Zinc-air batteries(ZABs)are promising energy storage systems because of high theoretical energy density,safety,low cost,and abundance of zinc.However,the slow multi-step reaction of oxygen and heavy reliance on noble-...Zinc-air batteries(ZABs)are promising energy storage systems because of high theoretical energy density,safety,low cost,and abundance of zinc.However,the slow multi-step reaction of oxygen and heavy reliance on noble-metal catalysts hinder the practical applications of ZABs.Therefore,feasible and advanced non-noble-metal elec-trocatalysts for air cathodes need to be identified to promote the oxygen catalytic reaction.In this review,we initially introduced the advancement of ZABs in the past two decades and provided an overview of key developments in this field.Then,we discussed the work-ing mechanism and the design of bifunctional electrocatalysts from the perspective of morphology design,crystal structure tuning,interface strategy,and atomic engineering.We also included theoretical studies,machine learning,and advanced characterization technologies to provide a comprehensive understanding of the structure-performance relationship of electrocatalysts and the reaction pathways of the oxygen redox reactions.Finally,we discussed the challenges and prospects related to designing advanced non-noble-metal bifunctional electrocatalysts for ZABs.展开更多
Metal tellurides(MTes) are highly attractive as promising anodes for high-performance potassium-ion batteries. The capacity attenuation of most reported MTe anodes is attributed to their poor electrical conductivity a...Metal tellurides(MTes) are highly attractive as promising anodes for high-performance potassium-ion batteries. The capacity attenuation of most reported MTe anodes is attributed to their poor electrical conductivity and large volume variation. The evolution mechanisms, dissolution properties, and corresponding manipulation strategies of intermediates(K-polytellurides, K-pTe_(x)) are rarely mentioned. Herein,we propose a novel structural engineering strategy to confine ultrafine CoTe_(2) nanodots in hierarchical nanogrid-in-nanofiber carbon substrates(CoTe_(2)@NC@NSPCNFs) for smooth immobilization of K-pTe_(x) and highly reversible conversion of CoTe_(2) by manipulating the intense electrochemical reaction process. Various in situ/ex situ techniques and density functional theory calculations have been performed to clarify the formation, transformation, and dissolution of K-pTe_(x)(K_(5)Te_(3) and K_(2)Te), as well as verifying the robust physical barrier and the strong chemisorption of K_(5)Te_(3) and K_(2)Te on S, N co-doped dual-type carbon substrates. Additionally, the hierarchical nanogrid-in-nanofiber nanostructure increases the chemical anchoring sites for K-pTe_(x), provides sufficient volume buffer space, and constructs highly interconnected conductive microcircuits, further propelling the battery reaction to new heights(3500 cycles at 2.0 A g^(-1)). Furthermore, the full cells further demonstrate the potential for practical applications. This work provides new insights into manipulating K-pTe_(x) in the design of ultralong-cycling MTe anodes for advanced PIBs.展开更多
Potassium-ion batteries(PIBs)are attractive for gridscale energy storage due to the abundant potassium resource and high energy density.The key to achieving high-performance and large-scale energy storage technology l...Potassium-ion batteries(PIBs)are attractive for gridscale energy storage due to the abundant potassium resource and high energy density.The key to achieving high-performance and large-scale energy storage technology lies in seeking eco-efficient synthetic processes to the design of suitable anode materials.Herein,a spherical sponge-like carbon superstructure(NCS)assembled by 2D nanosheets is rationally and efficiently designed for K+storage.The optimized NCS electrode exhibits an outstanding rate capability,high reversible specific capacity(250 mAh g^(−1) at 200 mA g^(−1) after 300 cycles),and promising cycling performance(205 mAh g^(−1) at 1000 mA g^(−1) after 2000 cycles).The superior performance can be attributed to the unique robust spherical structure and 3D electrical transfer network together with nitrogen-rich nanosheets.Moreover,the regulation of the nitrogen doping types and morphology of NCS-5 is also discussed in detail based on the experiments results and density functional theory calculations.This strategy for manipulating the structure and properties of 3D materials is expected to meet the grand challenges for advanced carbon materials as high-performance PIB anodes in practical applications.展开更多
The translucent GGAG:Ce/glass composites are prepared successfully by ball-milling,tableting,and pressureless sintering.The thickness of composites is about 400μm.The x-ray diffraction(XRD),differential scanning calo...The translucent GGAG:Ce/glass composites are prepared successfully by ball-milling,tableting,and pressureless sintering.The thickness of composites is about 400μm.The x-ray diffraction(XRD),differential scanning calorimetry(DSC),density of composite materials are measured and discussed systematically.The scanning electron microscopy(SEM)and energy dispersive spectrometer(EDS)elemental mapping are employed to analyze the particle size,the shape of powders,and the distribution of GGAG:Ce particles in the glass matrix,respectively.The decay time,ultraviolet,(UV),x-ray excitation luminescence spectra,and temperature spectra are studied.The results show that the composite materials have high light output,good thermostability,and short decay time.The method adopted in this work is an effective method to reduce the preparation time and cost of the sample.The ultralow afterglow indicates that the composite materials have an opportunity to be used for x-ray detection and imaging.展开更多
