A family of Said-Bézier type generalized Ball （SBGB） bases and surfaces with a parameter H over triangular domain is introduced,which unifies Bézier surface and Said-Ball surface and includes several inter...A family of Said-Bézier type generalized Ball （SBGB） bases and surfaces with a parameter H over triangular domain is introduced,which unifies Bézier surface and Said-Ball surface and includes several intermediate surfaces. To convert different bases and surfaces,the dual functionals of bases are presented. As an application of dual functionals,the subdivision formulas for surfaces are established.展开更多
Inorganic perovskite solar cells(IPSCs),due to their suitable bandgap and superior thermal stability,are ideal candidates for tandem solar cells combined with silicon.However,the development of inorganic perovskite so...Inorganic perovskite solar cells(IPSCs),due to their suitable bandgap and superior thermal stability,are ideal candidates for tandem solar cells combined with silicon.However,the development of inorganic perovskite solar cells has been hindered by suboptimal crystallization dynamics that generate detrimental defects in the perovskite lattice.Here,we propose 4-Methoxyphenylphosphonic Acid(4MPA)as a multifunctional additive to address this challenge.P=O in 4MPA establish strong coordination with undercoordinated Pb^(2+),while-OH engage in O...H-O hydrogen bonding interactions with DMSO,effectively weakening the solvent-[PbX_(6)]^(4-)octahedron interaction.This dual functionality facilitates complete and rapid DMA^(+)-to-Cs^(+)cation exchange while regulating crystallization kinetics,thereby optimizing crystal growth.Furthermore,π-π interactions between benzene rings significantly enhance the moisture resistance of the perovskite layer.The optimized device demonstrates a power conversion efficiency(PCE)of 21.35%,with unencapsulated devices retaining 93,63%of their initial efficiency after 200-hour continuous operation under ambient conditions(35%relative humidity).展开更多
In recent years,the direct introduction of sulfonyl and sulfenyl groups into unsaturated substrates by using thiosulfonates as unique dual functional reagents has inarguably provided chemists a new platform for the di...In recent years,the direct introduction of sulfonyl and sulfenyl groups into unsaturated substrates by using thiosulfonates as unique dual functional reagents has inarguably provided chemists a new platform for the diverse synthesis of important S-containing derivatives.These 1,n-thiosulfonylation reactions usually feature simple procedures,100%atom economy,and high regioselectivity.This review focuses on the recent advancements in the transformations of thiosulfonates through 1,n-thiosulfonylation involving the formation of two distinct C-S bonds under transition-metal-catalyzed or metal-free conditions,where thiosulfonates act as both a sulfonyl and a sulfenyl component.展开更多
Several common dual quaternion functions,such as the power function,the magnitude function,the 2-norm function,and the kth largest eigenvalue of a dual quaternion Hermitian matrix,are standard dual quaternion function...Several common dual quaternion functions,such as the power function,the magnitude function,the 2-norm function,and the kth largest eigenvalue of a dual quaternion Hermitian matrix,are standard dual quaternion functions,i.e.,the standard parts of their function values depend upon only the standard parts of their dual quaternion variables.Furthermore,the sum,product,minimum,maximum,and composite functions of two standard dual functions,the logarithm and the exponential of standard unit dual quaternion functions,are still standard dual quaternion functions.On the other hand,the dual quaternion optimization problem,where objective and constraint function values are dual numbers but variables are dual quaternions,naturally arises from applications.We show that to solve an equality constrained dual quaternion optimization(EQDQO)problem,we only need to solve two quaternion optimization problems.If the involved dual quaternion functions are all standard,the optimization problem is called a standard dual quaternion optimization problem,and some better results hold.Then,we show that the dual quaternion optimization problems arising from the hand-eye calibration problem and the simultaneous localization and mapping(SLAM)problem are equality constrained standard dual quaternion optimization problems.展开更多
Bioactive glass-chitosan-alginate hybrid scaffolds （BG-C-A scaffolds） were fabricated using BG sol as a dual function additive, which behaves as both bioactive inorganic phase to confer the bioactivity and cross-lin...Bioactive glass-chitosan-alginate hybrid scaffolds （BG-C-A scaffolds） were fabricated using BG sol as a dual function additive, which behaves as both bioactive inorganic phase to confer the bioactivity and cross-linker to improve the structural stability and mechanical properties. The microstructure, physicochemical and mechanical properties, in vitro bioactivity and cellular biocompatibility of the scaffolds were investigated. The results indicated that BG component was successfully incorporated into the BG-C-A scaffolds through a facile BG sol-immersing method and the original interconnected microstructure could be well preserved. The obtained BG-C-A scaffolds showed improved mechanical properties and structural stability as compared to C-A scaffolds. At the same time, they presented excellent in vitro bioactivity and cellular compatibility. All these results demonstrated that these BG-C-A scaffolds have promising potential for tissue engineering.展开更多
