Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electro...Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electrocatalytic oxidations of saturated alcohols(C_(1)-C_(6))to selectively form formate using Ni Co hydroxide(Ni Co-OH)derived Ni Co_(2)O_(4)solid-acid electrocatalysts with balanced Lewis acid(LASs)and Brønsted acid sites(BASs).Thermal treatment transforms BASs-rich(89.6%)Ni Co-OH into Ni Co_(2)O_(4)with nearly equal distribution of LASs(53.1%)and BASs(46.9%)which synergistically promote adsorption and activation of OH-and alcohol molecules for enhanced oxidation activity.In contrast,BASs-enriched Ni Co-OH facilitates formation of higher valence metal sites,beneficial for water oxidation.The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6alcohols increases as increased number of hydroxyl groups and decreased HOMO-LUMO gaps:methanol(C_(1))<ethylene glycol(C_(2))<glycerol(C3)<meso-erythritol(C4)<xylitol(C5)<sorbitol(C6),while the formate selectivity shows the opposite trend from 100 to 80%.This study unveils synergistic roles of LASs and BASs,as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.展开更多
In this study,we investigate the ef-ficacy of a hybrid parallel algo-rithm aiming at enhancing the speed of evaluation of two-electron repulsion integrals(ERI)and Fock matrix generation on the Hygon C86/DCU(deep compu...In this study,we investigate the ef-ficacy of a hybrid parallel algo-rithm aiming at enhancing the speed of evaluation of two-electron repulsion integrals(ERI)and Fock matrix generation on the Hygon C86/DCU(deep computing unit)heterogeneous computing platform.Multiple hybrid parallel schemes are assessed using a range of model systems,including those with up to 1200 atoms and 10000 basis func-tions.The findings of our research reveal that,during Hartree-Fock(HF)calculations,a single DCU ex-hibits 33.6 speedups over 32 C86 CPU cores.Compared with the efficiency of Wuhan Electronic Structure Package on Intel X86 and NVIDIA A100 computing platform,the Hygon platform exhibits good cost-effective-ness,showing great potential in quantum chemistry calculation and other high-performance scientific computations.展开更多
Linear mRNA vaccines are constrained by exonuclease susceptibility and instability,leading to compromised antigen expression.Circular RNA(circRNA) lacking canonical 5' and 3' untranslated regions demonstrates ...Linear mRNA vaccines are constrained by exonuclease susceptibility and instability,leading to compromised antigen expression.Circular RNA(circRNA) lacking canonical 5' and 3' untranslated regions demonstrates intrinsic exonuclease resistance.Current circularization strategies face three principal limitations:chemical methods produce non-native 2',5'-phosphodiester bonds;ribozyme-mediated approaches are restricted to RNA fragments shorter than 500 nucleotides;the Anabaena Group I intron system retains immunogenic exon sequences.In contrast,the self-splicing Group I intron ribozyme from Tetrahymena enables precisely controlled circularization through autonomous structural rearrangement,yielding exonfree constructs.Through optimized purification protocols,historical scalability challenges are systematically addressed.This Perspective establishes the mechanistic rationale and therapeutic superiority of this engineered RNA circularization platform.展开更多
The lithium battery is an essential component of electric cars;prompt and accurate problem detection is vital in guaranteeing electric cars’safe and dependable functioning and addressing the limitations of Back Propa...The lithium battery is an essential component of electric cars;prompt and accurate problem detection is vital in guaranteeing electric cars’safe and dependable functioning and addressing the limitations of Back Propagation(BP)neural networks in terms of vanishing gradients and inability to effectively capture dependencies in time series,and the limitations of Long-Short Term Memory(LSTM)neural network models in terms of risk of overfitting.A method based on LSTM-BP is put forward for power battery fault diagnosis to improve the accuracy of lithium battery fault diagnosis.First,a lithium battery model is constructed based on the second-order RC equivalent circuit and the electro-thermal coupling model,and various lithium battery failures are simulated to examine the fault characteristics.Then,the lithium battery charging and discharging experiments collect,clean,and process the battery data.By constructing a neural network LSTM-BP model,we verified the superiority and accuracy of the LSTM-BP neural network model by comparing the LSTM model and BP model vertically and by comparing the Recurrent Neural Network(RNN)model,the Gated Recurrent Unit(GRU)model,and the Residual Neural Network(ResNet)model of a more advanced architecture horizontally.Finally,the lithium battery fault diagnosis process is summarized through the threshold quantitative criteria,and different faults are diagnosed and analyzed.Theresults show that the LSTM-BP neural network not only overcomes the limitations of the LSTMneural network and BP neural network but also improves the ability to process sequence data and reduces the risk of overfitting.展开更多
