Accurately counting dense objects in complex and diverse backgrounds is a significant challenge in computer vision,with applications ranging from crowd counting to various other object counting tasks.To address this,w...Accurately counting dense objects in complex and diverse backgrounds is a significant challenge in computer vision,with applications ranging from crowd counting to various other object counting tasks.To address this,we propose HUANNet(High-Resolution Unified Attention Network),a convolutional neural network designed to capture both local features and rich semantic information through a high-resolution representation learning framework,while optimizing computational distribution across parallel branches.HUANNet introduces three core modules:the High-Resolution Attention Module(HRAM),which enhances feature extraction by optimizing multiresolution feature fusion;the Unified Multi-Scale Attention Module(UMAM),which integrates spatial,channel,and convolutional kernel information through an attention mechanism applied across multiple levels of the network;and the Grid-Assisted Point Matching Module(GPMM),which stabilizes and improves point-to-point matching by leveraging grid-based mechanisms.Extensive experiments show that HUANNet achieves competitive results on the ShanghaiTech Part A/B crowd counting datasets and sets new state-of-the-art performance on dense object counting datasets such as CARPK and XRAY-IECCD,demonstrating the effectiveness and versatility of HUANNet.展开更多
Lithium-ion batteries(LIBs)face significant limitations in low-temperature environments,with the slow interfacial de-solvation process and the hindered Li+transport through the interphase layer emerging as key obstacl...Lithium-ion batteries(LIBs)face significant limitations in low-temperature environments,with the slow interfacial de-solvation process and the hindered Li+transport through the interphase layer emerging as key obstacles beyond the issue of ionic conductivity.This investigation unveils a novel formulation that constructs an anion-rich solvation sheath within strong solvents,effectively addressing all three of these challenges to bolster low-temperature performance.The developed electrolyte,characterized by an enhanced concentration of contact ion pairs(CIPs)and aggregates(AGGs),facilitates the formation of an inorganic-rich interphase layer on the anode and cathode particles.This promotes de-solvation at low temperatures and stabilizes the electrode-electrolyte interphase.Full cells composed of LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)and graphite,when equipped with this electrolyte,showcase remarkable cycle stability and capacity retention,with 93.3% retention after 500 cycles at room temperature(RT)and 95.5%after 120 cycles at -20℃.This study validates the utility of the anion-rich solvation sheath in strong solvents as a strategy for the development of low-temperature electrolytes.展开更多
Coal-based soild wastes(CBSWs)are industrial byproducts that can be harmful to the environment.The exploitation and utilization of CBsWs offer societal advantages such as resource conservation,pollution reduction,and ...Coal-based soild wastes(CBSWs)are industrial byproducts that can be harmful to the environment.The exploitation and utilization of CBsWs offer societal advantages such as resource conservation,pollution reduction,and cost-effective production.However,environmentally sustainable management remains a worldwide challenge due to the substantial production volume and limited disposal capacity of CBSWs.The physicochemical properties and utilization of CBSWs are summarized,including fly ash,coal gangue and coal gasification slag.It also presents the current global applications status of CBSWs resources and examines market supply and demand.Subsequently,the paper provides an overview of studies on ways to utilise CBSWs,highlighting the primary avenues of CBSWs resource utilization which are mainly from the fields of chemical materials,metallurgy and agriculture.Furthermore,a comparative evaluation of the various methods for CBSWs resource recovery is conducted,outlining their respective advantages and disadvantages.The future development of CBSWs recycling processes is also discussed.The review concludes that while there is a growing need for attention in CBSWs recycling,its utilization will involve a combination of both large-scale treatment and refinement processes.The paper aims to offer references and insights for the effective utilization and environmental protection of CBSWs.Future direction will focus on the collaborative utilization of CBSWs,emphasizing on the combination of large-scale and high-value utilization.In addition,there is a need to establish a comprehensive database based on on-site production practices,explore on-site solutions to reduce transportation costs,and improve physicochemical properties during the production process.展开更多
Electrocatalysts are an effective strategy to mitigate the shuttling effect of lithium polysulfides(LiPSs)and accelerate the redox kinetics of LiPSs in lithium-sulfur(Li-S)batteries.However,traditional electrocatalyst...Electrocatalysts are an effective strategy to mitigate the shuttling effect of lithium polysulfides(LiPSs)and accelerate the redox kinetics of LiPSs in lithium-sulfur(Li-S)batteries.However,traditional electrocatalysts only have a single active site and often undergo structural collapse and aggregation during charging and discharging,resulting in reduced catalytic performance.Herein,the two-dimensional(2D)polar high-entropy La_(0.71)Sr_(0.29)Co_(0.21)Ni_(0.20)Fe_(0.19)Cr_(0.20)Cu_(0.20)O_(3)(LCO-HEO)nanosheets were rationally designed and successfully synthesized to address this issue.The distinct functional polar sites in LCOHEOs were formed by the d-d orbital hybridization between spatially coupling adjacent transition metals,which can strengthen the dipole-dipole interaction between polar LCO-HEOs and polar LiPSs.2D polar LCO-HEO nanosheets can efficiently capture and trigger the tandem catalysis of polar LiPSs during their sequential conversion.The S/LCO-HEO composite cathode exhibits a high specific capacity of 1161.1 mA h g^(-1)at 1.0 C,with an ultralow capacity attenuation rate of 0.036%per cycle over 1200 cycles,and achieves stable cycling for 1500 cycles even at 8.0 C.Furthermore,even with a high sulfur loading(5.5 mg cm^(-2))and a low electrolyte/sulfur(E/S)ratio(4.0μL mg^(-1)),the S/LCO-HEO composite cathode shows desirable sulfur utilization and good cycle stability.This work demonstrates the feasibility of high entropy-driven multiple distinct functional polar sites for high-rate and long-cycle Li-S batteries.展开更多
