6% of the second-cycle capacity(746.4 mAh g^−1).This work provides an original protocol for constructing 2D/2D material and demonstrates the FePS3@MXene composite as a potential anode material with excellent property for sodium-ion batteries.展开更多
Herein, combining solverthermal route and electrodeposition, we grew unique hybrid nanosheet arrays consisting of Co_3O_4 nanosheet as a core, PPy as a shell. Benefiting from the PPy as conducting polymer improving an...Herein, combining solverthermal route and electrodeposition, we grew unique hybrid nanosheet arrays consisting of Co_3O_4 nanosheet as a core, PPy as a shell. Benefiting from the PPy as conducting polymer improving an electron transport rate as well as synergistic effects from such a core/shell structure, a hybrid electrode made of the Co_3O_4@PPy core/shell nanosheet arrays exhibits a large areal capacitance of 2.11 F cm-2at the current density of 2 m A cm^(-2), a *4-fold enhancement compared with the pristine Co_3O_4electrode; furthermore, this hybrid electrode also displays good rate capability(*65 % retention of the initial capacitance from 2 to 20 m A cm^(-2)) and superior cycling performance(*85.5 % capacitance retention after 5000 cycles). In addition, the equivalent series resistance value of the Co_3O_4@PPy hybrid electrode(0.238 X) is significantly lower than that of the pristine Co_3O_4electrode(0.319 X). These results imply that the Co_3O_4@PPy hybrid composites have a potential for fabricating next-generation energy storage and conversion devices.展开更多
Photoanodes based on In_2S_3/ZnO heterojunction nanosheet arrays(NSAs) have been fabricated by atomic layer deposition of ZnO over In_2S_3 NSAs, which were in situ grown on fluorine-doped tin oxide glasses via a facil...Photoanodes based on In_2S_3/ZnO heterojunction nanosheet arrays(NSAs) have been fabricated by atomic layer deposition of ZnO over In_2S_3 NSAs, which were in situ grown on fluorine-doped tin oxide glasses via a facile solvothermal process. The as-prepared photoanodes show dramatically enhanced performance for photoelectrochemical(PEC) water splitting, compared to single semiconductor counterparts. The optical and PEC properties of In_2S_3/ZnO NSAs have been optimized by modulating the thickness of the Zn O overlayer. After pairing with ZnO, the NSAs exhibit a broadened absorption range and an increased light absorptance over a wide wavelength region of 250–850 nm. The optimized sample of In_2S_3/ZnO-50 NSAs shows a photocurrent density of 1.642 m A cm^(-2)(1.5 V vs. RHE) and an incident photonto-current efficiency of 27.64% at 380 nm(1.23 V vs.RHE), which are 70 and 116 times higher than those of the pristine In_2S_3 NSAs, respectively. A detailed energy band edge analysis reveals the type-II band alignment of the In_2S_3/ZnO heterojunction, which enables efficient separation and collection of photogenerated carriers,especially with the assistance of positive bias potential, and then results in the significantly increased PEC activity.展开更多
Exfoliation of bulk graphitic carbon nitride(g‐C3N4)into two‐dimensional(2D)nanosheets is one of the effective strategies to improve its photocatalytic properties so that the 2D g‐C3N4 nanosheets(CN)have larger spe...Exfoliation of bulk graphitic carbon nitride(g‐C3N4)into two‐dimensional(2D)nanosheets is one of the effective strategies to improve its photocatalytic properties so that the 2D g‐C3N4 nanosheets(CN)have larger specific surface areas and more reaction sites.In addition,poly‐o‐phenylenediamine(PoPD)can improve the electrical conductivity and photocatalytic activity of semiconductor materials.Here,the novel efficient composite PoPD/AgCl/g‐C3N4 nanosheets was first synthesized by a precipitation reaction and the photoinitiated polymerization approach.The obtained photocatalysts have larger specific surface areas and could achieve better visible‐light response.However,silver chloride(AgCl)is susceptible to agglomeration and photocorrosion.The PoPD/AgCl/CN composite exhibits an extremely high photocurrent density,which is three times that of