Dengue virus(DENV)is a mosquito-borne pathogen responsible for a spectrum of illnesses,including dengue fever,dengue hemorrhagic fever,and dengue shock syndrome.Nearly half of the global population is at risk of DENV ...Dengue virus(DENV)is a mosquito-borne pathogen responsible for a spectrum of illnesses,including dengue fever,dengue hemorrhagic fever,and dengue shock syndrome.Nearly half of the global population is at risk of DENV infection,making it a pressing public health issue worldwide.The limited cross-protection among the four DENV serotypes(DENV1-4)and the phenomenon of antibody-dependent enhancement(ADE)have posed significant challenges to the development of effective dengue vaccines.Furthermore,there are currently no specific antiviral treatments available.This review provides an overview of DENV's key characteristics,clinical manifestations,and recent advancements in antiviral drug development-including the repurposing of approved drugs,peptidebased antiviral agents,therapeutic antibodies,natural products with antiviral potential,and host factor inhibitors-aiming to offer critical insights to inform strategies for managing and preventing dengue outbreaks.展开更多
OBJECTIVE： To investigate the effects of Zhuyesh- igao granule （ZSG） on tumor necrosis factor-a （TNF-a）, interleukin-1 （IL-1）, IL-2, IL-6, and IL-8 in rats with radiation esophagitis. METHODS： Fifty Wistar rat...OBJECTIVE： To investigate the effects of Zhuyesh- igao granule （ZSG） on tumor necrosis factor-a （TNF-a）, interleukin-1 （IL-1）, IL-2, IL-6, and IL-8 in rats with radiation esophagitis. METHODS： Fifty Wistar rats were randomly divid- ed into five groups （10 rats in each group）： con- trol （without radiation）, saline-treated, and low, medium, and high-dose ISG-treated groups. Rats were given normal saline （10 mL/kg） or 1.15, 2.3, or 4.6 g/kg ZSG by intragastric administration once a day for 7 days. A rat model of radiation esophagi- tis was established by local irradiation of Co60 （490.25 cGy/min, totaling 30 Gy）. The administra- tion of ZSG was continued for another 7 days and on the 7th day post-irradiation, inferior vena cavablood was collected. The serum was separated, and TNF-a, IL-1, IL-2, 11_-6, and IL-8 protein levels were determined. RESULTS： Inflammatory response factors were found in the serum of each group. However, levels in ZSG-treated groups were significantly lower than in the saline-treated group （P〈0.05）. CONCLUSION： ZSG may prevent the development of radiation esophagitis, perhaps by inhibiting the generation and release of the inflammatory re- sponse factors TNF-a, IL-1, IL-2, IL-6, and IL-8.展开更多
An electrochemical sensor for doxycycline hyclate(DC)detection with high sensitivity and good selectivity is reported.The sensor was fabricated by electro-polymerization of molecularly imprinted polymers(MIPs)in the p...An electrochemical sensor for doxycycline hyclate(DC)detection with high sensitivity and good selectivity is reported.The sensor was fabricated by electro-polymerization of molecularly imprinted polymers(MIPs)in the presence of DC onto multi-walled carbon nanotubes modified glassy carbon electrode(MWCNTs/GCE).The MWCNTs can significantly increase the current response of the sensor,leading to enhanced sensitivity.The MIPs provide selective recognition sites for DC detection.The experimental parameters,such as the polymer monomer concentration,supporting electrolyte pH,the time for electro-polymerization and the incubation time of the sensor with DC were optimized.Under optimized experimental conditions,the sensor displayed a linear range of 0.05μmol/L-0.5μmol/L towards DC detection,with the detection limit of 1.3×10^-2μmol/L.The sensor was successfully applied for recovery test of DC in human serum samples.展开更多