A transition-metal-and oxidant-free amination/cyclization reaction to access 1,2,4-triazolo[1,5-a]pyridines was realized in water by using amino diphenylphosphinate as amino source.A broad array of readily accessible ...A transition-metal-and oxidant-free amination/cyclization reaction to access 1,2,4-triazolo[1,5-a]pyridines was realized in water by using amino diphenylphosphinate as amino source.A broad array of readily accessible N-(pyridyl)amides could be converted into the products featuring a diverse set of functional groups.The sustainable methodology was successfully applied to the late-stage functionalization of natural products and drugs.展开更多
The removal of cesium-137(^(137)Cs)from nuclear wastewater remains crucial due to its radioactivity and high solubility in water,which pose serious risk to human health and the environment.Aiming at selective capture ...The removal of cesium-137(^(137)Cs)from nuclear wastewater remains crucial due to its radioactivity and high solubility in water,which pose serious risk to human health and the environment.Aiming at selective capture of Cs^(+) from wastewater,a core-shell adsorbent,Prussian blue analog@y-alumina(PBA@Al_(2)O_(3))pellets were synthesized using the hydrothermal-stepwise deposition method.The coreshell PBA@Al_(2)O_(3)pellets showcased a PBA loading of 25%and demonstrated a maximum adsorption capacity of 15.65 mg·g^(-1).The adsorption data was consistent with the pseudo-second-order kinetic model and the Langmuir isotherm model.It effectively reduced bulk Cs^(+) concentrations from an initial 6.62 mg·L^(-1)to 2 μg·L^(-1),achieving a removal efficiency of 99.97%and distribution coefficient(Kd)of 1.265×10^(6)ml·g^(-1),surpassing the performance of other PBA-based materials.The material also indicated good mechanical properties and cesium ion removal rates of 99.7%across a wide pH range(1.82 to 11.12).Furthermore,PBA@Al_(2)O_(3)exhibited consistent removal rate of over 99%and good selectivity(SF=50-1600)towards Cs^(+) even in the presence of interfering ions such as Na^(+),K^(+),Mg^(2+),and Ca^(2+)ions.The Kd(Cs^(+))for PBA@Al2O3 in simulated seawater and groundwater were 9.92×10^(3)and 2.23×10^(4)ml·g^(-1),where the removal rates reached 96.1%and 98.2%,respectively.XPS confirms that the adsorption mechanism is the ion exchange between Cs^(+) and K^(+)ions.This study underscores the significant potential of inorganic core-shell pellets adsorbents as promising agents for the selective capture of Cs^(+) from wastewater.展开更多
A wide range of isoquinoline ring-modified Quinap oxides with different steric and electronic variations have been constructed through a palladium-catalyzed imidoylative cyclization of arylethenyl isocyanides with 2-d...A wide range of isoquinoline ring-modified Quinap oxides with different steric and electronic variations have been constructed through a palladium-catalyzed imidoylative cyclization of arylethenyl isocyanides with 2-diphenylphosphinyl-1-naphthyl bromides.The Pd-catalysis plays dual roles in the formation of both axial C–C bond and isoquinoline ring.This de novo synthetic strategy features good functional group tolerance,high yields and easy scale-up,providing Quinap derivatives with substitution patterns that could not be obtained using coupling reactions.Chiral ligands 7 and 12 can be readily prepared by transformation of the resulting Quinap oxide to their BINOL esters,and have been proven to be superb chiral ligands for the copper-catalyzed enantioselective A^(3)-coupling and alkynylation of quinoline reactions.In general,the enantioselectivies obtained using ligands 7 and 12 are excellent,and the ee values are higher than those using Quinap as ligand,even three times higher in some cases.Mechanism studies revealed that a monomeric copper(Ⅰ)complex bearing a single chiral ligand was formed and served as the catalytically active species.展开更多
The lead-free inorganic perovskite CsSnI_(3) is considered as one of the best candidates for emerging photovoltaics.Nevertheless,CsSnI_(3)-based perovskite solar cells experience a significant drop in performance due ...The lead-free inorganic perovskite CsSnI_(3) is considered as one of the best candidates for emerging photovoltaics.Nevertheless,CsSnI_(3)-based perovskite solar cells experience a significant drop in performance due to the nonradiative recombination facilitated by trapping.Here,we show an electron donor passivation method to regulate deep-level defects for CsSnI_(3) perovskite with electron donor pyrrole.Experimental observations combined with theoretical simulations verify that the saturation of Tin dangling bonds with pyrrole on the CsSnI_(3) surface via a Lewis acid-base addition reaction can significantly reduce the density of deep-level defects.Consequently,the printable mesoporous perovskite solar cells with an FTO/compact-TiO_(2)/mesoporous-TiO_(2)/Al_(2)O_(3)/NiO/carbon framework device structure penetrated with CsSnI_(3) achieve a power conversion efficiency of up to 10.11%.To our knowledge,this represents the highest efficiency reported to date for lead-free pero vs kite-based printable mesoporous solar cells.Furthermore,the unencapsulated devices demonstrated remarkable long-term stability,retaining 92%of their initial efficiency even after 2400 h of aging in a nitrogen atmosphere.展开更多