CN.Obviously enhanced photocatalytic activities of PoPD/AgCl/g‐C3N4 are revealed through the photodegradation of tetracycline.The stability of PoPD/AgCl/CN is demonstrated based on four cycles of experiments that reveal that the degradation rate only decreases slightly.Furthermore,.O2^-and h+are the main active species,which are confirmed through a trapping experiment and ESR spin‐trap technique.Therefore,the prepared PoPD/AgCl/CN can be considered as a stable photocatalyst,in which PoPD is added as a charge carrier and acts a photosensitive protective layer on the surface of the AgCl particles.This provides a new technology for preparing highly stable composite photocatalysts that can effectively deal with environmental issues.展开更多
In the pursuit of stable,high performance Ni-based oxygen evolution reaction(OER)electrocatalysts,modifying the local chemical compositions or fabricating hybrid nanostructures to generate abundant interfaces for impr...In the pursuit of stable,high performance Ni-based oxygen evolution reaction(OER)electrocatalysts,modifying the local chemical compositions or fabricating hybrid nanostructures to generate abundant interfaces for improving the water oxidation activity of electrocatalysts has emerged as an effective strategy.Herein,we report the facile development of a Ni_(3)S_(2)-CeO_(2)hybrid nanostructure via an electrodeposition method.Benefiting from the strong interfacial interaction between Ni_(3)S_(2)and CeO_(2),the electron transfer is notably improved and the water oxidation activity of Ni_(3)S_(2)nanosheets is significantly enhanced.In 1.0 M KOH,the Ni_(3)S_(2)-CeO_(2)electrocatalyst achieves a current density of 20 mA cm-2 at a low overpotential of 264 mV,which is 92 mV lower than that of Ni_(3)S_(2).Moreover,Ni_(3)S_(2)-CeO_(2)exhibits superior electrochemical stability.Density functional theory calculations demonstrate that the enhanced OER electrocatalytic performance of Ni_(3)S_(2)-CeO_(2)can be ascribed to an increase in the binding strength of the reaction intermediates at the Ni_(3)S_(2)-CeO_(2)interface.展开更多
基金supported by the National Natural Science Foundation of China(22172195)Central South University Graduate Students Independent Exploration and Innovation Project(2023ZZTS0736 and 2023ZZTS0760).
文摘Graphitic carbon nitride nanosheets(CNNs)become the most promising member in the carbon nitride family benefitted from their two-dimensional structural features.Recently,great endeavors have been made in the synthesis and modification of CNNs to improve their photocatalytic properties,and many exciting progresses have been gained.In order to elucidate the fundamentals of CNNs based catalysts and provide the insights into rational design of photocatalysis system,we describe recent progress made in CNNs preparation strategies and their applications in this review.Firstly,the physicochemical properties of CNNs are briefly introduced.Secondly,the synthesis approaches of CNNs are reviewed,including top-down stripping strategies(thermal,gas,liquid,and composite stripping)and bottom-up precursor molecules design strategies(solvothermal,template,and supramolecular self-assembly method).Subsequently,the modification strategies based on CNNs in recent years are discussed,including crystal structure design,doping,surface functionalization,constructing 2D heterojunction,and anchoring single-atom.Then the multifunctional applications of g-C_(3)N_(4) nanosheet based materials in photocatalysis including H_(2) evolution,O_(2) evolution,overall water splitting,H_(2)O_(2) production,CO_(2) reduction,N_(2) fixation,pollutant removal,organic synthesis,and sensing are highlighted.Finally,the opportunities and challenges for the development of high-performance CNNs photocatalytic systems are also prospected.
基金supported by the National Natural Science Foundation of China(52372289,52102368,52072192 and 51977009)Regional Joint Fund for Basic Research and Applied Basic Research of Guangdong Province(No.2020A1515110905)+1 种基金Guangdong Special Fund for key Areas(20237DZX3042)Shenzhen Stable Support Project.