Selective hydrogenation of chloronitrobenzene(CNB) to chloroaniline(CAN) catalyzed by water-soluble Ru/Pt bimetallic catalyst in an aqueous-organic biphasic system was studied. It was found that the catalytic activity...Selective hydrogenation of chloronitrobenzene(CNB) to chloroaniline(CAN) catalyzed by water-soluble Ru/Pt bimetallic catalyst in an aqueous-organic biphasic system was studied. It was found that the catalytic activity increased obviously due to the addition of platinum. Ru/Pt bimetallic catalysts exhibited a strong synergistic effect when the molar ratio of Pt was in the range of 5%—80%. Under the mild conditions including a temperature of 25 ℃, a hydrogen pressure of 1.0 MPa and a Pt molar ratio of 20%, the conversion of p-chloronitrobenzene(p-CNB) reached 99.9%, with the selectivity to p-chloroaniline(p-CAN) equating to 99.4%. The Ru/Pt catalyst also showed high activity and selectivity for the hydrogenation of other chloro- and dichloro-nitrobenzenes with different substituted positions. In addition, the catalyst can be recycled five times without significant loss of activity.展开更多
Lithium(Li)metal is regarded as a promising anode candidate for high-energy-density rechargeable batteries.Nevertheless,Li metal is highly reactive against electrolytes,leading to rapid decay of active Li metal reserv...Lithium(Li)metal is regarded as a promising anode candidate for high-energy-density rechargeable batteries.Nevertheless,Li metal is highly reactive against electrolytes,leading to rapid decay of active Li metal reservoir.Here,alloying Li metal with low-content magnesium(Mg)is proposed to mitigate the reaction kinetics between Li metal anodes and electrolytes.Mg atoms enter the lattice of Li atoms,forming solid solution due to the low amount(5 wt%)of Mg.Mg atoms mainly concentrate near the surface of Mg-alloyed Li metal anodes.The reactivity of Mg-alloyed Li metal is mitigated kinetically,which results from the electron transfer from Li to Mg atoms due to the electronegativity difference.Based on quantitative experimental analysis,the consumption rate of active Li and electrolytes is decreased by using Mgalloyed Li metal anodes,which increases the cycle life of Li metal batteries under demanding conditions.Further,a pouch cell(1.25 Ah)with Mg-alloyed Li metal anodes delivers an energy density of 340 Wh kg^(-1)and a cycle life of 100 cycles.This work inspires the strategy of modifying Li metal anodes to kinetically mitigate the side reactions with electrolytes.展开更多
Tin selenide(SnSe)is considered as a potential anode for sodium-ion batteries(SIBs)owing to its high theoretical specific capacity.Unfortunately,it suffers from drastic volume expansion/contraction during sodium ions ...Tin selenide(SnSe)is considered as a potential anode for sodium-ion batteries(SIBs)owing to its high theoretical specific capacity.Unfortunately,it suffers from drastic volume expansion/contraction during sodium ions insertion/extraction,resulting in poor cycling stability.Herein,a pomegranate-inspired porous carbon shell wrapped heterogeneous SnSe/ZnSe composite(SnSe/ZnSe@C)is exquisitely designed and fabricated through electrostatic spraying followed by high-temperature selenization.The polyacrylonitrile-derived carbon shell acts as an adhesive to link the porous cubic SnSe/ZnSe and form highly interconnected microcircuits to improve the electron/ion transfer efficiency and inhibit the bulk volume change of internal metallic selenide nanoparticles and polyselenides dissolution during repeated cycling.Moreover,the abundant heterostructure interface of SnSe/ZnSe further significantly accelerates the electrons/ions transport.As a result,the as-prepared SnSe/ZnSe@C electrode exhibits a high specific capacity(508.3 m Ah g^(-1)at 0.05 A g^(-1)),excellent rate performance(177.8 m Ah g^(-1)at 10.0 A g^(-1)),and remarkable cycling stability(195.9 m Ah g^(-1)after 10,000 cycles at 5.0 A g^(-1)).Furthermore,in-situ Xray diffraction(XRD)/Raman,ex-situ transmission electron microscopy,and kinetic analysis clearly reveal a four-step electrochemical reaction process and battery-capacitor dual-mode sodium storage mechanism.This work provides a new perspective for developing commercial SIBs anode materials with high capacity and long lifespan.展开更多
Cation vacancies can bring numerous surprising characters due to its multifarious electron and orbit distribution.In this work,d-MnO_(2) with alkali-ion(K,Na,Li)associated manganese(Mn)vacancies is fabricated by a sim...Cation vacancies can bring numerous surprising characters due to its multifarious electron and orbit distribution.In this work,d-MnO_(2) with alkali-ion(K,Na,Li)associated manganese(Mn)vacancies is fabricated by a simple hydrothermal reaction,and the correlation between their electronic structure and pseudocapacitance are systematically investigated.FESEM/TEM images have shown that the morphology of MnO_(2) is obviously changed after the introducing of cation vacancies.The position of alkali-ion in MnO_(2) structure can be controlled by adjusting the ion concentration.XRD patterns and Raman spectra demonstrate that the alkali-ion is embedded in Mn vacancies at low concentration,while entered the interlayer of MnO_(2) at high concentration.The existence of Mn vacancies will resulting in the distortion of neighboring atoms,leading to the electronic delocalization,and thus enhancing the conductivity,pseudocapacitance and rate capability of MnO_(2).Accordingly,the specific capacitances of optimized 0.4 KMO,0.4 NaMO and 0.4 LiMO samples are enhanced about 1.9,1.6 and 1.6 times compared to pure MnO_(2).Meanwhile,the rate performance has also been improved about 76%,46%and 42%,respectively.Theoretical calculations further confirm that the Mn vacancies can generate additional occupancy states and cause an increase in carrier concentration,which will improve the conductivity and further boost the pseudocapacitance of MnO_(2).This result open up a promising approach to explore active and durable electrode materials.展开更多