Ti-xNb alloys produced by laser powder bed fusion(LPBF)from mixed powder usually exhibit an inhomogeneous elemental distribution,leading to a deterioration in mechanical properties.To address this issue,we proposed a ...Ti-xNb alloys produced by laser powder bed fusion(LPBF)from mixed powder usually exhibit an inhomogeneous elemental distribution,leading to a deterioration in mechanical properties.To address this issue,we proposed a strategy to achieve heterostructure in laser powder bed fused Ti-xNb alloys from mixed powders through precipitation ofωwithinβ.Moreover,the effect of Nb content on the micro structure and mechanical behavior of Ti-xNb alloys was studied.The results indicated that in-situ laser re-melting can realize the homogeneous elemental distribution in Ti-xNb alloys.When the Nb content increases from 30 wt%,35 wt%to40 wt%,Ti-xNb alloys experience a transformation from β+α' to β+ω and monolithic β.Specifically,ωnano-precipitates in Ti-35Nb alloy are only distributed in some β grains,forming a heterostructure with“softβ”and“hard β+ω”grains.As a result,LPBF-produced Ti-35Nb alloy demonstrates excellent mechanical properties,with yield strength of ^(792±6)MPa,tensile strength of ^(806±7)MPa,Young's modulus of ^(68±6)GPa,and uniform elongation of ^(18.0±1.1)%.The Frank-Read mechanism induces dislocation proliferation and dislocation cross-slip,and the geometrically necessary dislocations(GNDs)are induced at the heterogeneous interface of“softβ”and“hard β+ω”grains,resulting in an enhancement in the strength-ductility synergy of Ti-35Nb alloy produced by LPBF.This work provides an innovative strategy to improve the strength-ductility synergy of LPBF-produced Ti-xNb alloys from mixed powders by tailoring ω nano-precipitates.展开更多
Dear Editor,People are often optimistic when forecasting the future,such that they believe they are less likely to encounter adverse life events.This phenomenon,known as optimism bias,emerges due to preferential encod...Dear Editor,People are often optimistic when forecasting the future,such that they believe they are less likely to encounter adverse life events.This phenomenon,known as optimism bias,emerges due to preferential encoding and consolidation of desirable over undesirable information[1,2],engaging frontal brain regions such as the anterior cingulate cortex and inferior frontal gyrus[1].An optimism bias is instrumental in supporting mental health:reduction or absence of optimism biases is associated with mood disorders such as depression,characterized by pessimistic thinking about the future[3].This relationship highlights the potential value of interventions that could enhance optimism bias[4].展开更多
Metal–organic frameworks(MOFs) packed in the column have been a promising candidate as the stationary phase for high performance liquid chromatography(HPLC). However, the direct packing of irregular MOF powder could ...Metal–organic frameworks(MOFs) packed in the column have been a promising candidate as the stationary phase for high performance liquid chromatography(HPLC). However, the direct packing of irregular MOF powder could raise some problems like high back pressure and low column efficiency in the HPLC separation. In this work, UiO-66 capable of separating xylenes was supported effectively on the surface of the monodisperse spherical silica microspheres by one-pot method. The hybridization of Ui O-66 and silica microspheres(termed UiO-66@SiO2 shell–core composite) was prepared by stirring the suspension of the precursors of Ui O-66 and\\COOH terminated silica in the N,N-dimethylformamide with heating. The shell–core composite material UiO66@SiO2 was characterized by SEM, TEM, PXRD and FTIR. Then, it was used as a packing material for the chromatographic separation of xylene isomers. Xylene isomers including o-xylene, m-xylene and p-xylene were efficiently separated on the column with high resolution and good reproducibility. Moreover, the Ui O-66@SiO2 shell–core composites packed column still remained reverse shape selectivity as Ui O-66 possessed, and the retention of xylenes was probably ascribed to the hydrophobic effect between analytes and the aromatic rings of the Ui O-66 shell. The Ui O-66@SiO2 shell–core composites obtained in this study have some potential for the separation of structural isomers in HPLC.展开更多
OSAHS(Obstructive Sleep Apnea Hypopnea Syndrome)is a respiratory disease mainly characterized by limited and repeated pauses of breathing in sleep.Currently,the optimal treatment is to apply CPAP(Continuous Positive A...OSAHS(Obstructive Sleep Apnea Hypopnea Syndrome)is a respiratory disease mainly characterized by limited and repeated pauses of breathing in sleep.Currently,the optimal treatment is to apply CPAP(Continuous Positive Airway Pressure)ventilation on the upper airway of the patient through a household respiratory machine.However,if the ventilator mask is designed improperly,it might cause the residue and repeated inhalation of CO2,which will exert an adverse impact on the therapeutic effect.Present research numerically analyzed the CO2 transportation inside a commercial ventilator mask(Mirage SoftGel,ResMed,Australia)based on the reconstructed 3D numerical model of a volunteer's face and performed the improved design of the ventilator mask in terms of the CO2 residual concentration below the nostrils.The fluid dynamic analyses showed that at the end time of expiratory,the CO2 residual concentration below the nostrils is close to 4%.To improve the therapeutic effect,we changed the position of the exhaust holes and found that by moving the exhaust holes to the bottom of the ventilator mask,the CO2 residual concentration below the nostrils would be reduced to no more than 1%.This study established a near physiological computational model and provided a new method for the individualized design of the commercial ventilator mask.展开更多
Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through soluti...Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through solution manufacturing.Herein,we report a solution-processed flexible OSC based on a transparent conducting PEDOT:PSS anode doped with trifluoromethanesulfonic acid(CF3SO3H).Through a low-concentration and low-temperature CF3SO3H doping,the conducting polymer anodes exhibited a main sheet resistance of 35Ωsq−1(minimum value:32Ωsq−1),a raised work function(≈5.0 eV),a superior wettability,and a high electrical stability.The high work function minimized the energy level mismatch among the anodes,hole-transporting layers and electron-donors of the active layers,thereby leading to an enhanced carrier extraction.The solution-processed flexible OSCs yielded a record-high efficiency of 16.41%(maximum value:16.61%).Besides,the flexible OSCs afforded the 1000 cyclic bending tests at the radius of 1.5 mm and the long-time thermal treatments at 85°C,demonstrating a high flexibility and a good thermal stability.展开更多
Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3...Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3 D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti_3 C_2 T_x flakes on sulfur-impregnated carbon cloth(Ti_3 C_2 T_x@S/CC) to achieve high loading and high energy density Li-S batteries,in which,the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer,while the outer-coated Ti_3 C_2 T_x can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode,achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion.Due to these advantages,at a sulfur loading of 4 mg cm^(-2),Li-S cells with Ti_3 C_2 T_x@S/CC cathodes can deliver outstanding cycling stability(746.1 mAh g^(-1) after 200 cycles at1 C),superb rate performance(866.8 mAh g^(-1) up to 2 C) and a high specific energy density(564.2 Wh kg^(-1) after 100 cycles at 0.5 C).More significantly,they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm^(-2) at the increased loading of 8 mg cm^(-2).展开更多
Electrode material based on a novel core–shell structure consisting of NiCoS（NCS） solid fiber core and Mn S（MS） sheet shell（NCS@MS） in situ grown on carbon cloth（CC） has been successfully prepared by a simple...Electrode material based on a novel core–shell structure consisting of NiCoS（NCS） solid fiber core and Mn S（MS） sheet shell（NCS@MS） in situ grown on carbon cloth（CC） has been successfully prepared by a simple sulfurization-assisted hydrothermal method for high performance supercapacitor. The synthesized NiCoS@Mn S/CC electrode shows high capacitance of 1908.3 F gat a current density of 0.5 A gwhich is higher than those of NiCoSand Mn S at the same current density. A flexible all-solid-state asymmetric supercapacitor（ASC） is constructed by using NiCoS@Mn S/CC as positive electrode, active carbon/CC as negative electrode and KOH/poly（vinyl alcohol）(PVA) as electrolyte. The optimized ASC shows a maximum energy density of 23.3 Wh kgat 1 A g, a maximum power density of about7.5 kw kgat 10 A gand remarkable cycling stability. After 9000 cycles, the ASC still exhibited67.8% retention rate and largely unchanged charge/discharge curves. The excellent electrochemical properties are resulted from the novel core–shell structure of the NiCoS@Mn S/CC electrode, which possesses both high surface area for Faraday redox reaction and superior kinetics of charge transport. The NiCoS@Mn S/CC electrode shows a promising potential for energy storage applications in the future.展开更多
Rosa rugosa Thunb.is recognized as both medicine and edible in China.The article investigated the antitumor activity of rose flavonoids.Water-extracted rose flavonoids(RFW)and ethanol-extracted rose flavonoids(RFE)wer...Rosa rugosa Thunb.is recognized as both medicine and edible in China.The article investigated the antitumor activity of rose flavonoids.Water-extracted rose flavonoids(RFW)and ethanol-extracted rose flavonoids(RFE)were achieved by extracting with distilled water and 70%ethanol,respectively.The effects of the two extracts on proliferation inhibition,apoptosis inducement and metastasis prevention of human HepG2 hepatocellular carcinoma cell lines were tested,via optical/fluorescence microscopy,MTT detection,Transwell assay,flow cytometry and Western blot,etc.The results indicated that rose flavonoids at low concentration(10-40μg/mL)had a better inhibitory effect on migration and invasion of HepG2 cells in a dose-dependent manner,while rose flavonoids at high concentration(80-160μg/mL)could induce apoptosis of HepG2 cells by up-regulating the expression of pro-apoptotic proteins p53 and Bax,and down-regulating the expression of anti-apoptotic proteins Bcl-2,leading to the functioning of caspase-3 and caspase-9.The effect of RFE at the same concentration was significantly better than that of RFW.Conclusion,this study found that rose flavonoids had a certain inhibitory effect on proliferation and metastasis of human liver cancer cells HepG2,indicating the application of rose flavonoids in preventing and treating of liver cancer.展开更多
MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their p...MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their practical application in lithium-ion batteries.In this work,a robust strategy is developed to control the functional groups of Nb_2 CT_x MXene.The capacity of pristine Nb_2 CT_x MXene can be significantly increased by Li~+ intercalation and surface modification.The specific capacity of the treated Nb_2 CT_x is up to 448 mAh g^(-1) at 0.05 A g^(-1),and at a large current density of 2 A g^(-1) remains a high reversible capacity retention rate of 75% after an ultra-long cycle of 2000 cycles.These values exceed most of the reported pristine MXenes(including the most studied Ti_3 C_2 T_x) and carbon-based materials.It demonstrates that this strategy has great help to improve the electrochemical performance of pristine MXene,and the results enhance the promise of MXenes in the application of lithium-ion batteries.展开更多
基金funded by the National Natural Science Foundation of China(62273213,62472262,62572287)Natural Science Foundation of Shandong Province(ZR2024MF144)+1 种基金Natural Science Foundation of Shandong Province for Innovation and Development Joint Funds(ZR2022LZH001)Taishan Scholarship Construction Engineering.
