Rechargeable magnesium(Mg)-metal batteries have brought great expect to overcome the safety and energy density concerns of typical lithium-ion batteries.However,interracial passivation of the Mgmetal anode impairs the...Rechargeable magnesium(Mg)-metal batteries have brought great expect to overcome the safety and energy density concerns of typical lithium-ion batteries.However,interracial passivation of the Mgmetal anode impairs the reversible Mg plating/stripping chemistries,resulting in low Coulombic efficiency and large overpotential.In this work,a facile isobutylamine(IBA)-assisted activation strategy has been proposed and the fundamental mechanism has been unveiled in a specific way of evolving active species and forming MgH_(2)-based solid-electrolyte interphase.After introducing IBA into a typical electrolyte of magnesium bis(trifluoromethanesulfo nyl) imide(Mg(TFSI)_(2)) in diglyme(G2) solvents,electrolyte species of [Mg^(2+)(IBA)5]^(2+) and protonated amine-based cations of [(IBA)H]^(+) have been detected by nuclear magnetic resonance and mass spectra.This not only indicates direct solvation of IBA toward Mg^(2+)but also suggests its ionization,which is central to mitigating the decomposition of G2 and TFSI anions by forming neutrally charged [(IBAH^(+))(TFSI^(-))]~0 and other complex ions.A series of experiments,including cryogenic-electron microscopy,D_(2)O titration-mass spectra,and time of flight secondary ion mass spectrometry results,reveal a thin,non-passivated,and MgH_(2)-containing interphase on the Mg-metal anode.Besides,uniform and dendrite-free Mg electrodeposits have been revealed in composite electrolytes.Benefiting from the activation effects of IBA,the composite electrolyte displays superior electrochemical performance(overpotential is approximately 0.16 V versus 2.00 V for conventional electrolyte;Coulombic efficiency is above 90% versus <10% for conventional electrolyte).This work offers a fresh direction to advanced electrolyte design for next-generation rechargeable batteries.展开更多
The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reve...The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of electrodeposits.In this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths.As revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of scaffolds.The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed.As a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best knowledge.Besides,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous results.This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.展开更多
The aim was to optimize ultrasonic extraction conditions and study antioxidant activities of lychee pericarp polysaccharides. The effects of extraction temperature,time,ultrasonic power,solid-liquid ratio on polysacch...The aim was to optimize ultrasonic extraction conditions and study antioxidant activities of lychee pericarp polysaccharides. The effects of extraction temperature,time,ultrasonic power,solid-liquid ratio on polysaccharides yield were investigated by single-factor experiment and orthogonal experiment to obtain optimum extraction conditions; the antioxidant activities of lychee pericarp polysaccharides were evaluated by the total antioxidant activity. Optimum extraction process was under extraction temperature of 80 ℃,extraction time of 2. 5 h,ultrasonic power of 180 W,solid-liquid ratio of 1∶ 25 g / m L; the total antioxidant activity was increased with the increasing concentration of polysaccharides. The extraction process is simple and efficient. The extraction rate of lychee pericarp polysaccharides with antioxidant activities is high.展开更多
Antitumor therapies based on adoptively transferred T cells or oncolytic viruses have made significant progress in recent years,but the limited efficiency of their infiltration into solid tumors makes it difficult to ...Antitumor therapies based on adoptively transferred T cells or oncolytic viruses have made significant progress in recent years,but the limited efficiency of their infiltration into solid tumors makes it difficult to achieve desired antitumor effects when used alone.In this study,an oncolytic virus(rVSV-LCMVG)that is not prone to induce virus-neutralizing antibodies was designed and combined with adoptively transferred T cells.By transforming the immunosuppressive tumor microenvironment into an immunosensitive one,in B16 tumor-bearing mice,combination therapy showed superior antitumor effects than monotherapy.This occurred whether the OV was administered intratumorally or intravenously.Combination therapy significantly increased cytokine and chemokine levels within tumors and recruited CD8^(+)T cells to the TME to trigger antitumor immune responses.Pretreatment with adoptively transferred T cells and subsequent oncolytic virotherapy sensitizes refractory tumors by boosting T-cell recruitment,downregulating the expression of PD-1,and restoring effector T-cell function.To offer a combination therapy with greater translational value,mRNA vaccines were introduced to induce tumor-specific T cells instead of adoptively transferred T cells.The combination of OVs and mRNA vaccine also displays a significant reduction in tumor burden and prolonged survival.This study proposed a rational combination therapy of OVs with adoptive T-cell transfer or mRNA vaccines encoding tumor-associated antigens,in terms of synergistic efficacy and mechanism.展开更多