As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an...As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an attractive route for generating efficient electrocatalysts with high mass transport capabilities.Herein,we report an efficient hard templating pathway to design and synthesize three-dimensional(3-D)mesoporous ternary nickel iron nitride(Ni3FeN).The as-synthesized electrocatalyst shows good OER performance in an alkaline solution with low overpotential(259 mV)and a small Tafel slope(54 mV dec?1),giving superior performance to IrO2 and RuO2 catalysts.The highly active contact area,the hierarchical porosity,and the synergistic effect of bimetal atoms contributed to the improved electrocatalytic performance toward OER.In a practical rechargeable Zn–air battery,mesoporous Ni3FeN is also shown to deliver a lower charging voltage and longer lifetime than RuO2.This work opens up a new promising approach to synthesize active OER electrocatalysts for energy-related devices.展开更多
Nitrogen-doped carbon materials with a large specific surface area,high conductivity,and adjustable microstructures have many prospects for energy-related applications.This is especially true for N-doped nanocarbons u...Nitrogen-doped carbon materials with a large specific surface area,high conductivity,and adjustable microstructures have many prospects for energy-related applications.This is especially true for N-doped nanocarbons used in the electrocatalytic oxygen reduction reaction(ORR)and supercapacitors.Here,we report a low-cost,environmentally friendly,large-scale mechanochemical method of preparing N-doped porous carbons(NPCs)with hierarchical micro-mesopores and a large surface area via ball-milling polymerization followed by pyrolysis.The optimized NPC prepared at 1000°C(NPC-1000)offers excellent ORR activity with an onset potential(Eonset)and half-wave potential(E1/2)of 0.9 and 0.82 V,respectively(vs.a reversible hydrogen electrode),which are only approximately 30 mV lower than that of Pt/C.The rechargeable Zn–air battery assembled using NPC-1000 and the NiFe-layered double hydroxide as bifunctional ORR and oxygen evolution reaction electrodes offered superior cycling stability and comparable discharge performance to RuO2 and Pt/C.Moreover,the supercapacitor electrode equipped with NPC prepared at 800℃ exhibited a high specific capacity(431 F g^−1 at 10 mV s^−1),outstanding rate,performance,and excellent cycling stability in an aqueous 6-M KOH solution.This work demonstrates the potential of the mechanochemical preparation method of porous carbons,which are important for energy conversion and storage.展开更多
Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline.However,the additional utilization of ...Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline.However,the additional utilization of a reductant and/or the operation at the elevating temperature causes the over-growth and agglomeration of Pt clusters,thus losing the high catalytic performance.Herein,we report that V dopant not only favors self-reducing Pt clusters on Ni Fe layered double hydroxide(LDH)(Pt/NiFeV)at room temperature,but also regulates interfacial charge redistribution to enhance the water-splitting performance.Experimental and theoretical studies reveal that V dopant into Ni Fe LDH triggers more electrons to transfer to adjacent Fe atoms,thus leading to a higher reducing ability compared to that without V-doping.When used as water-splitting electrocatalyst,V doping promotes electron loss of Pt clusters in Pt/Ni Fe V,optimizing the free energy of hydrogen adsorption and proton recombination kinetics at the cathode.Meanwhile,it also moves the d-band center of Ni away from the Fermi level to optimize the adsorption of*OH intermediates and facilitate the desorption of oxygen molecules at the anode.Thereby,Pt/Ni Fe V exhibits much higher bifunctional performance than V-free Pt/Ni Fe LDH toward both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).This work can spark inspiration of designing other bifunctional electrocatalysts for energy conversion and storage.展开更多
Background： Resveratrol, an important phyto-antioxidant commonly found in grapes, mulberry, and other plants,has a variety of functions including anti-aging, anti-cancer and anti-inflammatory activities. In the curre...Background： Resveratrol, an important phyto-antioxidant commonly found in grapes, mulberry, and other plants,has a variety of functions including anti-aging, anti-cancer and anti-inflammatory activities. In the current study, we investigated the beneficial effects of resveratrol on in vitro porcine oocyte maturation under heat stress（HS）. The effect of resveratrol, melatonin and their combination on alleviating HS was compared according to the maturation rate of oocytes and the development competence of embryos after parthenogenetic activation（PA）.Results： Supplementation with resveratrol（2.0 μmol/L） not only improved