Ag3PO4 microcrystals with highly enhanced visible light photocatalytic activity are prepared by a facile and simple solid state reaction at room temperature. The composition, morphology and optical properties of the a...Ag3PO4 microcrystals with highly enhanced visible light photocatalytic activity are prepared by a facile and simple solid state reaction at room temperature. The composition, morphology and optical properties of the asprepared Ag3PO4 microcrystMs are characterized by x-ray diffraction, scanning electron microscopy and UV-vis diffuse reflectance spectra. The photocatalytie properties of Ag3PO4 are investigated by the degradation of both methylene blue and methyl orange dyes under visible light irradiation. The as-prepared Ag3PO4 microcrystals possess high photocatalytic oxygen production with the rate of 673μmolh-1g-1. Moreover, the as-prepared Ag3PO4 microcrystals show an enhanced photoelectrochemistry performance under irradiation of visible light.展开更多
This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and ...This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and status are investigated.A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio(72%S).In contrast,a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio(44%S).In carbonate ester electrolyte,only the sulfur trapped in porous structures is active via‘solid-solid’behavior during cycling.The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents.To improve the capacity of the sulfur-rich cathode,ether electrolyte with NaNO_(3) additive is explored to realize a‘solid-liquid’sulfur redox process and confine the shuttle effect of the dissolved polysulfides.As a result,the sulfur-rich cathode achieved high reversible capacity(483 mAh g^(−1)),corresponding to a specific energy of 362 Wh kg^(−1) after 200 cycles,shedding light on the use of ether electrolyte for high-loading sulfur cathode.展开更多
The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(>...The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(> 400 ℃) conditions.Herein, a highly active catalytic conversion process of ethane at room temperature(25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-coordination structures.Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C2 chemicals, simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O–FeN4–O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals.This work deepens the understanding of alkane C–H activation on the FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane.展开更多
Zinc oxide(ZnO) doped with erbium at different concentrations was synthesized by solid-state reaction method and characterized by X-ray diffraction(XRD), scanning electron microscopic(SEM), UVabsorption spectroscopy, ...Zinc oxide(ZnO) doped with erbium at different concentrations was synthesized by solid-state reaction method and characterized by X-ray diffraction(XRD), scanning electron microscopic(SEM), UVabsorption spectroscopy, photoluminescence(PL) study and vibrating sample magnetometer. The XRD studies exhibit the presence of wurtzite crystal structure similar to the parent compound ZnO in 1% Er^(3+)doped Zn O,suggesting that doped Er^(3+)ions sit at the regular Zn^(2+)sites. However, same studies spread over the samples with Er^(3+)content>1% reveals the occurrence of secondary phase. SEM images of 1% Er^(3+)doped ZnO show the polycrystalline nature of the synthesized sample. UV-visible absorption spectrum of Er^(3+)doped ZnO nanocrystals shows a strong absorption peak at 388 nm due to ZnO band to band transition. The PL study exhibits emission in the visible region, due to excitonic as well as defect related transitions. The magnetizationfield curve of Er^(3+)doped ZnO nanocrystals showed ferromagnetic property at room-temperature.展开更多
Photoresponsive materials are considered as promising systems for intelligent technology applications owing to the contactless spatial and temporal control.Herein,controllable multi-photoresponsive behaviors are reali...Photoresponsive materials are considered as promising systems for intelligent technology applications owing to the contactless spatial and temporal control.Herein,controllable multi-photoresponsive behaviors are realized in benzo[b]thiophene derivatives(o-DMP-S,o-DMP-SO,and o-DMP-SO_(2))by modulating the sulfur oxidation state.Among them,o-DMP-S is photo-unreactive but possesses denser molecular packing upon ultraviolet(UV)light irradiation,exhibiting photoenhanced room-temperature phosphorescence