Accurate origin–destination(OD)demand prediction is crucial for the efficient operation and management of urban rail transit(URT)systems,particularly during a pandemic.However,this task faces several limitations,incl...Accurate origin–destination(OD)demand prediction is crucial for the efficient operation and management of urban rail transit(URT)systems,particularly during a pandemic.However,this task faces several limitations,including real-time availability,sparsity,and high-dimensionality issues,and the impact of the pandemic.Consequently,this study proposes a unified framework called the physics-guided adaptive graph spatial–temporal attention network(PAG-STAN)for metro OD demand prediction under pandemic conditions.Specifically,PAG-STAN introduces a real-time OD estimation module to estimate real-time complete OD demand matrices.Subsequently,a novel dynamic OD demand matrix compression module is proposed to generate dense real-time OD demand matrices.Thereafter,PAG-STAN leverages various heterogeneous data to learn the evolutionary trend of future OD ridership during the pandemic.Finally,a masked physics-guided loss function(MPG-loss function)incorporates the physical quantity information between the OD demand and inbound flow into the loss function to enhance model interpretability.PAG-STAN demonstrated favorable performance on two real-world metro OD demand datasets under the pandemic and conventional scenarios,highlighting its robustness and sensitivity for metro OD demand prediction.A series of ablation studies were conducted to verify the indispensability of each module in PAG-STAN.展开更多
Magnet-optical materials embracing coupled magnetic and photoluminescent properties in single phase are promising in microelectronics and optoelectronic devices.However,the current research mainly focuses on tradition...Magnet-optical materials embracing coupled magnetic and photoluminescent properties in single phase are promising in microelectronics and optoelectronic devices.However,the current research mainly focuses on traditional inorganic materials,and there are few reports on molecule materials.Recently,we synthesized an organic–inorganic hybrid complex((C_(6)H_(5)C_(2)H_(3)FNH_(3))_(2)MnCl_(4)(1)with perovskite structure.Physical measurements show that 1 not only behaves as an antiferromagnet with spin canting but also exhibits unusual fluorescent properties.Importantly,under the magnetic field at different temperatures,the luminous intensity of 1 changed,and a red-shift occurred with obviously optical hysteresis.These phenomena directly prove the existence of magneto-optical coupling in 1.More interestingly,the optical hysteresis can be observed in both low and high field,which is unprecedented in other molecular materials.Even in traditional inorganic materials,it can only be observed in strong field.This special function provides the possibility for the application of low energy consumption optoelectronic devices.展开更多
基金National Natural Science Foundation of China (22279068, 51972187)Natural Science Foundation of Shandong Province (ZR2021QE166)Qingdao New Energy Shandong Laboratory Open Project (QNESL OP202312)。
文摘Rechargeable magnesium(Mg)-metal batteries have brought great expect to overcome the safety and energy density concerns of typical lithium-ion batteries.However,interracial passivation of the Mgmetal anode impairs the reversible Mg plating/stripping chemistries,resulting in low Coulombic efficiency and large overpotential.In this work,a facile isobutylamine(IBA)-assisted activation strategy has been proposed and the fundamental mechanism has been unveiled in a specific way of evolving active species and forming MgH_(2)-based solid-electrolyte interphase.After introducing IBA into a typical electrolyte of magnesium bis(trifluoromethanesulfo nyl) imide(Mg(TFSI)_(2)) in diglyme(G2) solvents,electrolyte species of [Mg^(2+)(IBA)5]^(2+) and protonated amine-based cations of [(IBA)H]^(+) have been detected by nuclear magnetic resonance and mass spectra.This not only indicates direct solvation of IBA toward Mg^(2+)but also suggests its ionization,which is central to mitigating the decomposition of G2 and TFSI anions by forming neutrally charged [(IBAH^(+))(TFSI^(-))]~0 and other complex ions.A series of experiments,including cryogenic-electron microscopy,D_(2)O titration-mass spectra,and time of flight secondary ion mass spectrometry results,reveal a thin,non-passivated,and MgH_(2)-containing interphase on the Mg-metal anode.Besides,uniform and dendrite-free Mg electrodeposits have been revealed in composite electrolytes.Benefiting from the activation effects of IBA,the composite electrolyte displays superior electrochemical performance(overpotential is approximately 0.16 V versus 2.00 V for conventional electrolyte;Coulombic efficiency is above 90% versus <10% for conventional electrolyte).This work offers a fresh direction to advanced electrolyte design for next-generation rechargeable batteries.
基金supported by the National Natural Science Foundation of China(51972187,22279068,52374306)the Natural Science Foundation of Shandong Province(ZR2021QE166)Qingdao New Energy Shandong Laboratory Open Project(QNESL OP202312)。
文摘The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of electrodeposits.In this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths.As revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of scaffolds.The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed.As a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best knowledge.Besides,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous results.This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.
基金Supported by Superior and Characteristic Specialty Construction Project of Guangxi’s Colleges and Universities(201452)
文摘The aim was to optimize ultrasonic extraction conditions and study antioxidant activities of lychee pericarp polysaccharides. The effects of extraction temperature,time,ultrasonic power,solid-liquid ratio on polysaccharides yield were investigated by single-factor experiment and orthogonal experiment to obtain optimum extraction conditions; the antioxidant activities of lychee pericarp polysaccharides were evaluated by the total antioxidant activity. Optimum extraction process was under extraction temperature of 80 ℃,extraction time of 2. 5 h,ultrasonic power of 180 W,solid-liquid ratio of 1∶ 25 g / m L; the total antioxidant activity was increased with the increasing concentration of polysaccharides. The extraction process is simple and efficient. The extraction rate of lychee pericarp polysaccharides with antioxidant activities is high.