the nuclear maturation but also raised the blastocyst rate of porcine embryos＇ PA from oocytes that underwent HS by increasing their glutathione（GSH）level, reducing reactive oxygen species（ROS） and up-regulating the expression of Sirtuin 1（SIRT1）. It was also found that melatonin（10^-7mol/L） and the combination of resveratrol（2.0 μmol/L） plus melatonin（10^-7mol/L） exhibited more potent effects than resveratrol alone regarding their protective activities on oocyte maturation under HS.Conclusions： This study compared the efficiencies of resveratrol, melatonin and their combination for protecting porcine oocytes from heat stress. The mechanisms are attributed to the fact that each treatment may have different ability to regulate the synthesis of steroid hormones and the expression of mature related genes.展开更多
This article describes a fast and simple electrochemical assay for detecting cell concentration.After cell death,the membrane of cells will be broken,and DNA molecules contained in the cells will be released,but this ...This article describes a fast and simple electrochemical assay for detecting cell concentration.After cell death,the membrane of cells will be broken,and DNA molecules contained in the cells will be released,but this does not happen in living cells.Sodium molybdate can react with the phosphate backbone of the released DNA molecules to form phosphomolybdate precipitation and produces a corresponding redox current.The higher the concentration of DNA,the stronger the intensity of the current generated.Sodium molybdate solution and centrifuged cell supernatant were added onto the glassy carbon electrode to determine the cell concentration by measuring the current intensity.The cell viability,which means the ratio of living cells to the total cells,can also be determined by this method.This assay has the advantages of high sensitivity,low detection limit,and wide detection range.In addition,this method was successfully applied to the detection of cell concentration in human serum,which has potential clinical applications.展开更多
Nowadays,smart wearable devices are used widely in the Social Internet of Things(IoT),which record human physiological data in real time.To protect the data privacy of smart devices,researchers pay more attention to f...Nowadays,smart wearable devices are used widely in the Social Internet of Things(IoT),which record human physiological data in real time.To protect the data privacy of smart devices,researchers pay more attention to federated learning.Although the data leakage problem is somewhat solved,a new challenge has emerged.Asynchronous federated learning shortens the convergence time,while it has time delay and data heterogeneity problems.Both of the two problems harm the accuracy.To overcome these issues,we propose an asynchronous federated learning scheme based on double compensation to solve the problem of time delay and data heterogeneity problems.The scheme improves the Delay Compensated Asynchronous Stochastic Gradient Descent(DC-ASGD)algorithm based on the second-order Taylor expansion as the delay compensation.It adds the FedProx operator to the objective function as the heterogeneity compensation.Besides,the proposed scheme motivates the federated learning process by adjusting the importance of the participants and the central server.We conduct multiple sets of experiments in both conventional and heterogeneous scenarios.The experimental results show that our scheme improves the accuracy by about 5%while keeping the complexity constant.We can find that our scheme converges more smoothly during training and adapts better in heterogeneous environments through numerical experiments.The proposed double-compensation-based federated learning scheme is highly accurate,flexible in terms of participants and smooth the training process.Hence it is deemed suitable for data privacy protection of smart wearable devices.展开更多
CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operati...CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operation or storage,resulting in decreased catalytic performance.Herein,we report a efficient and stable BiIn@Cu-foam electrode through the in-situ regeneration of Bi^(0) active sites to renew the surface activation.The electronic structure of Bi site can be regulated by introducing In,thereby enhancing the adsorption strength of*OCHO.The optimized electrode exhibits over 90%FE_(formate)at a wide potential window(-0.9–-2.2 V),and formation rate for 3.15 mM cm^(-1)h^(-1).Especially,the electrode can maintain the high performance at continuously electrolysis for more than 300 h,or for more than 50 cycles,even repeated operation and storage for more than 2 years.This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.展开更多