properties.Through stoichiometric oxidation of the sulfur atom in o-DMP-S,the resulting sulfoxide compound o-DMP-SO undergoes a radical photolysis reaction involving photodeoxygenation and photochemical rearrangement,thereby leading to the photomechanical effect.The sulfone compound o-DMP-SO_(2)displays prominent reversible photochromism,resulting from the radical photocyclization under 365 nm UV light irradiation.Based on comprehensive experimental and computational investigations,the diverse photoresponsive behaviors of these benzo[b]thiophene derivatives are demonstrated to depend on the intersystem crossing efficiency and radical-mediated photochemical reaction activity in excited states due to the different sulfur oxidation states.This work provides an insightful understanding of the relationship between molecular structure and photoresponsive behavior and opens up the opportunity for the development of photoresponsive materials with potential applications.展开更多
Solid-liquid state bonding of Si3N4 ceramics with TiN-modified Ag-Cu-Ti brazing alloy was used'- to enhance joint strength. The effects of the TiN particles on the microstructures, interfacial reactions, and roo...Solid-liquid state bonding of Si3N4 ceramics with TiN-modified Ag-Cu-Ti brazing alloy was used'- to enhance joint strength. The effects of the TiN particles on the microstructures, interfacial reactions, and room-temperature properties of the joints were investigated. The results show that the TiN particles are gen- erally well dispersed in the Ag-Cu eutectic base and the interface between them is both clean and com-pact. Changes in the TiN volume fractions from 0 to 20% exert no noticeable effect on the interfacial reac-tion between Ag-Cu-Ti and the substrates. Other bonding parameters being constant, the TiN volume frac-tion in the filler material plays a key role in the joint properties. For TiN volume fractions below 20%, the joints are reinforced, especially joints with 5% and 20% TiN. The average shearing strength of joints with 5% TiN is 200.8 MPa, 30% higher than that of joints with no TiN (154.1 MPa). However, for TiN volumes frac- tions above 20%, the joint strengths decrease.展开更多
基金Supported by the Beijing Higher Education Young Elite Teacher Project under Grant No YETP1297the Fundamental Research Funds for the Central Universities under Grant No 2014MDLXYZY05+1 种基金the Undergraduate Innovative Test Program of China under Grant Nos GCCX2015110009 and BEIJ2015110024the National Natural Science Foundation of China under Grant Nos11074312 and 11374377
文摘Ag3PO4 microcrystals with highly enhanced visible light photocatalytic activity are prepared by a facile and simple solid state reaction at room temperature. The composition, morphology and optical properties of the asprepared Ag3PO4 microcrystMs are characterized by x-ray diffraction, scanning electron microscopy and UV-vis diffuse reflectance spectra. The photocatalytie properties of Ag3PO4 are investigated by the degradation of both methylene blue and methyl orange dyes under visible light irradiation. The as-prepared Ag3PO4 microcrystals possess high photocatalytic oxygen production with the rate of 673μmolh-1g-1. Moreover, the as-prepared Ag3PO4 microcrystals show an enhanced photoelectrochemistry performance under irradiation of visible light.
基金This research was supported by the Australian Research Council(ARC)(DE170100928,DP170101467)an Australian Renewable Energy Agency(ARENA)Project(G00849).The authors acknowledge the use of the facilities at the UOW Electron Microscopy Center(LE0882813 and LE0237478)and Dr.Tania Silver for critical reading of the manuscript.
文摘This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and status are investigated.A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio(72%S).In contrast,a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio(44%S).In carbonate ester electrolyte,only the sulfur trapped in porous structures is active via‘solid-solid’behavior during cycling.The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents.To improve the capacity of the sulfur-rich cathode,ether electrolyte with NaNO_(3) additive is explored to realize a‘solid-liquid’sulfur redox process and confine the shuttle effect of the dissolved polysulfides.As a result,the sulfur-rich cathode achieved high reversible capacity(483 mAh g^(−1)),corresponding to a specific energy of 362 Wh kg^(−1) after 200 cycles,shedding light on the use of ether electrolyte for high-loading sulfur cathode.