文摘As electromagnetic technology advances and demand for electronic devices grows,concerns about electromagnetic pollution intensify.This has spurred focused research on innovative electromagnetic absorbers,particularly chalcogenides,noted for their superior absorption capabilities.In this study,we successfully synthesize 3R–TaS_(2)nanosheets using a straightforward calcination method for the first time.These nanosheets exhibit significant absorption capabilities in both the C-band(4–8 GHz)and Ku-band(12–18 GHz)frequency ranges.By optimizing the calcination process,the complex permittivity of TaS_(2)is enhanced,specifically for those synthesized at 1000℃for 24 h.The nanosheets possess dual-band absorption properties,with a notable minimum reflection loss(RLmin)of41.4 dB in the C-band,and an average absorption intensity exceeding 10 dB in C-and Ku-bands,in the absorbers with a thickness of 5.6 mm.Additionally,the 3R–TaS_(2)nanosheets are demonstrated to have an effective absorption bandwidth of 5.04 GHz(3.84–8.88 GHz)in the absorbers with thicknesses of 3.5–5.5 mm.The results highlight the multiple reflection effects in 3R–TaS_(2)as caused by their stacked structures,which could be promising low-frequency absorbers.
基金financially supported by the National Key Research and Development Program of China(2021YFC2103300)the National Natural Science Foundation of China Youth Found(22308154 and 22108120)the Natural Science Foundation of Jiangsu Province(BK20231518 and BK20210549).
文摘Lysine is one of the essential amino acids for human body,and its imbalance is a major cause to anemia,aging process,leukemia cell proliferation and tumor growth.Therefore,its monitoring is dominative to the prevention the disease progress and guidance to the clinical treatment.However,traditional inhospital detection methods,such as colorimetry and fluorometric,often suffer the disadvantages of high cost and long time-consuming.These drawbacks show a difficulty in the home-in and dairy monitoring for the lysine regulation in body.In this study,we have proposed an ultrasensitive microchipbased portable device to achieve the onsite and precise determination of lysine within only 10 s.This microchip was functionalized through constructing a center-concave nanosheet of core-shell WO_(3)@Prussian blue(WO_(3)@PB)to remarkably strengthen the generation and transfer of the detection signal.In this special architecture,the core WO_(3)nanosheet can be exposed at the center region of this nanocomposite to effectively promote the enzymatic oxidation,while the PB shell enables to strongly reduce the H_(2)O_(2)produced by the enzymatic reaction.Under above synergetic effects,a handheld device was designed to support the plug-and-play microchip,which performed an outstanding accuracy for the lysine detection in blood.
基金supported by the National Natural Science Foundation of China(21871079,21501052)the Outstanding Youth Project of Natural Science Foundation of Heilongjiang Province(YQ2019B006)~~
文摘A possible mechanism for boosting the visible-light photoactivities of graphitic carbon nitride(g-C3N4)nanosheets for CO2 reduction via coupling with the electron donor Co-metal-organic framework(MOF)is proposed in this study.Specifically,Co-MOF as an electron donor is capable of transferring the photogenerated electrons in the lowest unoccupied molecular orbital(LUMO)to the conduction band of g-C3N4 to facilitate charge separation.As expected,the prepared Co-MOF/g-C3N4 nanocomposites display excellent visible-light-driven photocatalytic CO2 reduction activities.The CO production rate of 6.75μmol g–1 h–1 and CH4 evolution rate of 5.47μmol g–1 h–1 are obtained,which are approximately 2 times those obtained with the original g-C3N4 under the same conditions.Based on a series of analyses,it is shown that the introduction of Co-MOF not only broadens the range of visible-light absorption but also enhances the charge separation,which improves the photocatalytic activity of g-C3N4 to a higher level.In particular,the hydroxyl radical(·OH)experiment was operated under 590 nm(single-wavelength)irradiation,which further proved that the photogenerated electrons in the LUMO of Co-MOF can successfully migrate to g-C3N4.This work may provide an important strategy for the design of highly efficient g-C3N4-based photocatalysts for CO2 reduction.