A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless depo...A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless deposition method and evaluated for the deep oxidation of n-hexane as a model VOCs. The results show that the CeO_(2)and TiOxnanoparticles can highly disperse into each other and form Ce_(2)Ti_(2)O_(7)solid solution with appropriate Ce/Ti molar ratio, which significantly improves their redox ability by enhancing the interaction between CeO_(2)and TiO_(x). The dispersibility of Pt species can also be adjusted by altering the Ce/Ti molar ratio, and Pt/CeTi-2/1 catalyst with Ce/Ti molar ratio of 2:1 exhibits the best Pt dispersibility that Pt species mainly exist as Pt single atoms. The high dispersion of Pt species in the Pt/CeO_(2)-TiO_(2)catalysts would promote the catalytic activity of VOCs oxidation with low T90% values(1000 ppm, GHSV = 15,000 h^(-1)), such as for n-hexane degradation with T90% of 139℃. The characterizations reveal that the superior activity is mainly related to possessing the more Pt2+species,adsorbed oxygen species and higher low-temperature reducibility owing to the strong interaction between highly dispersed Pt species and CeO_(2)-TiO_(2)as well as the promoted migration of lattice oxygen by the formation of more Ce_(2)Ti_(2)O_(7)species. Furthermore, the Pt/CeTi-2/1 catalyst also exhibits excellent stability for chlorinated and other non-chlorinated VOCs oxidation, making it very promising for real application under various operating conditions.展开更多
FeCo-Al2O3 catalyst was prepared by an ultrasonic coprecipitation （UC） method for the growth of carbon nanotubes （CNTs） from catalytic decomposition of methane.Its catalytic performance was compared with that of t...FeCo-Al2O3 catalyst was prepared by an ultrasonic coprecipitation （UC） method for the growth of carbon nanotubes （CNTs） from catalytic decomposition of methane.Its catalytic performance was compared with that of the FeCo-Al2O3 catalyst counterparts prepared by stepwise impregnation （I） and conventional coprecipitation （C） methods,respectively.The structure and properties of the catalysts and the CNTs as produced thereon were investigated by means of XRD,XPS,TEM and N2 adsorption techniques.It was found that the catalyst prepared by the ultrasonic coprecipitation method was more active,and the yield and purity of the synthesized CNTs were promoted evidently.The XPS results revealed that there were more active components on the surface of the catalyst prepared by the ultrasonic coprecipitation method.On the other hand,N2 adsorption demonstrated that the catalyst prepared by the ultrasonic coprecipitation method conferred larger specific surface area,which was beneficial to dispersion of active components.TEM images further confirmed its higher dispersion.These factors could be responsible for its higher activity for the growth of CNTs from catalytic decomposition of methane.展开更多
The hybridization of fullerene and nanotube structures in newly isolated C;with the D;symmetric group(D;(1)-C;)provides an ideal model as a mediating allotrope of nanocarbon from zero-dimensional(OD)fullerene to one-d...The hybridization of fullerene and nanotube structures in newly isolated C;with the D;symmetric group(D;(1)-C;)provides an ideal model as a mediating allotrope of nanocarbon from zero-dimensional(OD)fullerene to one-dimensional nanotube.Raman and infrared spectroscopy combined with classical molecular dynamics simulation were used to investigate the structural evolution of D;(1)-C;at ambient and high pressure up to35.1 GPa.Interestingly,the high-pressure transformations of D;(1)-C;exhibit the features of both fullerene and nanotube.At around 2.5 GPa,the D;(1)-C;molecule in the crystal undergoes an orientational transition to a restricted rotation.At 6.6 GPa,the tubular hexagonal part occurs and transforms into a dumbbell-like structure at higher pressure.The material starts to amorphize above 13.9 GPa,and the transition is reversible until the pressure exceeds 25 GPa.The amorphization is probably correlated with both the intermolecular bonding and the morphology change.Our results enrich our understanding of structural changes in nano carbon from 0 D to1 D.展开更多
A decorated ruthenium catalyst was prepared by the coprecipitation method and used for the selective hydrogenation of maleic anhydride(MA) to γ-butyrolactone(GBL). The as-prepared catalyst was characterized by XRD, T...A decorated ruthenium catalyst was prepared by the coprecipitation method and used for the selective hydrogenation of maleic anhydride(MA) to γ-butyrolactone(GBL). The as-prepared catalyst was characterized by XRD, TGDTG and N2 adsorption techniques. The characterization tests revealed that the catalyst carrier was composed of monoclinic zirconia(m-ZrO2) and hydroxyl cobalt oxide(CoO(OH)). The hydrogenation results showed that the content of CoO(OH), the reaction temperature, the hydrogen pressure and the reaction time significantly affected the catalytic selectivity to GBL. The promotional effect of CoO(OH) was remarkable, which led to an obvious increase in GBL selectivity. An 100% MA conversion and 92.0% selectivity to GBL were achieved over the Ru/ZrO2-CoO(OH)(35%) catalyst in water solvent under the conditions involving a reaction temperature of 180 ℃, a hydrogen pressure of 3.0 MPa, and a reaction time of 6 h.展开更多