基金the financial support from the Ministry of Science and Technology of China (Nos.2016YFA0204100 and 2016YFA0200200)the National Natural Science Foundation of China (Nos.21890753, 21573220 and 21802124)+2 种基金the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (No.QYZDB-SSW-JSC020)the DNL Cooperation Fund, CAS (No.DNL180201)the financial and technique supports from the Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University
文摘The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(> 400 ℃) conditions.Herein, a highly active catalytic conversion process of ethane at room temperature(25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-coordination structures.Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C2 chemicals, simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O–FeN4–O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals.This work deepens the understanding of alkane C–H activation on the FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane.
文摘Zinc oxide(ZnO) doped with erbium at different concentrations was synthesized by solid-state reaction method and characterized by X-ray diffraction(XRD), scanning electron microscopic(SEM), UVabsorption spectroscopy, photoluminescence(PL) study and vibrating sample magnetometer. The XRD studies exhibit the presence of wurtzite crystal structure similar to the parent compound ZnO in 1% Er^(3+)doped Zn O,suggesting that doped Er^(3+)ions sit at the regular Zn^(2+)sites. However, same studies spread over the samples with Er^(3+)content>1% reveals the occurrence of secondary phase. SEM images of 1% Er^(3+)doped ZnO show the polycrystalline nature of the synthesized sample. UV-visible absorption spectrum of Er^(3+)doped ZnO nanocrystals shows a strong absorption peak at 388 nm due to ZnO band to band transition. The PL study exhibits emission in the visible region, due to excitonic as well as defect related transitions. The magnetizationfield curve of Er^(3+)doped ZnO nanocrystals showed ferromagnetic property at room-temperature.
基金supported by the Agency for Science,Technology and Research Singapore through its Manufacturing,Trade and Connectivity Individual Research Grant(grant no.M22K2c0077)the National Natural Science Foundation of China(grant nos.21788102,22375066,21874121,and 21974128)the Guangdong Basic and Applied Basic Research Foundation(grant nos.2023B1515040003 and 2022A1515010315).
文摘Photoresponsive materials are considered as promising systems for intelligent technology applications owing to the contactless spatial and temporal control.Herein,controllable multi-photoresponsive behaviors are realized in benzo[b]thiophene derivatives(o-DMP-S,o-DMP-SO,and o-DMP-SO_(2))by modulating the sulfur oxidation state.Among them,o-DMP-S is photo-unreactive but possesses denser molecular packing upon ultraviolet(UV)light irradiation,exhibiting photoenhanced room-temperature phosphorescence properties.Through stoichiometric oxidation of the sulfur atom in o-DMP-S,the resulting sulfoxide compound o-DMP-SO undergoes a radical photolysis reaction involving photodeoxygenation and photochemical rearrangement,thereby leading to the photomechanical effect.The sulfone compound o-DMP-SO_(2)displays prominent reversible photochromism,resulting from the radical photocyclization under 365 nm UV light irradiation.Based on comprehensive experimental and computational investigations,the diverse photoresponsive behaviors of these benzo[b]thiophene derivatives are demonstrated to depend on the intersystem crossing efficiency and radical-mediated photochemical reaction activity in excited states due to the different sulfur oxidation states.This work provides an insightful understanding of the relationship between molecular structure and photoresponsive behavior and opens up the opportunity for the development of photoresponsive materials with potential applications.
基金Supported by the National Natural Science Foundation of China (No. 50075046)
文摘Solid-liquid state bonding of Si3N4 ceramics with TiN-modified Ag-Cu-Ti brazing alloy was used'- to enhance joint strength. The effects of the TiN particles on the microstructures, interfacial reactions, and room-temperature properties of the joints were investigated. The results show that the TiN particles are gen- erally well dispersed in the Ag-Cu eutectic base and the interface between them is both clean and com-pact. Changes in the TiN volume fractions from 0 to 20% exert no noticeable effect on the interfacial reac-tion between Ag-Cu-Ti and the substrates. Other bonding parameters being constant, the TiN volume frac-tion in the filler material plays a key role in the joint properties. For TiN volume fractions below 20%, the joints are reinforced, especially joints with 5% and 20% TiN. The average shearing strength of joints with 5% TiN is 200.8 MPa, 30% higher than that of joints with no TiN (154.1 MPa). However, for TiN volumes frac- tions above 20%, the joint strengths decrease.