A fluorescent active organic–inorganic hybrid material Py N-SBA-15 was synthesized by implementing pyrene derivatives into mesoporous SBA-15 silica.Py N-SBA-15 had detection and removal functionalities toward Al^(3+)...A fluorescent active organic–inorganic hybrid material Py N-SBA-15 was synthesized by implementing pyrene derivatives into mesoporous SBA-15 silica.Py N-SBA-15 had detection and removal functionalities toward Al^(3+),Cu^(2+),and Hg^(2+).On the one hand,Py N-SBA-15 was used as a fluorescence sensor and displayed high sensitivity toward Al^(3+),Cu^(2+),and Hg^(2+)cations (limit of detection:8.0×10^(-7),1.1×10^(-7),and 2.9×10^(-6)mol·L^(–1),respectively) among various analytes with“turn-off”response.On the other hand,the adsorption studies for these toxic analytes (Cu^(2+),Hg^(2+),and Al^(3+)) showed that the ion removal capacity could reach up to 45,581,and 85 mg·g^(-1),respectively.Moreover,the Langmuir isotherm models were better fitted with the adsorption data,indicating that the adsorption was mono-layer adsorption.Kinetic analysis revealed that the adsorption process was well described by the pseudo-second-order kinetic model for Cu^(2+)and Hg^(2+)and pseudo-first-order kinetic model for Al^(3+).The prepared silica material could be reused in four recycles without significantly decreasing its adsorption capacity.Therefore,the Py N-SBA-15 material can serve as a promising candidate for the simultaneous rapid detection and efficient adsorption of metal ions.展开更多
Integrated CO_(2)capture and utilization(ICCU)technology requires dual functional materials(DFMs)to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8...Integrated CO_(2)capture and utilization(ICCU)technology requires dual functional materials(DFMs)to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8%Na_(2)CO_(3)-8%CaO/γ-Al_(2)O_(3)DFM is studied.The adsorbent precursors are first co-impregnated onto alumina and calcined in air.Then,Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols:static air in muffle or under different mixtures(10%H_(2)/N_(2),50%H_(2)/N_(2)and N_(2))streams.Samples are characterized by XRD,N_(2)adsorption-desorption,H_(2)chemisorption,TEM,XPS,H_(2)-TPD,H_(2)-TPR,CO_(2)-TPD and TPSR.The catalytic behavior is evaluated,in cycles of CO_(2)adsorption and hydrogenation to CH_(4),and temporal evolution of reactants and products concentrations is analyzed.The calcination atmosphere influences the physicochemical properties and,ultimately,activity of DFMs.Characterization data and catalytic performance discover the acccomodation of Ru nanoparticles disposition and basic sites is mostly influencing the catalytic activity.DFM calcined under N_(2)flow(RuNaCa-N_(2))shows the highest CH_(4)production(449μmol/g at 370℃),because a well-controlled decomposition of precursors which favors the better accomodation of adsorbent and Ru phases,maximizing the specific surface area,the Ru-basic sites interface and the participation of different basic sites in the CO_(2)methanation reaction.Thus,the calcination in a N_(2)flow is revealed as the optimal calcination protocol to achieve highly efficient DFM for integrated CO_(2)adsorption and hydrogenation applications.展开更多
In this paper,we proved that the infinitesimal generator of a strongly continuous cosine operator function is preserved under the time-dependent perturbation in the sun-reflexive case,where the perturbed operator is ...In this paper,we proved that the infinitesimal generator of a strongly continuous cosine operator function is preserved under the time-dependent perturbation in the sun-reflexive case,where the perturbed operator is a bounded linear operator from X into a bigger space Xθ(not X),then the corresponding 2-order abstract Cauchy problem is uniformly well-posed.展开更多
The dual algorithm for minimax problems is further studied in this paper.The resulting theoretical analysis shows that the condition number of the corresponding Hessian of the smooth modified Lagrange function with ch...The dual algorithm for minimax problems is further studied in this paper.The resulting theoretical analysis shows that the condition number of the corresponding Hessian of the smooth modified Lagrange function with changing parameter in the dual algorithm is proportional to the reciprocal of the parameter,which is very important for the efficiency of the dual algorithm.At last,the numerical experiments are reported to validate the analysis results.展开更多
The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of ...The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).展开更多
Nickel-based cathodes in aqueous nickel-zinc batteries typically suffer from sluggish reaction kinetics and limited energy density.In situ introduction of metal phosphides and rational construction of heterostructures...Nickel-based cathodes in aqueous nickel-zinc batteries typically suffer from sluggish reaction kinetics and limited energy density.In situ introduction of metal phosphides and rational construction of heterostructures can effectively promote electron/ion transport.However,the complex evolution of phosphidation and intractable phosphidizing degree greatly affect the composition of active phase,active sites,charge transfer rate,and ion adsorption strength of cathodes.Herein,the critical bimetallic phosphide layer(CBPL)is constructed on the NiCo-layered double hydroxide(NiCo-LDH)skeleton by a controllable anion-exchange strategy,yielding a novel nanohybrid cathode(NiCo-P1.0,1.0 representing the mass ratio of Na_(2)H_(2)PO_(2)to NiCo-LDH).The high-conductivity CBPL with the inner NiCo-LDH forms extensive heterostructures,effectively regulating the electronic structure via charge transfer,thereby improving electrical conductivity.Remarkably,the CBPL exhibits unexpected electrochemical activity and synergizes with NiCo-LDH for electrode reactions,ultimately delivering extra energy.Benefiting from the bifunctional CBPL,NiCo-P1.0 delivers an optimal capacity of 286.64 mAh g^(−1)at 1C(1C=289 mAh g^(−1))and superb rate performance(a capacity retention of 72.22%at 40C).The assembled NiCo-P1.0//Zn battery achieves ultrahigh energy/power density(503.62 Wh kg^(−1)/18.62 kW kg^(−1),based on the mass loading of active material on the cathode),and the flexible quasi-solid-state pouch cell validates its practicality.This work demonstrates the superiority of bifunctional CBPL for surface modification,providing an effective and scalable compositing strategy in achieving high-performance cathodes for aqueous batteries.展开更多