Cases abound in Fujian province of applying sustainable materials in the construction of traditional residential buildings, which demonstrate the skills and creative techniques of local builders, reflecting their wisd...Cases abound in Fujian province of applying sustainable materials in the construction of traditional residential buildings, which demonstrate the skills and creative techniques of local builders, reflecting their wisdom in molding and adapting to the environment. This paper probes into the utilization of locally available resources in Fujian traditional residential architecture from the perspective of the characteristics of "reduction, recycling and reuse" of sustainable materials, and puts forward the view that sustainability study of contemporary architecture should be approached from the relationship between man and environment and that inspiration can be drawn from the creative and innovative ideas of the folk residential builders.展开更多
Two Cu-Mo-Fe-Ox samples, which can store and supply pure hydrogen through repeated redox reaction （Fe3O4＋4H23Fe＋4H2O）, were prepared by co-precipitation （FCM-C） and impregnation （FCM-I） methods, respectively, ...Two Cu-Mo-Fe-Ox samples, which can store and supply pure hydrogen through repeated redox reaction （Fe3O4＋4H23Fe＋4H2O）, were prepared by co-precipitation （FCM-C） and impregnation （FCM-I） methods, respectively, and the performance of hydrogen production from water were investigated. Compared with the impregnated sample, the co-precipitation sample presented better catalytic activity. The samples were characterized by X-ray diffraction （XRD）, field emission scanning electron microscopy （FE-SEM）, X-ray photoelectron spectroscopy （XPS）, Fourier transform infrared spectroscopy （FT-IR） and temperature-programmed reduction （H2-TPR） techniques. XRD, FE-SEM and XPS results suggest that the FCM-C sample has smaller particle size and higher dispersion of iron oxide than that of FCM-I sample. In addition, FT-IR and H2-TPR analyses indicate that the weak interaction among metal oxides in FCM-C sample may induce facile reduction of active metal and superior property of hydrogen production by decomposing water in success展开更多
The root development of Actinidia chinensis planUets was studied in exposure to environmental stress of mechanical vibration at respectively 1 Hz, 2 Hz, 3 Hz, 4 Hz and 5 Hz. The plantlets exposed to vibration stimuli ...The root development of Actinidia chinensis planUets was studied in exposure to environmental stress of mechanical vibration at respectively 1 Hz, 2 Hz, 3 Hz, 4 Hz and 5 Hz. The plantlets exposed to vibration stimuli at all those frequencies have a larger total number and a larger total length of roots and a smaller permeability of root plasma-membrane, compared with those cultivated in an environment without vibration stress. Vibration at respectively 1 Hz, 2 Hz, 3 Hz and 4 Hz enhances root activity and the 3 Hz vibration is the most favorable. There is an obvious negative correlation between root activity and permeability of root plasma-membrane. The effects may be explained by the likelihood that mechanical Vibration at an appropriate frequency facilitates roots＇ absorbing water and minerals which are indispensable to inducing and synthesizing in roots some active substances favorable to growth. Nevertheless, overstress damages the integrity of root plasm-membrane, increases the permeability, and results in the disability of protecting root cells.展开更多
The lithium(Li)metal anode is widely regarded as an ideal anode material for high-energy-density batteries.However,uncontrolled Li dendrite growth often leads to unfavorable interfaces and low Coulombic efficiency(CE)...The lithium(Li)metal anode is widely regarded as an ideal anode material for high-energy-density batteries.However,uncontrolled Li dendrite growth often leads to unfavorable interfaces and low Coulombic efficiency(CE),limiting its broader application.Herein,an ether-based electrolyte(termed FGN-182)is formulated,exhibiting ultra-stable Li metal anodes through the incorporation of LiFSI and LiNO3 as dual salts.The synergistic effect of the dual salts facilitates the formation of a highly robust SEI film with fast Li+transport kinetics.Notably,Li||Cu half cells exhibit an average CE reaching up to 99.56%.In particular,pouch cells equipped with high-loading lithium cobalt oxide(LCO,3 mAh cm^(-2))cathodes,ultrathin Li chips(25μm),and lean electrolytes(5 g Ah-1)demonstrate outstanding cycling performance,retaining 80%capacity after 125 cycles.To address the gas issue in the cathode under high voltage,cathode additives 1,3,6-tricyanohexane is incorporated with FGN-182;the resulting high-voltage LCO||Li(4.4 V)pouch cells can cycle steadily over 93 cycles.This study demonstrates that,even with the use of ether-based electrolytes,it is possible to simultaneously achieve significant improvements in both high Li utilization and electrolyte tolerance to high voltage by exploring appropriate functional additives for both the cathode and anode.展开更多
基金the Natural Science Foundation of China(Grant No:22309180)Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No:XDB0600000,XDB0600400)+3 种基金Liaoning Binhai Laboratory,(Grant No:LILBLB-2023-04)Dalian Revitalization Talents Program(Grant No:2022RG01)Youth Science and Technology Foundation of Dalian(Grant No:2023RQ015)the University of Waterloo.