基金supported by National Natural Science Foundation of China (Nos. 21805111 and 11405073)Taishan Scholar Fund
文摘Wet chemistry methods,including hot-injection and precipitation methods,have emerged as major synthetic routes for high-quality perovskite nanocrystals in backlit display and scintillation applications.However,low chemical yield hinders their upscale production for practical use.Meanwhile,the labile nature of halide-based perovskite poses a major challenge for long-term storage of perovskite nanocrystals.Herein,we report a green synthesis at room temperature for gram-scale production of CsPbBr3 nanosheets with minimum use of solvent,saving over 95% of the solvent for the unity mass nanocrystal production.The perovskite colloid exhibits record stability upon long-term storage for up to 8 months,preserving a photoluminescence quantum yield of 63% in solid state.Importantly,the colloidal nanosheets show self-assembly behavior upon slow solidification,generating a crack-free thin film in a large area.The uniform film was then demonstrated as an efficient scintillation screen for X-ray imaging.Our findings bring a scalable tool for synthesis of high-quality perovskite nanocrystals,which may inspire the industrial optoelectronic application of large-area perovskite film.
文摘Constructing binary heterojunctions is an important strategy to improve the photocatalytic performance of graphitic carbon nitride(g‐C3N4).In this paper,a novel g‐C3N4 nanosheet‐based composite was constructed via in situ growth of bismuth oxyiodide(BiOI)nanoplates on the surface of g‐C3N4 nanosheets.The crystal phase,microstructure,optical absorption and textural properties of the synthesized photocatalysts were analyzed by X‐ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),ultraviolet‐visible(UV‐vis)diffuse reflectance spectroscopy(DRS),and nitrogen adsorption‐desorption isotherm measurements.The BiOI/g‐C3N4 nanosheet composite showed high activity and recyclability for the photodegradation of the target pollutant rhodamine B(RhB).The conversion of RhB(20 mg L?1)by the photocatalyst was nearly 100%after 50 min under visible‐light irradiation.The high photoactivity of the BiOI/g‐C3N4 nanosheet composite can be attributed to the enhanced visible‐light absorption of the g‐C3N4 nanosheets sensitized by BiOI nanoplates as well as the high charge separation efficiency obtained by the establishment of an internal electric field between the n‐type g‐C3N4 and p‐type BiOI.Based on the characterization and experimental results,a double‐transfer mechanism of the photoinduced electrons in the BiOI/g‐C3N4 nanosheet composite was proposed to explain its activity.This work represents a new strategy to understand and realize the design and synthesis of g‐C3N4 nanosheet‐based heterojunctions that display highly efficient charge separation and transfer.
基金financially supported from the National Natural Science Foundation of China (Grant Nos.: 61376068, 11304132, 11304133, and 11405144)the Specialized Research Fund of the Doctoral Program of Higher Education (Grant Nos.: 20120211120003 and 20130211120009)the Fundamental Research Funds for the Central Universities (Grant Nos.: lzujbky2013-36 and lzujbky-2014-30)
文摘In this study, the effect of reduced graphene oxide(rGO) on interconnected Co_3O_4 nanosheets and the improved supercapacitive behaviors is reported. By optimizing the experimental parameters, we achieved a specific capacitance of ~1016.4 F g^(-1) for the Co_3O_4/rGO/NF(nickel foam) system at a current density of 1 A g^(-1). However, the Co_3O_4/NF structure without rGO only delivers a specific capacitance of ~520.0 F g^(-1)at the same current density. The stability test demonstrates that Co_3O_4/rGO/NF retains ~95.5% of the initial capacitance value even after 3000 charge–discharge cycles at a high current density of 7 A g^(-1). Further investigation reveals that capacitance improvement for the Co_3O_4/rGO/NF structure is mainly because of a higher specific surface area(~87.8 m^2g^(-1))and a more optimal mesoporous size(4–15 nm) compared to the corresponding values of 67.1 m^2g^(-1) and 6–25 nm,respectively, for the Co_3O_4/NF structure. rGO and the thinner Co_3O_4 nanosheets benefit from the strain relaxation during the charge and discharge processes, improving the cycling stability of Co_3O_4/rGO/NF.