文摘Accurately counting dense objects in complex and diverse backgrounds is a significant challenge in computer vision,with applications ranging from crowd counting to various other object counting tasks.To address this,we propose HUANNet(High-Resolution Unified Attention Network),a convolutional neural network designed to capture both local features and rich semantic information through a high-resolution representation learning framework,while optimizing computational distribution across parallel branches.HUANNet introduces three core modules:the High-Resolution Attention Module(HRAM),which enhances feature extraction by optimizing multiresolution feature fusion;the Unified Multi-Scale Attention Module(UMAM),which integrates spatial,channel,and convolutional kernel information through an attention mechanism applied across multiple levels of the network;and the Grid-Assisted Point Matching Module(GPMM),which stabilizes and improves point-to-point matching by leveraging grid-based mechanisms.Extensive experiments show that HUANNet achieves competitive results on the ShanghaiTech Part A/B crowd counting datasets and sets new state-of-the-art performance on dense object counting datasets such as CARPK and XRAY-IECCD,demonstrating the effectiveness and versatility of HUANNet.
基金the National Natural Science Foundation of China(No.22279070[L.Wang]and U21A20170[X.He])the Ministry of Science and Technology of China(No.2019YFA0705703[L.Wang])。
文摘Lithium-ion batteries(LIBs)face significant limitations in low-temperature environments,with the slow interfacial de-solvation process and the hindered Li+transport through the interphase layer emerging as key obstacles beyond the issue of ionic conductivity.This investigation unveils a novel formulation that constructs an anion-rich solvation sheath within strong solvents,effectively addressing all three of these challenges to bolster low-temperature performance.The developed electrolyte,characterized by an enhanced concentration of contact ion pairs(CIPs)and aggregates(AGGs),facilitates the formation of an inorganic-rich interphase layer on the anode and cathode particles.This promotes de-solvation at low temperatures and stabilizes the electrode-electrolyte interphase.Full cells composed of LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)and graphite,when equipped with this electrolyte,showcase remarkable cycle stability and capacity retention,with 93.3% retention after 500 cycles at room temperature(RT)and 95.5%after 120 cycles at -20℃.This study validates the utility of the anion-rich solvation sheath in strong solvents as a strategy for the development of low-temperature electrolytes.
基金supported by the following:“National Natural Science Foundation of China”(22478231)“Natural Science Foundation of Henan”(242300421449)“Fundamental Research Program of Shanxi Province”(202403021221011).
文摘Coal-based soild wastes(CBSWs)are industrial byproducts that can be harmful to the environment.The exploitation and utilization of CBsWs offer societal advantages such as resource conservation,pollution reduction,and cost-effective production.However,environmentally sustainable management remains a worldwide challenge due to the substantial production volume and limited disposal capacity of CBSWs.The physicochemical properties and utilization of CBSWs are summarized,including fly ash,coal gangue and coal gasification slag.It also presents the current global applications status of CBSWs resources and examines market supply and demand.Subsequently,the paper provides an overview of studies on ways to utilise CBSWs,highlighting the primary avenues of CBSWs resource utilization which are mainly from the fields of chemical materials,metallurgy and agriculture.Furthermore,a comparative evaluation of the various methods for CBSWs resource recovery is conducted,outlining their respective advantages and disadvantages.The future development of CBSWs recycling processes is also discussed.The review concludes that while there is a growing need for attention in CBSWs recycling,its utilization will involve a combination of both large-scale treatment and refinement processes.The paper aims to offer references and insights for the effective utilization and environmental protection of CBSWs.Future direction will focus on the collaborative utilization of CBSWs,emphasizing on the combination of large-scale and high-value utilization.In addition,there is a need to establish a comprehensive database based on on-site production practices,explore on-site solutions to reduce transportation costs,and improve physicochemical properties during the production process.
基金supported by grants from the National Natural Science Foundation of China(52072099)Team program of the Natural Science Foundation of Heilongjiang Province,China(No.TD2021E005)Joint Guidance Project of the Natural Science Foundation of Heilongjiang Province,China(No.LH2022E093)。
文摘Electrocatalysts are an effective strategy to mitigate the shuttling effect of lithium polysulfides(LiPSs)and accelerate the redox kinetics of LiPSs in lithium-sulfur(Li-S)batteries.However,traditional electrocatalysts only have a single active site and often undergo structural collapse and aggregation during charging and discharging,resulting in reduced catalytic performance.Herein,the two-dimensional(2D)polar high-entropy La_(0.71)Sr_(0.29)Co_(0.21)Ni_(0.20)Fe_(0.19)Cr_(0.20)Cu_(0.20)O_(3)(LCO-HEO)nanosheets were rationally designed and successfully synthesized to address this issue.The distinct functional polar sites in LCOHEOs were formed by the d-d orbital hybridization between spatially coupling adjacent transition metals,which can strengthen the dipole-dipole interaction between polar LCO-HEOs and polar LiPSs.2D polar LCO-HEO nanosheets can efficiently capture and trigger the tandem catalysis of polar LiPSs during their sequential conversion.The S/LCO-HEO composite cathode exhibits a high specific capacity of 1161.1 mA h g^(-1)at 1.0 C,with an ultralow capacity attenuation rate of 0.036%per cycle over 1200 cycles,and achieves stable cycling for 1500 cycles even at 8.0 C.Furthermore,even with a high sulfur loading(5.5 mg cm^(-2))and a low electrolyte/sulfur(E/S)ratio(4.0μL mg^(-1)),the S/LCO-HEO composite cathode shows desirable sulfur utilization and good cycle stability.This work demonstrates the feasibility of high entropy-driven multiple distinct functional polar sites for high-rate and long-cycle Li-S batteries.