文摘Zinc-air batteries(ZABs)are promising energy storage systems because of high theoretical energy density,safety,low cost,and abundance of zinc.However,the slow multi-step reaction of oxygen and heavy reliance on noble-metal catalysts hinder the practical applications of ZABs.Therefore,feasible and advanced non-noble-metal elec-trocatalysts for air cathodes need to be identified to promote the oxygen catalytic reaction.In this review,we initially introduced the advancement of ZABs in the past two decades and provided an overview of key developments in this field.Then,we discussed the work-ing mechanism and the design of bifunctional electrocatalysts from the perspective of morphology design,crystal structure tuning,interface strategy,and atomic engineering.We also included theoretical studies,machine learning,and advanced characterization technologies to provide a comprehensive understanding of the structure-performance relationship of electrocatalysts and the reaction pathways of the oxygen redox reactions.Finally,we discussed the challenges and prospects related to designing advanced non-noble-metal bifunctional electrocatalysts for ZABs.
基金supported by the National Natural Science Foundation of China (Grant Nos. 51920105004, 52102223, 52002081)。
文摘Metal tellurides(MTes) are highly attractive as promising anodes for high-performance potassium-ion batteries. The capacity attenuation of most reported MTe anodes is attributed to their poor electrical conductivity and large volume variation. The evolution mechanisms, dissolution properties, and corresponding manipulation strategies of intermediates(K-polytellurides, K-pTe_(x)) are rarely mentioned. Herein,we propose a novel structural engineering strategy to confine ultrafine CoTe_(2) nanodots in hierarchical nanogrid-in-nanofiber carbon substrates(CoTe_(2)@NC@NSPCNFs) for smooth immobilization of K-pTe_(x) and highly reversible conversion of CoTe_(2) by manipulating the intense electrochemical reaction process. Various in situ/ex situ techniques and density functional theory calculations have been performed to clarify the formation, transformation, and dissolution of K-pTe_(x)(K_(5)Te_(3) and K_(2)Te), as well as verifying the robust physical barrier and the strong chemisorption of K_(5)Te_(3) and K_(2)Te on S, N co-doped dual-type carbon substrates. Additionally, the hierarchical nanogrid-in-nanofiber nanostructure increases the chemical anchoring sites for K-pTe_(x), provides sufficient volume buffer space, and constructs highly interconnected conductive microcircuits, further propelling the battery reaction to new heights(3500 cycles at 2.0 A g^(-1)). Furthermore, the full cells further demonstrate the potential for practical applications. This work provides new insights into manipulating K-pTe_(x) in the design of ultralong-cycling MTe anodes for advanced PIBs.
基金the National Natural Science Foundation of China(Grant Nos.51772086,51572078,51872087,and 11605053)the Natural Science Foundation of Hunan Province(Grant No.2018JJ2038)the Hunan Provincial Natural Science Foundation of China(Grant No.2017JJ3052)。
文摘Potassium-ion batteries(PIBs)are attractive for gridscale energy storage due to the abundant potassium resource and high energy density.The key to achieving high-performance and large-scale energy storage technology lies in seeking eco-efficient synthetic processes to the design of suitable anode materials.Herein,a spherical sponge-like carbon superstructure(NCS)assembled by 2D nanosheets is rationally and efficiently designed for K+storage.The optimized NCS electrode exhibits an outstanding rate capability,high reversible specific capacity(250 mAh g^(−1) at 200 mA g^(−1) after 300 cycles),and promising cycling performance(205 mAh g^(−1) at 1000 mA g^(−1) after 2000 cycles).The superior performance can be attributed to the unique robust spherical structure and 3D electrical transfer network together with nitrogen-rich nanosheets.Moreover,the regulation of the nitrogen doping types and morphology of NCS-5 is also discussed in detail based on the experiments results and density functional theory calculations.This strategy for manipulating the structure and properties of 3D materials is expected to meet the grand challenges for advanced carbon materials as high-performance PIB anodes in practical applications.
基金the National Natural Science Foundation of China(Grant Nos.11975220,51972291,11575170,and 11605194)。
文摘The translucent GGAG:Ce/glass composites are prepared successfully by ball-milling,tableting,and pressureless sintering.The thickness of composites is about 400μm.The x-ray diffraction(XRD),differential scanning calorimetry(DSC),density of composite materials are measured and discussed systematically.The scanning electron microscopy(SEM)and energy dispersive spectrometer(EDS)elemental mapping are employed to analyze the particle size,the shape of powders,and the distribution of GGAG:Ce particles in the glass matrix,respectively.The decay time,ultraviolet,(UV),x-ray excitation luminescence spectra,and temperature spectra are studied.The results show that the composite materials have high light output,good thermostability,and short decay time.The method adopted in this work is an effective method to reduce the preparation time and cost of the sample.The ultralow afterglow indicates that the composite materials have an opportunity to be used for x-ray detection and imaging.