Graphene nanosheets are widely used in anti-corrosion polymeric coating as filler,owing to the excellent electrochemical inertness and barrier property.However,as the arrangement of graphene nanosheets is difficult to...Graphene nanosheets are widely used in anti-corrosion polymeric coating as filler,owing to the excellent electrochemical inertness and barrier property.However,as the arrangement of graphene nanosheets is difficult to form a perfect layered structure,polymeric coating with graphene nanosheets usually needs micron-scale thickness to ensure the enhancement of corrosion protection.In this work,layer-by-layer stacked graphene nanocoatings were fabricated on stainless steel by self-assembly based on Marangoni effect.The anti-corrosion property of graphene coatings were studied through Tafel polarization curves,electrochemical impedance spectroscopy and accelerated corrosion test with extra applied voltage.The self corrosion current density of optimized three-layered graphene coated sample was one quarter of that of bare stainless steel.And the self corrosion potential of optimized sample is increased to-0.045 V.According to the results,graphene nanocoatings composed of layered nanosheets exhibits good anticorrosion property.Besides,the self-assembly method provide a promising approach to make layeredstructure coating for other researches about 2 D material nanosheets.展开更多
As a promising imaging technology,the low sensitivity of fluorine-19 magnetic resonance imaging(^(19)F MRI)severely hinders its biomedical applications.Herein,we have developed an unprecedented rotaxanebased strategy ...As a promising imaging technology,the low sensitivity of fluorine-19 magnetic resonance imaging(^(19)F MRI)severely hinders its biomedical applications.Herein,we have developed an unprecedented rotaxanebased strategy to improve the sensitivity of^(19)F MRI agents.By threading the fluorinated macrocycle into2-blade pinwheel[2]rotaxanes,the^(19)F longitudinal relaxation rate R1was dramatically increased,resulting in a significant^(19)F MRI signal intensity enhancement of up to 79%.Through comparative molecular dynamics studies using a series of solution and solid-state^(1)H/^(19)F nuclear magnetic resonance(^(1)H/^(19)F NMR)and molecular dynamics simulations,it was found that the formation of mechanical bonds dramatically restricts the motion of the wheel fluorines and thus increasing the R1for higher^(19)F MRI sensitivity.Besides a novel strategy for improving^(19)F MRI sensitivity,this study has established^(19)F NMR/MRI as a valuable technology for monitoring the molecular dynamics of rotaxanes,which may shed new light on high-performance^(19)F MRI agents and molecular devices.展开更多
The monkeypox virus(MPXV)outbreak,declared a Public Health Emergency of International Concern(PHEIC)by the World Health Organization(WHO)in 2022,continues to pose a significant threat due to the absence of vaccines or...The monkeypox virus(MPXV)outbreak,declared a Public Health Emergency of International Concern(PHEIC)by the World Health Organization(WHO)in 2022,continues to pose a significant threat due to the absence of vaccines or drugs for MPXV infection.In this study,we developed an mRNA vaccine that expressing the A29L antigen,a specific protein of the intracellular mature virus.Our vaccine utilizes a thermostable ionizable lipid nanoparticle(iLNP)platform and has been administered to mice.Our find-ings demonstrate that the MPXV A29L mRNA vaccine candidate induces robust cross-neutralizing immune responses against both vaccinia virus(VACV)and MPXV live virus.Furthermore,immunization with the vaccine candidate provided protection against the VACV challenge in mice.These findings underscore the potential of mRNA-LNP vaccines as safe and effective candidates against monkeypox epidemics.Given the current absence of specific interventions for MPXV infection,our study represents a significant step forward in developing a viable solution to combat this ongoing public health threat.展开更多