基金financial support from the National Natural Science Foundation of China(No.82003585)the Program for Science&Technology Innovation Talents in Universities of Henan Province(No.24HASTIT069)+5 种基金the Technical Innovation Team of Henan Normal University(No.2022TD03)the Special Project for Fundamental Research in University of Henan Province(No.23ZX009)the Henan Science and Technology Program(No.232102310364)the Key Project of Henan Educational Committee(No.22A150041)Excellent Youth Foundation of Henan Scientific Committee(No.222300420012)the Young Core Instructor Training Program of Xinyang Agriculture and Forestry University(2023)。
文摘A transition-metal-and oxidant-free amination/cyclization reaction to access 1,2,4-triazolo[1,5-a]pyridines was realized in water by using amino diphenylphosphinate as amino source.A broad array of readily accessible N-(pyridyl)amides could be converted into the products featuring a diverse set of functional groups.The sustainable methodology was successfully applied to the late-stage functionalization of natural products and drugs.
基金supported by the Key Reasearch and Development Program of Zhejiang(2022C01029)the National Natural Science Foundation of China(22225802 and 22288102)the Research Funds of Institute of Zhejiang University-Quzhou(IZQ2022KJ3005).
文摘The removal of cesium-137(^(137)Cs)from nuclear wastewater remains crucial due to its radioactivity and high solubility in water,which pose serious risk to human health and the environment.Aiming at selective capture of Cs^(+) from wastewater,a core-shell adsorbent,Prussian blue analog@y-alumina(PBA@Al_(2)O_(3))pellets were synthesized using the hydrothermal-stepwise deposition method.The coreshell PBA@Al_(2)O_(3)pellets showcased a PBA loading of 25%and demonstrated a maximum adsorption capacity of 15.65 mg·g^(-1).The adsorption data was consistent with the pseudo-second-order kinetic model and the Langmuir isotherm model.It effectively reduced bulk Cs^(+) concentrations from an initial 6.62 mg·L^(-1)to 2 μg·L^(-1),achieving a removal efficiency of 99.97%and distribution coefficient(Kd)of 1.265×10^(6)ml·g^(-1),surpassing the performance of other PBA-based materials.The material also indicated good mechanical properties and cesium ion removal rates of 99.7%across a wide pH range(1.82 to 11.12).Furthermore,PBA@Al_(2)O_(3)exhibited consistent removal rate of over 99%and good selectivity(SF=50-1600)towards Cs^(+) even in the presence of interfering ions such as Na^(+),K^(+),Mg^(2+),and Ca^(2+)ions.The Kd(Cs^(+))for PBA@Al2O3 in simulated seawater and groundwater were 9.92×10^(3)and 2.23×10^(4)ml·g^(-1),where the removal rates reached 96.1%and 98.2%,respectively.XPS confirms that the adsorption mechanism is the ion exchange between Cs^(+) and K^(+)ions.This study underscores the significant potential of inorganic core-shell pellets adsorbents as promising agents for the selective capture of Cs^(+) from wastewater.
基金Financial support from the National Natural Science Foundation of China(No.22171168)Excellent Youth Foundation of Henan Scientific Committee(No.222300420012)Taishan Scholar Program of Shandong Province is gratefully acknowledged。
文摘A wide range of isoquinoline ring-modified Quinap oxides with different steric and electronic variations have been constructed through a palladium-catalyzed imidoylative cyclization of arylethenyl isocyanides with 2-diphenylphosphinyl-1-naphthyl bromides.The Pd-catalysis plays dual roles in the formation of both axial C–C bond and isoquinoline ring.This de novo synthetic strategy features good functional group tolerance,high yields and easy scale-up,providing Quinap derivatives with substitution patterns that could not be obtained using coupling reactions.Chiral ligands 7 and 12 can be readily prepared by transformation of the resulting Quinap oxide to their BINOL esters,and have been proven to be superb chiral ligands for the copper-catalyzed enantioselective A^(3)-coupling and alkynylation of quinoline reactions.In general,the enantioselectivies obtained using ligands 7 and 12 are excellent,and the ee values are higher than those using Quinap as ligand,even three times higher in some cases.Mechanism studies revealed that a monomeric copper(Ⅰ)complex bearing a single chiral ligand was formed and served as the catalytically active species.
基金supported by the National Key Research and Development Program of China(2022YFB4200305)the National Natural Science Foundation of China(22379049)Hubei Provincial Key Research and Development Program(2023BAB113)。
文摘The lead-free inorganic perovskite CsSnI_(3) is considered as one of the best candidates for emerging photovoltaics.Nevertheless,CsSnI_(3)-based perovskite solar cells experience a significant drop in performance due to the nonradiative recombination facilitated by trapping.Here,we show an electron donor passivation method to regulate deep-level defects for CsSnI_(3) perovskite with electron donor pyrrole.Experimental observations combined with theoretical simulations verify that the saturation of Tin dangling bonds with pyrrole on the CsSnI_(3) surface via a Lewis acid-base addition reaction can significantly reduce the density of deep-level defects.Consequently,the printable mesoporous perovskite solar cells with an FTO/compact-TiO_(2)/mesoporous-TiO_(2)/Al_(2)O_(3)/NiO/carbon framework device structure penetrated with CsSnI_(3) achieve a power conversion efficiency of up to 10.11%.To our knowledge,this represents the highest efficiency reported to date for lead-free pero vs kite-based printable mesoporous solar cells.Furthermore,the unencapsulated devices demonstrated remarkable long-term stability,retaining 92%of their initial efficiency even after 2400 h of aging in a nitrogen atmosphere.