基金the financial supports of the Natural Science Foundation of China(No.21303139)the Open Project of Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province(No.CSPC2013-1)+1 种基金the Key Fund Project of Educational Department of Sichuan Province(No.14ZA0126)the Doctoral Initiating Fund of China West Normal University(No.10B010)
文摘Selective hydrogenation of chloronitrobenzene(CNB) to chloroaniline(CAN) catalyzed by water-soluble Ru/Pt bimetallic catalyst in an aqueous-organic biphasic system was studied. It was found that the catalytic activity increased obviously due to the addition of platinum. Ru/Pt bimetallic catalysts exhibited a strong synergistic effect when the molar ratio of Pt was in the range of 5%—80%. Under the mild conditions including a temperature of 25 ℃, a hydrogen pressure of 1.0 MPa and a Pt molar ratio of 20%, the conversion of p-chloronitrobenzene(p-CNB) reached 99.9%, with the selectivity to p-chloroaniline(p-CAN) equating to 99.4%. The Ru/Pt catalyst also showed high activity and selectivity for the hydrogenation of other chloro- and dichloro-nitrobenzenes with different substituted positions. In addition, the catalyst can be recycled five times without significant loss of activity.
基金supported by the National Key Research and Development Program(2021YFB2400300)National Natural Science Foundation of China(22379013 and 22209010)the Beijing Institute of Technology“Xiaomi Young Scholars”program。
文摘Lithium(Li)metal is regarded as a promising anode candidate for high-energy-density rechargeable batteries.Nevertheless,Li metal is highly reactive against electrolytes,leading to rapid decay of active Li metal reservoir.Here,alloying Li metal with low-content magnesium(Mg)is proposed to mitigate the reaction kinetics between Li metal anodes and electrolytes.Mg atoms enter the lattice of Li atoms,forming solid solution due to the low amount(5 wt%)of Mg.Mg atoms mainly concentrate near the surface of Mg-alloyed Li metal anodes.The reactivity of Mg-alloyed Li metal is mitigated kinetically,which results from the electron transfer from Li to Mg atoms due to the electronegativity difference.Based on quantitative experimental analysis,the consumption rate of active Li and electrolytes is decreased by using Mgalloyed Li metal anodes,which increases the cycle life of Li metal batteries under demanding conditions.Further,a pouch cell(1.25 Ah)with Mg-alloyed Li metal anodes delivers an energy density of 340 Wh kg^(-1)and a cycle life of 100 cycles.This work inspires the strategy of modifying Li metal anodes to kinetically mitigate the side reactions with electrolytes.
基金support from the National Natural Science Foundation of China(51920105004,52102223)the Basic and Applied Basic Research Fund Project of Guangdong Province(2020A1515110401)。
文摘Tin selenide(SnSe)is considered as a potential anode for sodium-ion batteries(SIBs)owing to its high theoretical specific capacity.Unfortunately,it suffers from drastic volume expansion/contraction during sodium ions insertion/extraction,resulting in poor cycling stability.Herein,a pomegranate-inspired porous carbon shell wrapped heterogeneous SnSe/ZnSe composite(SnSe/ZnSe@C)is exquisitely designed and fabricated through electrostatic spraying followed by high-temperature selenization.The polyacrylonitrile-derived carbon shell acts as an adhesive to link the porous cubic SnSe/ZnSe and form highly interconnected microcircuits to improve the electron/ion transfer efficiency and inhibit the bulk volume change of internal metallic selenide nanoparticles and polyselenides dissolution during repeated cycling.Moreover,the abundant heterostructure interface of SnSe/ZnSe further significantly accelerates the electrons/ions transport.As a result,the as-prepared SnSe/ZnSe@C electrode exhibits a high specific capacity(508.3 m Ah g^(-1)at 0.05 A g^(-1)),excellent rate performance(177.8 m Ah g^(-1)at 10.0 A g^(-1)),and remarkable cycling stability(195.9 m Ah g^(-1)after 10,000 cycles at 5.0 A g^(-1)).Furthermore,in-situ Xray diffraction(XRD)/Raman,ex-situ transmission electron microscopy,and kinetic analysis clearly reveal a four-step electrochemical reaction process and battery-capacitor dual-mode sodium storage mechanism.This work provides a new perspective for developing commercial SIBs anode materials with high capacity and long lifespan.
基金supported by Zhejiang Provincial Natural Science Foundation of China under Grant No.LQ18E030005,LY18E060005,LY19E020006,LY18E020007National Natural Science Foundation of China(No.51902301)。
文摘Cation vacancies can bring numerous surprising characters due to its multifarious electron and orbit distribution.In this work,d-MnO_(2) with alkali-ion(K,Na,Li)associated manganese(Mn)vacancies is fabricated by a simple hydrothermal reaction,and the correlation between their electronic structure and pseudocapacitance are systematically investigated.FESEM/TEM images have shown that the morphology of MnO_(2) is obviously changed after the introducing of cation vacancies.The position of alkali-ion in MnO_(2) structure can be controlled by adjusting the ion concentration.XRD patterns and Raman spectra demonstrate that the alkali-ion is embedded in Mn vacancies at low concentration,while entered the interlayer of MnO_(2) at high concentration.The existence of Mn vacancies will resulting in the distortion of neighboring atoms,leading to the electronic delocalization,and thus enhancing the conductivity,pseudocapacitance and rate capability of MnO_(2).Accordingly,the specific capacitances of optimized 0.4 KMO,0.4 NaMO and 0.4 LiMO samples are enhanced about 1.9,1.6 and 1.6 times compared to pure MnO_(2).Meanwhile,the rate performance has also been improved about 76%,46%and 42%,respectively.Theoretical calculations further confirm that the Mn vacancies can generate additional occupancy states and cause an increase in carrier concentration,which will improve the conductivity and further boost the pseudocapacitance of MnO_(2).This result open up a promising approach to explore active and durable electrode materials.