The mode selectivity of the H+CH_(3)D→H_(2)+CH_(2)D reaction was studied using a recently developed ten-dimensional time-dependent wave packet method.The reaction dynamics are studied for the reactant CH_(3)D initial...The mode selectivity of the H+CH_(3)D→H_(2)+CH_(2)D reaction was studied using a recently developed ten-dimensional time-dependent wave packet method.The reaction dynamics are studied for the reactant CH_(3)D initially from the ground state,the CH_(3) symmetry and asymmetry stretching excitation,the CD stretching excitation and the fundamental and the first overtone of the CH_(3) bending mode.The calculated reaction probabilities show that exciting either of the CH_(3) stretching modes enhances the reactivity in the collision energy range below 1.0 eV,while the CD stretching excitation does not obviously prompt the reaction.Fundamental CH_(3) bending excitation has nearly no effect on promoting reactivity.However,a significant enhancement is observed for the first overtone excitation of the CH_(3) bending mode,resulting from the Fermi resonance between the fundamental state of the CH_(3) symmetry stretching mode and the first overtone state of the CH_(3) bending mode.展开更多
The realization of good aqueous dispersibility of commercial graphene products composed of exfoliated graphene sheets is of significance for downstream applications.However,the tap density of commercial graphene powde...The realization of good aqueous dispersibility of commercial graphene products composed of exfoliated graphene sheets is of significance for downstream applications.However,the tap density of commercial graphene powder is quite low(0.03-0.1 kg/m3),meaning that 1 kg graphene powder occupies about 10-30 m3 in volume during transportation.And,the available content of commercial graphene dispersion/slurry in aqueous medium cannot exceed 5 wt%,although the density is high(≈1050 kg/m3).In this work,a graphene monolith was prepared by oven-drying of graphene sheets prefunctionalized with poloxamer surfactants.Our graphene monoliths not only have a high density(1500 kg/m^3) and high graphene content(≈10 wt%),but also a full capability to be completely redispersed(≈100%) in water by bath sonication to obtain solubilized graphene sheets,whose lateral size and thickness are unchanged compared to as-exfoliated ones.Moreover,a simple empirical method was proposed to predict the redispersion capability of graphene monoliths using different poloxamers by contact angle measurements.Our results provide a universal approach to make exfoliated graphene-based products with better downstream availability and lower transportation cost.展开更多
基金the financial support from the National Natural Science Foundation of China(52172110,52472231,52311530113)Shanghai"Science and Technology Innovation Action Plan"intergovernmental international science and technology cooperation project(23520710600)+1 种基金Science and Technology Commission of Shanghai Municipality(22DZ1205600)the Central Guidance on Science and Technology Development Fund of Zhejiang Province(2024ZY01011)。
文摘Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electrocatalytic oxidations of saturated alcohols(C_(1)-C_(6))to selectively form formate using Ni Co hydroxide(Ni Co-OH)derived Ni Co_(2)O_(4)solid-acid electrocatalysts with balanced Lewis acid(LASs)and Brønsted acid sites(BASs).Thermal treatment transforms BASs-rich(89.6%)Ni Co-OH into Ni Co_(2)O_(4)with nearly equal distribution of LASs(53.1%)and BASs(46.9%)which synergistically promote adsorption and activation of OH-and alcohol molecules for enhanced oxidation activity.In contrast,BASs-enriched Ni Co-OH facilitates formation of higher valence metal sites,beneficial for water oxidation.The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6alcohols increases as increased number of hydroxyl groups and decreased HOMO-LUMO gaps:methanol(C_(1))<ethylene glycol(C_(2))<glycerol(C3)<meso-erythritol(C4)<xylitol(C5)<sorbitol(C6),while the formate selectivity shows the opposite trend from 100 to 80%.This study unveils synergistic roles of LASs and BASs,as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.
基金supported by the National Natural Science Foundation of China(No.22373112 to Ji Qi,No.22373111 and 21921004 to Minghui Yang)GH-fund A(No.202107011790)。
文摘In this study,we investigate the ef-ficacy of a hybrid parallel algo-rithm aiming at enhancing the speed of evaluation of two-electron repulsion integrals(ERI)and Fock matrix generation on the Hygon C86/DCU(deep computing unit)heterogeneous computing platform.Multiple hybrid parallel schemes are assessed using a range of model systems,including those with up to 1200 atoms and 10000 basis func-tions.The findings of our research reveal that,during Hartree-Fock(HF)calculations,a single DCU ex-hibits 33.6 speedups over 32 C86 CPU cores.Compared with the efficiency of Wuhan Electronic Structure Package on Intel X86 and NVIDIA A100 computing platform,the Hygon platform exhibits good cost-effective-ness,showing great potential in quantum chemistry calculation and other high-performance scientific computations.