Achieving efficient adsorption and separation of C_(2)H_(2)/CO_(2)mixtures is a goal that people have always pursued to improve the situation of high energy consumption brought by traditional separation technologies i...Achieving efficient adsorption and separation of C_(2)H_(2)/CO_(2)mixtures is a goal that people have always pursued to improve the situation of high energy consumption brought by traditional separation technologies in industry today.High-nuclearity metal cluster-based MOFs with different functionalities are promising for this separation,but it is a complicated and difficult task to precisely control their structures.The strategy of pore-space partition(PSP)is a powerful way to construct this type MOFs,which has the characteristic of isostructural relationship,and can be resulted in a similar performance for them.Therefore,it is an interesting work to explore the effect of MOFs property by adjusting the size of PSP dividers.Herein,three tetranuclear Cu(Ⅱ)cluster-based MOFs(FJU-112/113/114)with dual functionalities has been successfully obtained by PSP strategy with various lengths of divider units.With the highest microporosity and unique functional site,FJU-114 realized a good improvement in the adsorption and separation performance of C_(2)H_(2)/CO_(2).The gas adsorption and lab-scale C_(2)H_(2)/CO_(2)breakthrough experiments demonstrated that FJU-114 exhibits the highest adsorption uptake of 77 cm^(3)/g for C_(2)H_(2),and shows the best separation factor of 4.2 among three MOFs.The GCMC simulation reveals that a stronger adsorption binding site of C_(2)H_(2)in FJU-114a located in the cage II near the unchanged tetranuclear copper node,combined with its high microporosity to achieve the effect of dual functionalities for the improvement performance of C_(2)H_(2)adsorption and separation.展开更多
The Lon proteases are evolutionarily conserved oligomeric hydrolases characterized by a built-in ATPase module.Here,we report the structures of LonC from Meiothermus taiwanensis(MtaLonC),a unique member in the Lon pro...The Lon proteases are evolutionarily conserved oligomeric hydrolases characterized by a built-in ATPase module.Here,we report the structures of LonC from Meiothermus taiwanensis(MtaLonC),a unique member in the Lon protein family with a dual chaperone-protease function but lacking ATPase activity,determined by cryo-electron microscopy(cryo-EM).In its apo state,LonC forms phosphate-bound open-ring pentamers,open-ring hexamers,and close-ring heptamers.However,upon interaction with ATPγS,inhibitor,or substrate,MtaLonC assembles into close-ring hexamers,wherein the protease domain’s substrate-binding loop adopts an extended active conformation.We show that proteolytic and chaperone activities may be carried out by the close-ring hexameric and heptameric forms,respectively.We further show that MtaLonC forms exclusively close-ring heptamers at elevated temperatures.This study sheds light on the bifurcated assembly pathway of MtaLonC,leading to two distinct oligomeric close-ring complexes that carry out a dual function.展开更多
A new class of cyclometalated iridium(III)complexes with imine-N-heterocyclic carbenes(NHC)as ligands were synthesized and fully characterized.One crystal structure is reported.All the six complexes exhibited highly p...A new class of cyclometalated iridium(III)complexes with imine-N-heterocyclic carbenes(NHC)as ligands were synthesized and fully characterized.One crystal structure is reported.All the six complexes exhibited highly potent anticancer activity against A549 cells,HeLa cells,HepG2 cells,GL261 cells and A549R cells.In particular,they were up to 9 and 37 times more potent than clinically used anticancer drug cisplatin towards A549 and A549R cell lines,respectively.Remarkably,mechanism studies showed that the complexes pass into cancer cells through an energy-dependent pathway and cause apoptosis via reactive oxygen species(ROS)generation,mitochondrial membrane potential dysfunction,and lysosomal damage.In addition,complex Ir6 effectively impeded cell migration and colony formation.展开更多
Desalination of seawater and renewable energy storage are quite promising for a sustainable society,but their combination for high efficiency is a difficult task.Herein,we demonstrate a dual-function battery,which is ...Desalination of seawater and renewable energy storage are quite promising for a sustainable society,but their combination for high efficiency is a difficult task.Herein,we demonstrate a dual-function battery,which is composed of a NaTi_(2)(PO_(4))_(3) anode and a Ag cathode with NaCl aqueous electrolyte,for desalination and electrical energy storage.In a charging process,Na+and Cl-are extracted from the electrolyte and inserted into the separate electrodes,while in a reverse process,the stored electricity and ions are released into electrolyte.As a demonstration,the dual-function battery can be continuously photocharged with a solar cell and discharged for 50 cycles without significant decrease in both the discharge voltage and capacity.This study will provide new insights into both seawater desalination and efficient renewable energy utilization.展开更多
The adsorption,degradation,and sensing of chemical warfare agents are highly important.In this work,a new Zr_((IV))-based metal-organic gel(MOG)was designed and synthesized,which demonstrated dualfunctional performanc...The adsorption,degradation,and sensing of chemical warfare agents are highly important.In this work,a new Zr_((IV))-based metal-organic gel(MOG)was designed and synthesized,which demonstrated dualfunctional performance in the degradation of nerve agent simulants and the adsorptive sensing of blister agent simulants.A Zr_((IV))-based MOG,namely,Zr-MOG-taBDC(H_(2)taBDC=2-(1H-1,2,4-triazol-1-yl)terephthalic acid),was synthesized through the thermal transformation of a tetrahedral Zr_((IV))-based metal-organic cage,{[Cp_(3)Zr_(3)(μ_(3)-O)(μ_(2)-OH)_(3)]_(4)(taBDC)_(6)}·(Cl^(-))_(4)(Zr-MOC-taBDC),in a mixed acetonitrile/water solvent system,bypassing the need for tedious anion exchange and high-boiling solvents.The resulting MOG exhibited hierarchical porosity and high stability across a wide pH range(1-11).Catalytic tests revealed that Zr-MOG-taBDC achieved 95.4%degradation efficiency for the nerve agent simulant diethyl phenylphosphonate(DEPPT),with a half-life of 49.5 minutes,outperforming its crystalline MOC precursor.Additionally,the gel demonstrated a high adsorption capacity(0.6 g g^(-1))for the mustard gas simulant 2-chloroethyl ethyl sulfide(CEES),enabling real-time detection via a quartz crystal microbalance(QCM)with a linear response range up to 100 ppm.Mechanistic studies indicated that degradation proceeds via P-S bond cleavage catalyzed by Zr-OH-H_(2)O Lewis acid-base sites,whereas adsorption involves reversible physical and irreversible chemical interactions with triazole groups and Zr-oxo clusters.This work highlights the potential of Zr-MOGs as multifunctional materials for chemical warfare agent mitigation and sensing.展开更多