基金supported by a grant from the National Key Research and Development Program of China (2016YFC0204300)the National Nature Science Foundation of China (21477109)。
文摘A series of CeO_(2)-TiO_(2)mixed oxides supports with various Ce/Ti molar ratio were synthesized by modified coprecipitation method. The corresponding Pt loaded(0.5 wt% Pt) catalysts were prepared by electronless deposition method and evaluated for the deep oxidation of n-hexane as a model VOCs. The results show that the CeO_(2)and TiOxnanoparticles can highly disperse into each other and form Ce_(2)Ti_(2)O_(7)solid solution with appropriate Ce/Ti molar ratio, which significantly improves their redox ability by enhancing the interaction between CeO_(2)and TiO_(x). The dispersibility of Pt species can also be adjusted by altering the Ce/Ti molar ratio, and Pt/CeTi-2/1 catalyst with Ce/Ti molar ratio of 2:1 exhibits the best Pt dispersibility that Pt species mainly exist as Pt single atoms. The high dispersion of Pt species in the Pt/CeO_(2)-TiO_(2)catalysts would promote the catalytic activity of VOCs oxidation with low T90% values(1000 ppm, GHSV = 15,000 h^(-1)), such as for n-hexane degradation with T90% of 139℃. The characterizations reveal that the superior activity is mainly related to possessing the more Pt2+species,adsorbed oxygen species and higher low-temperature reducibility owing to the strong interaction between highly dispersed Pt species and CeO_(2)-TiO_(2)as well as the promoted migration of lattice oxygen by the formation of more Ce_(2)Ti_(2)O_(7)species. Furthermore, the Pt/CeTi-2/1 catalyst also exhibits excellent stability for chlorinated and other non-chlorinated VOCs oxidation, making it very promising for real application under various operating conditions.
文摘FeCo-Al2O3 catalyst was prepared by an ultrasonic coprecipitation （UC） method for the growth of carbon nanotubes （CNTs） from catalytic decomposition of methane.Its catalytic performance was compared with that of the FeCo-Al2O3 catalyst counterparts prepared by stepwise impregnation （I） and conventional coprecipitation （C） methods,respectively.The structure and properties of the catalysts and the CNTs as produced thereon were investigated by means of XRD,XPS,TEM and N2 adsorption techniques.It was found that the catalyst prepared by the ultrasonic coprecipitation method was more active,and the yield and purity of the synthesized CNTs were promoted evidently.The XPS results revealed that there were more active components on the surface of the catalyst prepared by the ultrasonic coprecipitation method.On the other hand,N2 adsorption demonstrated that the catalyst prepared by the ultrasonic coprecipitation method conferred larger specific surface area,which was beneficial to dispersion of active components.TEM images further confirmed its higher dispersion.These factors could be responsible for its higher activity for the growth of CNTs from catalytic decomposition of methane.
基金supported fnancially by the National Key R&D Program of China(Grant No.2018YFA0305900)the National Natural Science Foundation of China(Grant Nos.12011530063 and 51822204)+3 种基金supported by NSF(DMR-0805056EAR 06–49658,COMPRES)DOE/NNSA(DE-FC03-03N00144,CDAC)supported by the DOE/BES(DEAC02-98CH10886)。
文摘The hybridization of fullerene and nanotube structures in newly isolated C;with the D;symmetric group(D;(1)-C;)provides an ideal model as a mediating allotrope of nanocarbon from zero-dimensional(OD)fullerene to one-dimensional nanotube.Raman and infrared spectroscopy combined with classical molecular dynamics simulation were used to investigate the structural evolution of D;(1)-C;at ambient and high pressure up to35.1 GPa.Interestingly,the high-pressure transformations of D;(1)-C;exhibit the features of both fullerene and nanotube.At around 2.5 GPa,the D;(1)-C;molecule in the crystal undergoes an orientational transition to a restricted rotation.At 6.6 GPa,the tubular hexagonal part occurs and transforms into a dumbbell-like structure at higher pressure.The material starts to amorphize above 13.9 GPa,and the transition is reversible until the pressure exceeds 25 GPa.The amorphization is probably correlated with both the intermolecular bonding and the morphology change.Our results enrich our understanding of structural changes in nano carbon from 0 D to1 D.