基金supported by the National Natural Science Foundation of China(51572295,21273285,21003157)the Beijing Nova Program(2008B76)the Science Foundation of China University of Petroleum Beijing(KYJJ2012-06-20 and 2462016YXBS05)~~
文摘PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g^–1 h^–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g^–1 h^–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.
基金support funding is from the National Natural Science Foundation of China(51871119 and 51901100)China Jiangsu Specially Appointed Professor,Jiangsu Provincial Founds for Natural Science Foundation(BK20170793 and BK20180015)+2 种基金China Postdoctoral Science Foundation(2018M640481 and 2019T120426)Jiangsu Postdoctoral Research Fund(2019K003 and 2019K201)Jiangsu-Innovate UK Business Competition(BZ2017061)
文摘Searching for advanced anode materials with excellent electrochemical properties in sodium-ion battery is essential and imperative for next-generation energy storage system to solve the energy shortage problem.In this work,two-dimensional(2D)ultrathin FePS3 nanosheets,a typical ternary metal phosphosulfide,are first prepared by ultrasonic exfoliation.The novel 2D/2D heterojunction of FePS3 nanosheets@MXene composite is then successfully synthesized by in situ mixing ultrathin MXene nanosheets with FePS3 nanosheets.The resultant FePS3 nanosheets@MXene hybrids can increase the electronic conductivity and specific surface area,assuring excellent surface and interfacial charge transfer abilities.Furthermore,the unique heterojunction endows FePS3 nanosheets@MXene composite to promote the diffusion of Na^+ and alleviate the drastic change in volume in the cyclic process,enhancing the sodium storage capability.Consequently,the few-layered FePS3 nanosheets uniformly coated by ultrathin MXene provide an exceptional reversible capacity of 676.1 mAh g^−1 at the current of 100 mA g^−1 after 90 cycles,which is equivalent to around 90.6% of the second-cycle capacity(746.4 mAh g^−1).This work provides an original protocol for constructing 2D/2D material and demonstrates the FePS3@MXene composite as a potential anode material with excellent property for sodium-ion batteries.
基金financially supported by the National Natural Science Foundation of China(Grant No.2117103551472049 and 51302035)+7 种基金the Key Grant Project of Chinese Ministry of Education(Grant No.313015)the PhD Programs Foundation of the Ministry of Education of China(Grant No.20110075110008 and20130075120001)the National 863 Program of China(Grant No.2013AA031903)the Science and Technology Commission of Shanghai Municipality(Grant No.13ZR1451200)the Fundamental Research Funds for the Central Universitiesthe Program Innovative Research Team in University(IRT1221)the Shanghai Leading Academic Discipline Project(Grant No.B603)the Program of Introducing Talents of Discipline to Universities(No.111-2-04)
文摘Herein, combining solverthermal route and electrodeposition, we grew unique hybrid nanosheet arrays consisting of Co_3O_4 nanosheet as a core, PPy as a shell. Benefiting from the PPy as conducting polymer improving an electron transport rate as well as synergistic effects from such a core/shell structure, a hybrid electrode made of the Co_3O_4@PPy core/shell nanosheet arrays exhibits a large areal capacitance of 2.11 F cm-2at the current density of 2 m A cm^(-2), a *4-fold enhancement compared with the pristine Co_3O_4electrode; furthermore, this hybrid electrode also displays good rate capability(*65 % retention of the initial capacitance from 2 to 20 m A cm^(-2)) and superior cycling performance(*85.5 % capacitance retention after 5000 cycles). In addition, the equivalent series resistance value of the Co_3O_4@PPy hybrid electrode(0.238 X) is significantly lower than that of the pristine Co_3O_4electrode(0.319 X). These results imply that the Co_3O_4@PPy hybrid composites have a potential for fabricating next-generation energy storage and conversion devices.