A series of rigid-flexible-ligand functionalized dodeca-nuclear lanthanide-tungsten heterometal cluster incorporated ring-shaped selenotungstates[H_(2)N(CH_(3))_(2)]_(16)Na_(2)[Ln_(4)(H_(2)O)_(6)(HPZDA)_(2)(HFMA)_(2)W...A series of rigid-flexible-ligand functionalized dodeca-nuclear lanthanide-tungsten heterometal cluster incorporated ring-shaped selenotungstates[H_(2)N(CH_(3))_(2)]_(16)Na_(2)[Ln_(4)(H_(2)O)_(6)(HPZDA)_(2)(HFMA)_(2)W_(8)O_(21)][B-α-SeW_(9)O_(33)]_(4)·_(2)_(9)H_(2)O[Ln=Ce^(3+)(1),Pr^(3+)(2),Nd^(3+)(3);H_(2)PZDA=2,3-pyrazine dicarboxylic acid,H_(2)FMA=fumaric acid]and[H_(2)N(CH_(3))_(2)]_(14)Cs_(2)Na_(2)[Eu4(H_(2)O)_(6)(HPZDA)_(2)(HFMA)_(2)W_(8)O_(21)][B-α-SeW_(9)O_(33)]_(4)·_(3)0H_(2)O(4)were prepared by a cooperative strategy of rigid and flexible ligands.展开更多
Rapid-response ratiometric sensors are promising tools to detect trace water and temperature.However,achieving an accurately visualized water assay in a very narrow range is still a challenge.Herein,a novel dual-funct...Rapid-response ratiometric sensors are promising tools to detect trace water and temperature.However,achieving an accurately visualized water assay in a very narrow range is still a challenge.Herein,a novel dual-functional ratiometric luminescent sensor,i.e.,Eu_(2.2)Tb_(97.8)-TCA,was successfully fabricated based on lanthanide metal-organic frameworks.This sensor showed a very fast(less than 20 s)and relatively ultrasensitive(limit of detection 0.016%v/v)response to trace water in ethanol,achieving the sensitive visual determination of water in ethanol with multiple readouts.Intriguingly,visual and quantitative determination of water with a detection limit of 0.035%v/v was achieved based on the ratio of green(G)to red(R)values combined with a smartphone color picker application(APP).展开更多
Aqueous Zn-ion batteries(AZIBs)deliver outstanding potential as next-generation energy storage systems due to the attractive merits of inherent safety and low cost.However,uncurbed dendrite growth and non-negligible w...Aqueous Zn-ion batteries(AZIBs)deliver outstanding potential as next-generation energy storage systems due to the attractive merits of inherent safety and low cost.However,uncurbed dendrite growth and non-negligible water-induced side reactions can be fatal to the stability of Zn anodes and the commercial development of AZIBs.Herein,we construct a bifunctional zincophilic-hydrophobic interfacial layer(STA-ZnO layer)for attaining a stable Zn anode.Exposed hydrophobic alkyl chains can repel H_(2)O to prevent it reaching the Zn foil surface,effectively alleviating the HER and corrosion side reactions.Meanwhile,the zincophilic ZnO ensures that the STA-ZnO@Zn anode accelerates Zn^(2+)deposition and constrains the growth of Zn dendrites.Benefitting from these advantages,symmetric cells based on the STA-ZnO@Zn anode can deliver long-term cycling stability over 4900 h and 4000 h at 1 mA cm^(-2) and 5 mA cm^(-2) for 1 mAh cm^(-2),respectively.Encouragingly,the STA-ZnO@Zn anode also exhibits a high average CE of 99.81%(2000 cycles).This work develops a feasible strategy to protect Zn anodes for achieving the practical application of AZIBs.展开更多
Electrochemical water splitting holds promise for sustainable hydrogen(H_(2))production,yet it faces the challenge of high energy demand due to significant overpotentials and sluggish kinetics for the anodic oxygen ev...Electrochemical water splitting holds promise for sustainable hydrogen(H_(2))production,yet it faces the challenge of high energy demand due to significant overpotentials and sluggish kinetics for the anodic oxygen evolution reaction(OER).An efficient alternative is to replace the energy-intensive OER with the more thermodynamically advantageous alcohol oxidation reaction(AOR).Accordingly,catalysts that enhance both the hydrogen evolution reaction(HER)and the AOR may pave the way for sustainable and efficient hydrogen production.Herein,we demonstrate that the composition and morphology engineering of Rh-Ni alloy nanocrystals can significantly boost their dual functionality for the HER and the ethanol oxidation reaction(EOR).Theoretical and experimental analyses reveal the enhanced H_(2)O dissociation,alcohol oxidation capacity,and CO tolerance of RhNi NCs with predominant{100}facets.As a result,a two-electrode electrolysis cell using RhNi NCs as dual-functional catalysts for the HER||EOR can achieve a current density of 10 mA cm^(-2)and 50 mA cm^(-2)at 0.53 V and 0.68 V,respectively,outperforming the Pt/C and IrO_(2)benchmark catalysts.Remarkably,the RhNi NCs can also catalyze the oxidation of a range of alcohols for energy-saving H_(2)production at low cell voltages.Our strategy represents a rational catalyst design achieved through controlled solution synthesis,holding potential for broader applicability in future electrocatalysis and clean energy conversion.展开更多
文摘A family of Said-Bézier type generalized Ball （SBGB） bases and surfaces with a parameter H over triangular domain is introduced,which unifies Bézier surface and Said-Ball surface and includes several intermediate surfaces. To convert different bases and surfaces,the dual functionals of bases are presented. As an application of dual functionals,the subdivision formulas for surfaces are established.