基金supported by National Natural Science Foundation of China grants 82322027(to T.Z.),82341043(to T.Z.),32170943(to T.Z.),81991491(to N.X.),32300744(to H.X.)Fundamental Research Funds for the Central Universities 20720220003(to N.X.)。
文摘Antitumor therapies based on adoptively transferred T cells or oncolytic viruses have made significant progress in recent years,but the limited efficiency of their infiltration into solid tumors makes it difficult to achieve desired antitumor effects when used alone.In this study,an oncolytic virus(rVSV-LCMVG)that is not prone to induce virus-neutralizing antibodies was designed and combined with adoptively transferred T cells.By transforming the immunosuppressive tumor microenvironment into an immunosensitive one,in B16 tumor-bearing mice,combination therapy showed superior antitumor effects than monotherapy.This occurred whether the OV was administered intratumorally or intravenously.Combination therapy significantly increased cytokine and chemokine levels within tumors and recruited CD8^(+)T cells to the TME to trigger antitumor immune responses.Pretreatment with adoptively transferred T cells and subsequent oncolytic virotherapy sensitizes refractory tumors by boosting T-cell recruitment,downregulating the expression of PD-1,and restoring effector T-cell function.To offer a combination therapy with greater translational value,mRNA vaccines were introduced to induce tumor-specific T cells instead of adoptively transferred T cells.The combination of OVs and mRNA vaccine also displays a significant reduction in tumor burden and prolonged survival.This study proposed a rational combination therapy of OVs with adoptive T-cell transfer or mRNA vaccines encoding tumor-associated antigens,in terms of synergistic efficacy and mechanism.
基金supported by the National Natural Science Foundation of China(72288101,72201029,and 72322022).
文摘Accurate origin–destination(OD)demand prediction is crucial for the efficient operation and management of urban rail transit(URT)systems,particularly during a pandemic.However,this task faces several limitations,including real-time availability,sparsity,and high-dimensionality issues,and the impact of the pandemic.Consequently,this study proposes a unified framework called the physics-guided adaptive graph spatial–temporal attention network(PAG-STAN)for metro OD demand prediction under pandemic conditions.Specifically,PAG-STAN introduces a real-time OD estimation module to estimate real-time complete OD demand matrices.Subsequently,a novel dynamic OD demand matrix compression module is proposed to generate dense real-time OD demand matrices.Thereafter,PAG-STAN leverages various heterogeneous data to learn the evolutionary trend of future OD ridership during the pandemic.Finally,a masked physics-guided loss function(MPG-loss function)incorporates the physical quantity information between the OD demand and inbound flow into the loss function to enhance model interpretability.PAG-STAN demonstrated favorable performance on two real-world metro OD demand datasets under the pandemic and conventional scenarios,highlighting its robustness and sensitivity for metro OD demand prediction.A series of ablation studies were conducted to verify the indispensability of each module in PAG-STAN.
基金National Key Research and Development Program of China,Grant/Award Numbers:2018YFA0306004,2017YFA0204800National Natural Science Foundation of China,Grant/Award Numbers:21973038,21805119,12064002,21875093,22105089,61904119,11974126+4 种基金The Joint Fund for Regional Innovation and Development,Grant/Award Number:U20A2073Natural Science Foundation of Jiangxi Province,Grant/Award Numbers:20204BCJ22015,20202ACBL203001Natural Science Foundation of the Jiangsu Higher Education Institutions of China(,Grant/Award Number:20KJB140019)Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry,Grant/Award Number:20212BCD42018Interdisciplinary program of Wuhan National High Magnetic Field Center,Grant/Award Number:WHMFC202133。
文摘Magnet-optical materials embracing coupled magnetic and photoluminescent properties in single phase are promising in microelectronics and optoelectronic devices.However,the current research mainly focuses on traditional inorganic materials,and there are few reports on molecule materials.Recently,we synthesized an organic–inorganic hybrid complex((C_(6)H_(5)C_(2)H_(3)FNH_(3))_(2)MnCl_(4)(1)with perovskite structure.Physical measurements show that 1 not only behaves as an antiferromagnet with spin canting but also exhibits unusual fluorescent properties.Importantly,under the magnetic field at different temperatures,the luminous intensity of 1 changed,and a red-shift occurred with obviously optical hysteresis.These phenomena directly prove the existence of magneto-optical coupling in 1.More interestingly,the optical hysteresis can be observed in both low and high field,which is unprecedented in other molecular materials.Even in traditional inorganic materials,it can only be observed in strong field.This special function provides the possibility for the application of low energy consumption optoelectronic devices.