基金supported by the National Natural Science Foundation of China(Grant Nos.92166112,52373236 and 52271132)the Natural Science Foundation of Guangdong Province(Grant No.2024A1515010658)+6 种基金the Guangdong Province International Science and Technology Cooperation Project(Grant No.2023A0505050103)the Guangxi Key Laboratory of Information Materials(Grant No.231033-K)the Open Project Program of Wuhan National Laboratory for Optoelectronics(Grant No.2021WNLOKF010)Guangzhou Science and Technology Planning Project(2024A04J9966)Guangdong Provincial Science and Technology Plan Project(2022A0505050043)The financial support from the ECU industrial grant(No.G1006320)ECU DVC strategic research fund(project number 23965)。
文摘Ti-xNb alloys produced by laser powder bed fusion(LPBF)from mixed powder usually exhibit an inhomogeneous elemental distribution,leading to a deterioration in mechanical properties.To address this issue,we proposed a strategy to achieve heterostructure in laser powder bed fused Ti-xNb alloys from mixed powders through precipitation ofωwithinβ.Moreover,the effect of Nb content on the micro structure and mechanical behavior of Ti-xNb alloys was studied.The results indicated that in-situ laser re-melting can realize the homogeneous elemental distribution in Ti-xNb alloys.When the Nb content increases from 30 wt%,35 wt%to40 wt%,Ti-xNb alloys experience a transformation from β+α' to β+ω and monolithic β.Specifically,ωnano-precipitates in Ti-35Nb alloy are only distributed in some β grains,forming a heterostructure with“softβ”and“hard β+ω”grains.As a result,LPBF-produced Ti-35Nb alloy demonstrates excellent mechanical properties,with yield strength of ^(792±6)MPa,tensile strength of ^(806±7)MPa,Young's modulus of ^(68±6)GPa,and uniform elongation of ^(18.0±1.1)%.The Frank-Read mechanism induces dislocation proliferation and dislocation cross-slip,and the geometrically necessary dislocations(GNDs)are induced at the heterogeneous interface of“softβ”and“hard β+ω”grains,resulting in an enhancement in the strength-ductility synergy of Ti-35Nb alloy produced by LPBF.This work provides an innovative strategy to improve the strength-ductility synergy of LPBF-produced Ti-xNb alloys from mixed powders by tailoring ω nano-precipitates.
基金supported by the Ministry of Science and Technology of China STI2030-Major Projects(2022ZD0214100)the National Natural Science Foundation of China(32171056 and 82272114)+2 种基金the General Research Fund of Hong Kong Research Grants Council(17614922)the Shenzhen Soft Science Research Program Project(RKX20220705152815035)the Shenzhen-Hong Kong Institute of Brain Science-Shenzhen Fundamental Research Institutions(2023SHIBS0003).
文摘Dear Editor,People are often optimistic when forecasting the future,such that they believe they are less likely to encounter adverse life events.This phenomenon,known as optimism bias,emerges due to preferential encoding and consolidation of desirable over undesirable information[1,2],engaging frontal brain regions such as the anterior cingulate cortex and inferior frontal gyrus[1].An optimism bias is instrumental in supporting mental health:reduction or absence of optimism biases is associated with mood disorders such as depression,characterized by pessimistic thinking about the future[3].This relationship highlights the potential value of interventions that could enhance optimism bias[4].
基金Supported by the National Natural Science Foundation of China(21722609,21776240)Zhejiang Provincial Natural Science Foundation of China(LR17B060001)
文摘Metal–organic frameworks(MOFs) packed in the column have been a promising candidate as the stationary phase for high performance liquid chromatography(HPLC). However, the direct packing of irregular MOF powder could raise some problems like high back pressure and low column efficiency in the HPLC separation. In this work, UiO-66 capable of separating xylenes was supported effectively on the surface of the monodisperse spherical silica microspheres by one-pot method. The hybridization of Ui O-66 and silica microspheres(termed UiO-66@SiO2 shell–core composite) was prepared by stirring the suspension of the precursors of Ui O-66 and\\COOH terminated silica in the N,N-dimethylformamide with heating. The shell–core composite material UiO66@SiO2 was characterized by SEM, TEM, PXRD and FTIR. Then, it was used as a packing material for the chromatographic separation of xylene isomers. Xylene isomers including o-xylene, m-xylene and p-xylene were efficiently separated on the column with high resolution and good reproducibility. Moreover, the Ui O-66@SiO2 shell–core composites packed column still remained reverse shape selectivity as Ui O-66 possessed, and the retention of xylenes was probably ascribed to the hydrophobic effect between analytes and the aromatic rings of the Ui O-66 shell. The Ui O-66@SiO2 shell–core composites obtained in this study have some potential for the separation of structural isomers in HPLC.
基金We acknowledge the National Natural Science Foundation of China for supporting the project via the grant number 11472062 and 11002034.
文摘OSAHS(Obstructive Sleep Apnea Hypopnea Syndrome)is a respiratory disease mainly characterized by limited and repeated pauses of breathing in sleep.Currently,the optimal treatment is to apply CPAP(Continuous Positive Airway Pressure)ventilation on the upper airway of the patient through a household respiratory machine.However,if the ventilator mask is designed improperly,it might cause the residue and repeated inhalation of CO2,which will exert an adverse impact on the therapeutic effect.Present research numerically analyzed the CO2 transportation inside a commercial ventilator mask(Mirage SoftGel,ResMed,Australia)based on the reconstructed 3D numerical model of a volunteer's face and performed the improved design of the ventilator mask in terms of the CO2 residual concentration below the nostrils.The fluid dynamic analyses showed that at the end time of expiratory,the CO2 residual concentration below the nostrils is close to 4%.To improve the therapeutic effect,we changed the position of the exhaust holes and found that by moving the exhaust holes to the bottom of the ventilator mask,the CO2 residual concentration below the nostrils would be reduced to no more than 1%.This study established a near physiological computational model and provided a new method for the individualized design of the commercial ventilator mask.
基金The authors acknowledge funding from the National Natural Science Foundation of China(61974150 and 51773213)Key Research Program of Frontier Sciences,CAS(QYZDB-SSW-JSC047)+1 种基金the Fundamental Research Funds for the Central Universities,the CAS-EU S&T cooperation partner program(174433KYSB20150013)the Natural Science Foundation of Ningbo(2018A610135).