基金the financial support from the Yunnan Provincial Science and Technology Project at Southwest United Graduate School(Grant No.202302A0370009)the National Natural Science Foundation Joint Fund(Grant No.U21A2072)+4 种基金the National Science Foundation(Grant No.62274099)the Key Project of Tianjin Natural Science Foundation(Grant No.24JCZDJC01360)the China Higher Education Discipline Innovation Overseas Expert Introduction Project(Grant No.B16027)Tianjin Science and Technology Project(Grant No.24ZXZSSS00160)the Special Fund for Basic Scientific Research of the Central Universities。
文摘Inorganic perovskite solar cells(IPSCs),due to their suitable bandgap and superior thermal stability,are ideal candidates for tandem solar cells combined with silicon.However,the development of inorganic perovskite solar cells has been hindered by suboptimal crystallization dynamics that generate detrimental defects in the perovskite lattice.Here,we propose 4-Methoxyphenylphosphonic Acid(4MPA)as a multifunctional additive to address this challenge.P=O in 4MPA establish strong coordination with undercoordinated Pb^(2+),while-OH engage in O...H-O hydrogen bonding interactions with DMSO,effectively weakening the solvent-[PbX_(6)]^(4-)octahedron interaction.This dual functionality facilitates complete and rapid DMA^(+)-to-Cs^(+)cation exchange while regulating crystallization kinetics,thereby optimizing crystal growth.Furthermore,π-π interactions between benzene rings significantly enhance the moisture resistance of the perovskite layer.The optimized device demonstrates a power conversion efficiency(PCE)of 21.35%,with unencapsulated devices retaining 93,63%of their initial efficiency after 200-hour continuous operation under ambient conditions(35%relative humidity).
基金financial support from the Natural Science Foundation of China(No.22001121)Natural Science Foundation of Jiangsu Province(No.BK20180690)+1 种基金Nanjing Tech University(Start-up Grant Nos.39837118 and39837146)Xuzhou Medical University(Start-up Grant No.RC20552038)。
文摘In recent years,the direct introduction of sulfonyl and sulfenyl groups into unsaturated substrates by using thiosulfonates as unique dual functional reagents has inarguably provided chemists a new platform for the diverse synthesis of important S-containing derivatives.These 1,n-thiosulfonylation reactions usually feature simple procedures,100%atom economy,and high regioselectivity.This review focuses on the recent advancements in the transformations of thiosulfonates through 1,n-thiosulfonylation involving the formation of two distinct C-S bonds under transition-metal-catalyzed or metal-free conditions,where thiosulfonates act as both a sulfonyl and a sulfenyl component.
基金Hong Kong Innovation and Technology Commission(InnoHK Project CIMDA).
文摘Several common dual quaternion functions,such as the power function,the magnitude function,the 2-norm function,and the kth largest eigenvalue of a dual quaternion Hermitian matrix,are standard dual quaternion functions,i.e.,the standard parts of their function values depend upon only the standard parts of their dual quaternion variables.Furthermore,the sum,product,minimum,maximum,and composite functions of two standard dual functions,the logarithm and the exponential of standard unit dual quaternion functions,are still standard dual quaternion functions.On the other hand,the dual quaternion optimization problem,where objective and constraint function values are dual numbers but variables are dual quaternions,naturally arises from applications.We show that to solve an equality constrained dual quaternion optimization(EQDQO)problem,we only need to solve two quaternion optimization problems.If the involved dual quaternion functions are all standard,the optimization problem is called a standard dual quaternion optimization problem,and some better results hold.Then,we show that the dual quaternion optimization problems arising from the hand-eye calibration problem and the simultaneous localization and mapping(SLAM)problem are equality constrained standard dual quaternion optimization problems.
基金supported by the National Natural Science Foundation of China(No. 51773209)the National Basic Research Program(No. 2017YFC1103300)the Strategic Priority Research Program of Chinese Academy of Sciences(No. XDB12020300)
文摘Bioactive glass-chitosan-alginate hybrid scaffolds （BG-C-A scaffolds） were fabricated using BG sol as a dual function additive, which behaves as both bioactive inorganic phase to confer the bioactivity and cross-linker to improve the structural stability and mechanical properties. The microstructure, physicochemical and mechanical properties, in vitro bioactivity and cellular biocompatibility of the scaffolds were investigated. The results indicated that BG component was successfully incorporated into the BG-C-A scaffolds through a facile BG sol-immersing method and the original interconnected microstructure could be well preserved. The obtained BG-C-A scaffolds showed improved mechanical properties and structural stability as compared to C-A scaffolds. At the same time, they presented excellent in vitro bioactivity and cellular compatibility. All these results demonstrated that these BG-C-A scaffolds have promising potential for tissue engineering.
基金supported by the National Natural Science Foundation of China (21966006)。
文摘A fluorescent active organic–inorganic hybrid material Py N-SBA-15 was synthesized by implementing pyrene derivatives into mesoporous SBA-15 silica.Py N-SBA-15 had detection and removal functionalities toward Al^(3+),Cu^(2+),and Hg^(2+).On the one hand,Py N-SBA-15 was used as a fluorescence sensor and displayed high sensitivity toward Al^(3+),Cu^(2+),and Hg^(2+)cations (limit of detection:8.0×10^(-7),1.1×10^(-7),and 2.9×10^(-6)mol·L^(–1),respectively) among various analytes with“turn-off”response.On the other hand,the adsorption studies for these toxic analytes (Cu^(2+),Hg^(2+),and Al^(3+)) showed that the ion removal capacity could reach up to 45,581,and 85 mg·g^(-1),respectively.Moreover,the Langmuir isotherm models were better fitted with the adsorption data,indicating that the adsorption was mono-layer adsorption.Kinetic analysis revealed that the adsorption process was well described by the pseudo-second-order kinetic model for Cu^(2+)and Hg^(2+)and pseudo-first-order kinetic model for Al^(3+).The prepared silica material could be reused in four recycles without significantly decreasing its adsorption capacity.Therefore,the Py N-SBA-15 material can serve as a promising candidate for the simultaneous rapid detection and efficient adsorption of metal ions.