基金the financial support from the Natural Science Foundation of China(No.21303139)the Key Fund Project of Educational Department of Sichuan Province(No.14ZA0126)the Open Project of Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province(No.CSPC2013-1)
文摘A decorated ruthenium catalyst was prepared by the coprecipitation method and used for the selective hydrogenation of maleic anhydride(MA) to γ-butyrolactone(GBL). The as-prepared catalyst was characterized by XRD, TGDTG and N2 adsorption techniques. The characterization tests revealed that the catalyst carrier was composed of monoclinic zirconia(m-ZrO2) and hydroxyl cobalt oxide(CoO(OH)). The hydrogenation results showed that the content of CoO(OH), the reaction temperature, the hydrogen pressure and the reaction time significantly affected the catalytic selectivity to GBL. The promotional effect of CoO(OH) was remarkable, which led to an obvious increase in GBL selectivity. An 100% MA conversion and 92.0% selectivity to GBL were achieved over the Ru/ZrO2-CoO(OH)(35%) catalyst in water solvent under the conditions involving a reaction temperature of 180 ℃, a hydrogen pressure of 3.0 MPa, and a reaction time of 6 h.
基金Founded by National Natural Science Foundation (No. 51278123)Fujian Natural Science Foundation (No.2010J01285)
文摘Cases abound in Fujian province of applying sustainable materials in the construction of traditional residential buildings, which demonstrate the skills and creative techniques of local builders, reflecting their wisdom in molding and adapting to the environment. This paper probes into the utilization of locally available resources in Fujian traditional residential architecture from the perspective of the characteristics of "reduction, recycling and reuse" of sustainable materials, and puts forward the view that sustainability study of contemporary architecture should be approached from the relationship between man and environment and that inspiration can be drawn from the creative and innovative ideas of the folk residential builders.
基金supported by the National Basic Research Program of China(973 Program,2011CB201202)of Ministry of Science and Technology of China(MOST)
文摘Two Cu-Mo-Fe-Ox samples, which can store and supply pure hydrogen through repeated redox reaction （Fe3O4＋4H23Fe＋4H2O）, were prepared by co-precipitation （FCM-C） and impregnation （FCM-I） methods, respectively, and the performance of hydrogen production from water were investigated. Compared with the impregnated sample, the co-precipitation sample presented better catalytic activity. The samples were characterized by X-ray diffraction （XRD）, field emission scanning electron microscopy （FE-SEM）, X-ray photoelectron spectroscopy （XPS）, Fourier transform infrared spectroscopy （FT-IR） and temperature-programmed reduction （H2-TPR） techniques. XRD, FE-SEM and XPS results suggest that the FCM-C sample has smaller particle size and higher dispersion of iron oxide than that of FCM-I sample. In addition, FT-IR and H2-TPR analyses indicate that the weak interaction among metal oxides in FCM-C sample may induce facile reduction of active metal and superior property of hydrogen production by decomposing water in success
基金Funded by the Natural Science Foundation of China (No. 39770206).
文摘The root development of Actinidia chinensis planUets was studied in exposure to environmental stress of mechanical vibration at respectively 1 Hz, 2 Hz, 3 Hz, 4 Hz and 5 Hz. The plantlets exposed to vibration stimuli at all those frequencies have a larger total number and a larger total length of roots and a smaller permeability of root plasma-membrane, compared with those cultivated in an environment without vibration stress. Vibration at respectively 1 Hz, 2 Hz, 3 Hz and 4 Hz enhances root activity and the 3 Hz vibration is the most favorable. There is an obvious negative correlation between root activity and permeability of root plasma-membrane. The effects may be explained by the likelihood that mechanical Vibration at an appropriate frequency facilitates roots＇ absorbing water and minerals which are indispensable to inducing and synthesizing in roots some active substances favorable to growth. Nevertheless, overstress damages the integrity of root plasm-membrane, increases the permeability, and results in the disability of protecting root cells.
基金supported by the National Key Research and Development Program of China(2022YFB2502103)the Xiamen Science and Technology Project(3502Z20231057)+1 种基金the National Natural Science Foundation of China(Nos.22279107 and 22288102)J.You,R.Wei,and L.Niu acknowledge the China Scholarship Council(CSC)for a doctoral scholarship(Grant Nos.202006310030,202108530138,and 202108530139).
文摘The lithium(Li)metal anode is widely regarded as an ideal anode material for high-energy-density batteries.However,uncontrolled Li dendrite growth often leads to unfavorable interfaces and low Coulombic efficiency(CE),limiting its broader application.Herein,an ether-based electrolyte(termed FGN-182)is formulated,exhibiting ultra-stable Li metal anodes through the incorporation of LiFSI and LiNO3 as dual salts.The synergistic effect of the dual salts facilitates the formation of a highly robust SEI film with fast Li+transport kinetics.Notably,Li||Cu half cells exhibit an average CE reaching up to 99.56%.In particular,pouch cells equipped with high-loading lithium cobalt oxide(LCO,3 mAh cm^(-2))cathodes,ultrathin Li chips(25μm),and lean electrolytes(5 g Ah-1)demonstrate outstanding cycling performance,retaining 80%capacity after 125 cycles.To address the gas issue in the cathode under high voltage,cathode additives 1,3,6-tricyanohexane is incorporated with FGN-182;the resulting high-voltage LCO||Li(4.4 V)pouch cells can cycle steadily over 93 cycles.This study demonstrates that,even with the use of ether-based electrolytes,it is possible to simultaneously achieve significant improvements in both high Li utilization and electrolyte tolerance to high voltage by exploring appropriate functional additives for both the cathode and anode.