基金sponsored by the National Natural Science Foundation of China (Nos. 51402190, 61574091)Shanghai Sailing Program (18YF1427800)the special funds for theoretical physics of the National Natural Science Foundation of China (No. 11747029)
文摘Photoanodes based on In_2S_3/ZnO heterojunction nanosheet arrays(NSAs) have been fabricated by atomic layer deposition of ZnO over In_2S_3 NSAs, which were in situ grown on fluorine-doped tin oxide glasses via a facile solvothermal process. The as-prepared photoanodes show dramatically enhanced performance for photoelectrochemical(PEC) water splitting, compared to single semiconductor counterparts. The optical and PEC properties of In_2S_3/ZnO NSAs have been optimized by modulating the thickness of the Zn O overlayer. After pairing with ZnO, the NSAs exhibit a broadened absorption range and an increased light absorptance over a wide wavelength region of 250–850 nm. The optimized sample of In_2S_3/ZnO-50 NSAs shows a photocurrent density of 1.642 m A cm^(-2)(1.5 V vs. RHE) and an incident photonto-current efficiency of 27.64% at 380 nm(1.23 V vs.RHE), which are 70 and 116 times higher than those of the pristine In_2S_3 NSAs, respectively. A detailed energy band edge analysis reveals the type-II band alignment of the In_2S_3/ZnO heterojunction, which enables efficient separation and collection of photogenerated carriers,especially with the assistance of positive bias potential, and then results in the significantly increased PEC activity.
基金supported by the National Natural Science Foundation of China(21576125,21776117)the China Postdoctoral Science Foundation(2017M611716,2017M611734)+1 种基金the Six talent peaks project of Jiangsu Province(XCL-014)the Zhenjiang Science&Technology Program(SH2016012)~~
文摘Exfoliation of bulk graphitic carbon nitride(g‐C3N4)into two‐dimensional(2D)nanosheets is one of the effective strategies to improve its photocatalytic properties so that the 2D g‐C3N4 nanosheets(CN)have larger specific surface areas and more reaction sites.In addition,poly‐o‐phenylenediamine(PoPD)can improve the electrical conductivity and photocatalytic activity of semiconductor materials.Here,the novel efficient composite PoPD/AgCl/g‐C3N4 nanosheets was first synthesized by a precipitation reaction and the photoinitiated polymerization approach.The obtained photocatalysts have larger specific surface areas and could achieve better visible‐light response.However,silver chloride(AgCl)is susceptible to agglomeration and photocorrosion.The PoPD/AgCl/CN composite exhibits an extremely high photocurrent density,which is three times that of CN.Obviously enhanced photocatalytic activities of PoPD/AgCl/g‐C3N4 are revealed through the photodegradation of tetracycline.The stability of PoPD/AgCl/CN is demonstrated based on four cycles of experiments that reveal that the degradation rate only decreases slightly.Furthermore,.O2^-and h+are the main active species,which are confirmed through a trapping experiment and ESR spin‐trap technique.Therefore,the prepared PoPD/AgCl/CN can be considered as a stable photocatalyst,in which PoPD is added as a charge carrier and acts a photosensitive protective layer on the surface of the AgCl particles.This provides a new technology for preparing highly stable composite photocatalysts that can effectively deal with environmental issues.
文摘In the pursuit of stable,high performance Ni-based oxygen evolution reaction(OER)electrocatalysts,modifying the local chemical compositions or fabricating hybrid nanostructures to generate abundant interfaces for improving the water oxidation activity of electrocatalysts has emerged as an effective strategy.Herein,we report the facile development of a Ni_(3)S_(2)-CeO_(2)hybrid nanostructure via an electrodeposition method.Benefiting from the strong interfacial interaction between Ni_(3)S_(2)and CeO_(2),the electron transfer is notably improved and the water oxidation activity of Ni_(3)S_(2)nanosheets is significantly enhanced.In 1.0 M KOH,the Ni_(3)S_(2)-CeO_(2)electrocatalyst achieves a current density of 20 mA cm-2 at a low overpotential of 264 mV,which is 92 mV lower than that of Ni_(3)S_(2).Moreover,Ni_(3)S_(2)-CeO_(2)exhibits superior electrochemical stability.Density functional theory calculations demonstrate that the enhanced OER electrocatalytic performance of Ni_(3)S_(2)-CeO_(2)can be ascribed to an increase in the binding strength of the reaction intermediates at the Ni_(3)S_(2)-CeO_(2)interface.