基金supported by Ministry of Science and InnovationNational Research Agency(Project PID2019-105960RBC21)+1 种基金by the Basque Government(Project IT1509-2022)One of the authors(JAOC)acknowledges the post-doctoral research grant(DOCREC20/49)provided by the University of the Basque Country。
文摘Integrated CO_(2)capture and utilization(ICCU)technology requires dual functional materials(DFMs)to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8%Na_(2)CO_(3)-8%CaO/γ-Al_(2)O_(3)DFM is studied.The adsorbent precursors are first co-impregnated onto alumina and calcined in air.Then,Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols:static air in muffle or under different mixtures(10%H_(2)/N_(2),50%H_(2)/N_(2)and N_(2))streams.Samples are characterized by XRD,N_(2)adsorption-desorption,H_(2)chemisorption,TEM,XPS,H_(2)-TPD,H_(2)-TPR,CO_(2)-TPD and TPSR.The catalytic behavior is evaluated,in cycles of CO_(2)adsorption and hydrogenation to CH_(4),and temporal evolution of reactants and products concentrations is analyzed.The calcination atmosphere influences the physicochemical properties and,ultimately,activity of DFMs.Characterization data and catalytic performance discover the acccomodation of Ru nanoparticles disposition and basic sites is mostly influencing the catalytic activity.DFM calcined under N_(2)flow(RuNaCa-N_(2))shows the highest CH_(4)production(449μmol/g at 370℃),because a well-controlled decomposition of precursors which favors the better accomodation of adsorbent and Ru phases,maximizing the specific surface area,the Ru-basic sites interface and the participation of different basic sites in the CO_(2)methanation reaction.Thus,the calcination in a N_(2)flow is revealed as the optimal calcination protocol to achieve highly efficient DFM for integrated CO_(2)adsorption and hydrogenation applications.
文摘In this paper,we proved that the infinitesimal generator of a strongly continuous cosine operator function is preserved under the time-dependent perturbation in the sun-reflexive case,where the perturbed operator is a bounded linear operator from X into a bigger space Xθ(not X),then the corresponding 2-order abstract Cauchy problem is uniformly well-posed.
文摘The dual algorithm for minimax problems is further studied in this paper.The resulting theoretical analysis shows that the condition number of the corresponding Hessian of the smooth modified Lagrange function with changing parameter in the dual algorithm is proportional to the reciprocal of the parameter,which is very important for the efficiency of the dual algorithm.At last,the numerical experiments are reported to validate the analysis results.
基金National Key R&D Program of China(2022YFE0105900)National Natural Science Foundation of China(52306179)+1 种基金Science and Technology Innovation Program of Hunan Province(2021RC4006)High Performance Computing Center of Central South University。
文摘The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).
基金supported by the National Natural Science Foundation of China(No.52373249,W2433146)the Science and Technology Project of Yibin Sanjiang New Area(No.2023SJXQSXZJ003)the Fundamental Research Funds for the Central Universities(No.20822041F4045).
文摘Nickel-based cathodes in aqueous nickel-zinc batteries typically suffer from sluggish reaction kinetics and limited energy density.In situ introduction of metal phosphides and rational construction of heterostructures can effectively promote electron/ion transport.However,the complex evolution of phosphidation and intractable phosphidizing degree greatly affect the composition of active phase,active sites,charge transfer rate,and ion adsorption strength of cathodes.Herein,the critical bimetallic phosphide layer(CBPL)is constructed on the NiCo-layered double hydroxide(NiCo-LDH)skeleton by a controllable anion-exchange strategy,yielding a novel nanohybrid cathode(NiCo-P1.0,1.0 representing the mass ratio of Na_(2)H_(2)PO_(2)to NiCo-LDH).The high-conductivity CBPL with the inner NiCo-LDH forms extensive heterostructures,effectively regulating the electronic structure via charge transfer,thereby improving electrical conductivity.Remarkably,the CBPL exhibits unexpected electrochemical activity and synergizes with NiCo-LDH for electrode reactions,ultimately delivering extra energy.Benefiting from the bifunctional CBPL,NiCo-P1.0 delivers an optimal capacity of 286.64 mAh g^(−1)at 1C(1C=289 mAh g^(−1))and superb rate performance(a capacity retention of 72.22%at 40C).The assembled NiCo-P1.0//Zn battery achieves ultrahigh energy/power density(503.62 Wh kg^(−1)/18.62 kW kg^(−1),based on the mass loading of active material on the cathode),and the flexible quasi-solid-state pouch cell validates its practicality.This work demonstrates the superiority of bifunctional CBPL for surface modification,providing an effective and scalable compositing strategy in achieving high-performance cathodes for aqueous batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.21975044,21971038,21922810 and 22271046)the Fujian Provincial Department of Science and Technology(Nos.2023J01355,2023J011106 and 2022R1022001).