文摘Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through solution manufacturing.Herein,we report a solution-processed flexible OSC based on a transparent conducting PEDOT:PSS anode doped with trifluoromethanesulfonic acid(CF3SO3H).Through a low-concentration and low-temperature CF3SO3H doping,the conducting polymer anodes exhibited a main sheet resistance of 35Ωsq−1(minimum value:32Ωsq−1),a raised work function(≈5.0 eV),a superior wettability,and a high electrical stability.The high work function minimized the energy level mismatch among the anodes,hole-transporting layers and electron-donors of the active layers,thereby leading to an enhanced carrier extraction.The solution-processed flexible OSCs yielded a record-high efficiency of 16.41%(maximum value:16.61%).Besides,the flexible OSCs afforded the 1000 cyclic bending tests at the radius of 1.5 mm and the long-time thermal treatments at 85°C,demonstrating a high flexibility and a good thermal stability.
基金supported by the National Natural Science Foundation of China (51772069)。
文摘Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3 D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti_3 C_2 T_x flakes on sulfur-impregnated carbon cloth(Ti_3 C_2 T_x@S/CC) to achieve high loading and high energy density Li-S batteries,in which,the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer,while the outer-coated Ti_3 C_2 T_x can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode,achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion.Due to these advantages,at a sulfur loading of 4 mg cm^(-2),Li-S cells with Ti_3 C_2 T_x@S/CC cathodes can deliver outstanding cycling stability(746.1 mAh g^(-1) after 200 cycles at1 C),superb rate performance(866.8 mAh g^(-1) up to 2 C) and a high specific energy density(564.2 Wh kg^(-1) after 100 cycles at 0.5 C).More significantly,they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm^(-2) at the increased loading of 8 mg cm^(-2).
基金supported by the Grant-in-Aid for Scientific Research (KAKENHI) program, Japan (C, Grant Number 15K05597)Takahashi Industrial and Economic Research Foundation (Takahashi Grant Number 06-003-154)
文摘Electrode material based on a novel core–shell structure consisting of NiCoS（NCS） solid fiber core and Mn S（MS） sheet shell（NCS@MS） in situ grown on carbon cloth（CC） has been successfully prepared by a simple sulfurization-assisted hydrothermal method for high performance supercapacitor. The synthesized NiCoS@Mn S/CC electrode shows high capacitance of 1908.3 F gat a current density of 0.5 A gwhich is higher than those of NiCoSand Mn S at the same current density. A flexible all-solid-state asymmetric supercapacitor（ASC） is constructed by using NiCoS@Mn S/CC as positive electrode, active carbon/CC as negative electrode and KOH/poly（vinyl alcohol）(PVA) as electrolyte. The optimized ASC shows a maximum energy density of 23.3 Wh kgat 1 A g, a maximum power density of about7.5 kw kgat 10 A gand remarkable cycling stability. After 9000 cycles, the ASC still exhibited67.8% retention rate and largely unchanged charge/discharge curves. The excellent electrochemical properties are resulted from the novel core–shell structure of the NiCoS@Mn S/CC electrode, which possesses both high surface area for Faraday redox reaction and superior kinetics of charge transport. The NiCoS@Mn S/CC electrode shows a promising potential for energy storage applications in the future.
基金supported by the natural science foundation of Shandong province ZR2017BH053the youth doctor cooperation foundation of Qilu University of Technology(Shandong Academy of Sciences)2017BSH2017。
文摘Rosa rugosa Thunb.is recognized as both medicine and edible in China.The article investigated the antitumor activity of rose flavonoids.Water-extracted rose flavonoids(RFW)and ethanol-extracted rose flavonoids(RFE)were achieved by extracting with distilled water and 70%ethanol,respectively.The effects of the two extracts on proliferation inhibition,apoptosis inducement and metastasis prevention of human HepG2 hepatocellular carcinoma cell lines were tested,via optical/fluorescence microscopy,MTT detection,Transwell assay,flow cytometry and Western blot,etc.The results indicated that rose flavonoids at low concentration(10-40μg/mL)had a better inhibitory effect on migration and invasion of HepG2 cells in a dose-dependent manner,while rose flavonoids at high concentration(80-160μg/mL)could induce apoptosis of HepG2 cells by up-regulating the expression of pro-apoptotic proteins p53 and Bax,and down-regulating the expression of anti-apoptotic proteins Bcl-2,leading to the functioning of caspase-3 and caspase-9.The effect of RFE at the same concentration was significantly better than that of RFW.Conclusion,this study found that rose flavonoids had a certain inhibitory effect on proliferation and metastasis of human liver cancer cells HepG2,indicating the application of rose flavonoids in preventing and treating of liver cancer.
基金Project supported by the National Science Foundation of China (No.51772070 and 51772069)。
文摘MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their practical application in lithium-ion batteries.In this work,a robust strategy is developed to control the functional groups of Nb_2 CT_x MXene.The capacity of pristine Nb_2 CT_x MXene can be significantly increased by Li~+ intercalation and surface modification.The specific capacity of the treated Nb_2 CT_x is up to 448 mAh g^(-1) at 0.05 A g^(-1),and at a large current density of 2 A g^(-1) remains a high reversible capacity retention rate of 75% after an ultra-long cycle of 2000 cycles.These values exceed most of the reported pristine MXenes(including the most studied Ti_3 C_2 T_x) and carbon-based materials.It demonstrates that this strategy has great help to improve the electrochemical performance of pristine MXene,and the results enhance the promise of MXenes in the application of lithium-ion batteries.