文摘Achieving efficient adsorption and separation of C_(2)H_(2)/CO_(2)mixtures is a goal that people have always pursued to improve the situation of high energy consumption brought by traditional separation technologies in industry today.High-nuclearity metal cluster-based MOFs with different functionalities are promising for this separation,but it is a complicated and difficult task to precisely control their structures.The strategy of pore-space partition(PSP)is a powerful way to construct this type MOFs,which has the characteristic of isostructural relationship,and can be resulted in a similar performance for them.Therefore,it is an interesting work to explore the effect of MOFs property by adjusting the size of PSP dividers.Herein,three tetranuclear Cu(Ⅱ)cluster-based MOFs(FJU-112/113/114)with dual functionalities has been successfully obtained by PSP strategy with various lengths of divider units.With the highest microporosity and unique functional site,FJU-114 realized a good improvement in the adsorption and separation performance of C_(2)H_(2)/CO_(2).The gas adsorption and lab-scale C_(2)H_(2)/CO_(2)breakthrough experiments demonstrated that FJU-114 exhibits the highest adsorption uptake of 77 cm^(3)/g for C_(2)H_(2),and shows the best separation factor of 4.2 among three MOFs.The GCMC simulation reveals that a stronger adsorption binding site of C_(2)H_(2)in FJU-114a located in the cage II near the unchanged tetranuclear copper node,combined with its high microporosity to achieve the effect of dual functionalities for the improvement performance of C_(2)H_(2)adsorption and separation.
基金supported by the National Natural Science Foundation of China(32301044 and 32371345)Anhui Provincial Natural Science Foundation(2308085QC80)+5 种基金the National Key R&D Program of China(2022YFA1302700 and 2022YFC2303700)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0490000)Center for Advanced Interdisciplinary Science and Biomedicine of IHM(QYPY20220019)the Fundamental Research Funds for the Central Universities(WK9100000032 and WK9100000044)the USTC startup funding(KY9100000032,KY9100000056,and KJ2070000080)National Science and Technology Council of Taiwan(NSTC108-2320-B-001-011-MY3).
文摘The Lon proteases are evolutionarily conserved oligomeric hydrolases characterized by a built-in ATPase module.Here,we report the structures of LonC from Meiothermus taiwanensis(MtaLonC),a unique member in the Lon protein family with a dual chaperone-protease function but lacking ATPase activity,determined by cryo-electron microscopy(cryo-EM).In its apo state,LonC forms phosphate-bound open-ring pentamers,open-ring hexamers,and close-ring heptamers.However,upon interaction with ATPγS,inhibitor,or substrate,MtaLonC assembles into close-ring hexamers,wherein the protease domain’s substrate-binding loop adopts an extended active conformation.We show that proteolytic and chaperone activities may be carried out by the close-ring hexameric and heptameric forms,respectively.We further show that MtaLonC forms exclusively close-ring heptamers at elevated temperatures.This study sheds light on the bifurcated assembly pathway of MtaLonC,leading to two distinct oligomeric close-ring complexes that carry out a dual function.
基金National Natural Science Foundation of China(Grant No.21671118)Taishan Scholars Program。
文摘A new class of cyclometalated iridium(III)complexes with imine-N-heterocyclic carbenes(NHC)as ligands were synthesized and fully characterized.One crystal structure is reported.All the six complexes exhibited highly potent anticancer activity against A549 cells,HeLa cells,HepG2 cells,GL261 cells and A549R cells.In particular,they were up to 9 and 37 times more potent than clinically used anticancer drug cisplatin towards A549 and A549R cell lines,respectively.Remarkably,mechanism studies showed that the complexes pass into cancer cells through an energy-dependent pathway and cause apoptosis via reactive oxygen species(ROS)generation,mitochondrial membrane potential dysfunction,and lysosomal damage.In addition,complex Ir6 effectively impeded cell migration and colony formation.
基金supported by National Key R&D Program of China(2017YFA0206700&2016YFB0101200)National Natural Science Foundation of China(grant no.51671107&21603108)111 project of B12015.
文摘Desalination of seawater and renewable energy storage are quite promising for a sustainable society,but their combination for high efficiency is a difficult task.Herein,we demonstrate a dual-function battery,which is composed of a NaTi_(2)(PO_(4))_(3) anode and a Ag cathode with NaCl aqueous electrolyte,for desalination and electrical energy storage.In a charging process,Na+and Cl-are extracted from the electrolyte and inserted into the separate electrodes,while in a reverse process,the stored electricity and ions are released into electrolyte.As a demonstration,the dual-function battery can be continuously photocharged with a solar cell and discharged for 50 cycles without significant decrease in both the discharge voltage and capacity.This study will provide new insights into both seawater desalination and efficient renewable energy utilization.
基金supported by the National Natural Science Foundation of China(grant no.22073032).
文摘The adsorption,degradation,and sensing of chemical warfare agents are highly important.In this work,a new Zr_((IV))-based metal-organic gel(MOG)was designed and synthesized,which demonstrated dualfunctional performance in the degradation of nerve agent simulants and the adsorptive sensing of blister agent simulants.A Zr_((IV))-based MOG,namely,Zr-MOG-taBDC(H_(2)taBDC=2-(1H-1,2,4-triazol-1-yl)terephthalic acid),was synthesized through the thermal transformation of a tetrahedral Zr_((IV))-based metal-organic cage,{[Cp_(3)Zr_(3)(μ_(3)-O)(μ_(2)-OH)_(3)]_(4)(taBDC)_(6)}·(Cl^(-))_(4)(Zr-MOC-taBDC),in a mixed acetonitrile/water solvent system,bypassing the need for tedious anion exchange and high-boiling solvents.The resulting MOG exhibited hierarchical porosity and high stability across a wide pH range(1-11).Catalytic tests revealed that Zr-MOG-taBDC achieved 95.4%degradation efficiency for the nerve agent simulant diethyl phenylphosphonate(DEPPT),with a half-life of 49.5 minutes,outperforming its crystalline MOC precursor.Additionally,the gel demonstrated a high adsorption capacity(0.6 g g^(-1))for the mustard gas simulant 2-chloroethyl ethyl sulfide(CEES),enabling real-time detection via a quartz crystal microbalance(QCM)with a linear response range up to 100 ppm.Mechanistic studies indicated that degradation proceeds via P-S bond cleavage catalyzed by Zr-OH-H_(2)O Lewis acid-base sites,whereas adsorption involves reversible physical and irreversible chemical interactions with triazole groups and Zr-oxo clusters.This work highlights the potential of Zr-MOGs as multifunctional materials for chemical warfare agent mitigation and sensing.
基金supported by the National Natural Science Foundation of China(21871077,22071042,22101072,and 22171070)the Program for Innovation Teams in Science and Technology in Universities of Henan Province(20IRTSTHN004)+1 种基金the China Postdoctoral Science Foundation(2021M701067)the Innovation and Entrepreneurship Training Program for College Students of Henan University(202210475001 and 20222404112).
文摘A series of rigid-flexible-ligand functionalized dodeca-nuclear lanthanide-tungsten heterometal cluster incorporated ring-shaped selenotungstates[H_(2)N(CH_(3))_(2)]_(16)Na_(2)[Ln_(4)(H_(2)O)_(6)(HPZDA)_(2)(HFMA)_(2)W_(8)O_(21)][B-α-SeW_(9)O_(33)]_(4)·_(2)_(9)H_(2)O[Ln=Ce^(3+)(1),Pr^(3+)(2),Nd^(3+)(3);H_(2)PZDA=2,3-pyrazine dicarboxylic acid,H_(2)FMA=fumaric acid]and[H_(2)N(CH_(3))_(2)]_(14)Cs_(2)Na_(2)[Eu4(H_(2)O)_(6)(HPZDA)_(2)(HFMA)_(2)W_(8)O_(21)][B-α-SeW_(9)O_(33)]_(4)·_(3)0H_(2)O(4)were prepared by a cooperative strategy of rigid and flexible ligands.
基金support of National Natural Science Foundation of China(Projects 21871121)Science and Technological Plan of Gansu Province(20YF3GA012)the 111 project(B20027).
文摘Rapid-response ratiometric sensors are promising tools to detect trace water and temperature.However,achieving an accurately visualized water assay in a very narrow range is still a challenge.Herein,a novel dual-functional ratiometric luminescent sensor,i.e.,Eu_(2.2)Tb_(97.8)-TCA,was successfully fabricated based on lanthanide metal-organic frameworks.This sensor showed a very fast(less than 20 s)and relatively ultrasensitive(limit of detection 0.016%v/v)response to trace water in ethanol,achieving the sensitive visual determination of water in ethanol with multiple readouts.Intriguingly,visual and quantitative determination of water with a detection limit of 0.035%v/v was achieved based on the ratio of green(G)to red(R)values combined with a smartphone color picker application(APP).
基金supported by Research Contract for High Performance Aqueous Zinc Ion Battery Technology[grant numbers A342-JS-2024-0007]the Opening Project of thenState Key Laboratory of Special Chemical Power Sources[grant numbers SKL-ACPS-C-03]the Natural Science Foundation of Chongqing(CSTB2023NSCQ-MSX0617)。
文摘Aqueous Zn-ion batteries(AZIBs)deliver outstanding potential as next-generation energy storage systems due to the attractive merits of inherent safety and low cost.However,uncurbed dendrite growth and non-negligible water-induced side reactions can be fatal to the stability of Zn anodes and the commercial development of AZIBs.Herein,we construct a bifunctional zincophilic-hydrophobic interfacial layer(STA-ZnO layer)for attaining a stable Zn anode.Exposed hydrophobic alkyl chains can repel H_(2)O to prevent it reaching the Zn foil surface,effectively alleviating the HER and corrosion side reactions.Meanwhile,the zincophilic ZnO ensures that the STA-ZnO@Zn anode accelerates Zn^(2+)deposition and constrains the growth of Zn dendrites.Benefitting from these advantages,symmetric cells based on the STA-ZnO@Zn anode can deliver long-term cycling stability over 4900 h and 4000 h at 1 mA cm^(-2) and 5 mA cm^(-2) for 1 mAh cm^(-2),respectively.Encouragingly,the STA-ZnO@Zn anode also exhibits a high average CE of 99.81%(2000 cycles).This work develops a feasible strategy to protect Zn anodes for achieving the practical application of AZIBs.
基金financial support from the National Natural Science Foundation of China(No.22322101 and 21971012)the Beijing Municipal Natural Science Foundation(JQ20007)the Beijing Institute of Technology Research Fund Program.
文摘Electrochemical water splitting holds promise for sustainable hydrogen(H_(2))production,yet it faces the challenge of high energy demand due to significant overpotentials and sluggish kinetics for the anodic oxygen evolution reaction(OER).An efficient alternative is to replace the energy-intensive OER with the more thermodynamically advantageous alcohol oxidation reaction(AOR).Accordingly,catalysts that enhance both the hydrogen evolution reaction(HER)and the AOR may pave the way for sustainable and efficient hydrogen production.Herein,we demonstrate that the composition and morphology engineering of Rh-Ni alloy nanocrystals can significantly boost their dual functionality for the HER and the ethanol oxidation reaction(EOR).Theoretical and experimental analyses reveal the enhanced H_(2)O dissociation,alcohol oxidation capacity,and CO tolerance of RhNi NCs with predominant{100}facets.As a result,a two-electrode electrolysis cell using RhNi NCs as dual-functional catalysts for the HER||EOR can achieve a current density of 10 mA cm^(-2)and 50 mA cm^(-2)at 0.53 V and 0.68 V,respectively,outperforming the Pt/C and IrO_(2)benchmark catalysts.Remarkably,the RhNi NCs can also catalyze the oxidation of a range of alcohols for energy-saving H_(2)production at low cell voltages.Our strategy represents a rational catalyst design achieved through controlled solution synthesis,holding potential for broader applicability in future electrocatalysis and clean energy conversion.