基金supported by the National Key Research&Development Program of China(Nos.2021YFC2302400,2021YFA1201000,2023YFC2606004)the Fundamental Research Funds for the Central Universities(No.2022CX01013)。
文摘Linear mRNA vaccines are constrained by exonuclease susceptibility and instability,leading to compromised antigen expression.Circular RNA(circRNA) lacking canonical 5' and 3' untranslated regions demonstrates intrinsic exonuclease resistance.Current circularization strategies face three principal limitations:chemical methods produce non-native 2',5'-phosphodiester bonds;ribozyme-mediated approaches are restricted to RNA fragments shorter than 500 nucleotides;the Anabaena Group I intron system retains immunogenic exon sequences.In contrast,the self-splicing Group I intron ribozyme from Tetrahymena enables precisely controlled circularization through autonomous structural rearrangement,yielding exonfree constructs.Through optimized purification protocols,historical scalability challenges are systematically addressed.This Perspective establishes the mechanistic rationale and therapeutic superiority of this engineered RNA circularization platform.
文摘The lithium battery is an essential component of electric cars;prompt and accurate problem detection is vital in guaranteeing electric cars’safe and dependable functioning and addressing the limitations of Back Propagation(BP)neural networks in terms of vanishing gradients and inability to effectively capture dependencies in time series,and the limitations of Long-Short Term Memory(LSTM)neural network models in terms of risk of overfitting.A method based on LSTM-BP is put forward for power battery fault diagnosis to improve the accuracy of lithium battery fault diagnosis.First,a lithium battery model is constructed based on the second-order RC equivalent circuit and the electro-thermal coupling model,and various lithium battery failures are simulated to examine the fault characteristics.Then,the lithium battery charging and discharging experiments collect,clean,and process the battery data.By constructing a neural network LSTM-BP model,we verified the superiority and accuracy of the LSTM-BP neural network model by comparing the LSTM model and BP model vertically and by comparing the Recurrent Neural Network(RNN)model,the Gated Recurrent Unit(GRU)model,and the Residual Neural Network(ResNet)model of a more advanced architecture horizontally.Finally,the lithium battery fault diagnosis process is summarized through the threshold quantitative criteria,and different faults are diagnosed and analyzed.Theresults show that the LSTM-BP neural network not only overcomes the limitations of the LSTMneural network and BP neural network but also improves the ability to process sequence data and reduces the risk of overfitting.
基金funded by National Natural Science Foundation of China(92578123)Shenzhen High-level Hospital Construction Fund(23250G1001)+3 种基金the Sanming Project of Medicine in Shenzhen(SZSM202311033)National Key Research and Development Program of China(2023YFC2606004)National Natural Science Foundation of China(32501262)Beijing Institute of Technology Research Fund Program for Young Scholars(6120220072).
文摘Dengue virus(DENV)is a mosquito-borne pathogen responsible for a spectrum of illnesses,including dengue fever,dengue hemorrhagic fever,and dengue shock syndrome.Nearly half of the global population is at risk of DENV infection,making it a pressing public health issue worldwide.The limited cross-protection among the four DENV serotypes(DENV1-4)and the phenomenon of antibody-dependent enhancement(ADE)have posed significant challenges to the development of effective dengue vaccines.Furthermore,there are currently no specific antiviral treatments available.This review provides an overview of DENV's key characteristics,clinical manifestations,and recent advancements in antiviral drug development-including the repurposing of approved drugs,peptidebased antiviral agents,therapeutic antibodies,natural products with antiviral potential,and host factor inhibitors-aiming to offer critical insights to inform strategies for managing and preventing dengue outbreaks.
基金Supported by National Natural Science Fund of China(Effect of Modified Zhuyeshigao granule and Its Componentson Preventing Radiation Esophagitis of Rats)(No.81173195)Capital Medical Development Fund(Traditional Chinese Medicine Class,No.SF-2009-III-45)
文摘OBJECTIVE： To investigate the effects of Zhuyesh- igao granule （ZSG） on tumor necrosis factor-a （TNF-a）, interleukin-1 （IL-1）, IL-2, IL-6, and IL-8 in rats with radiation esophagitis. METHODS： Fifty Wistar rats were randomly divid- ed into five groups （10 rats in each group）： con- trol （without radiation）, saline-treated, and low, medium, and high-dose ISG-treated groups. Rats were given normal saline （10 mL/kg） or 1.15, 2.3, or 4.6 g/kg ZSG by intragastric administration once a day for 7 days. A rat model of radiation esophagi- tis was established by local irradiation of Co60 （490.25 cGy/min, totaling 30 Gy）. The administra- tion of ZSG was continued for another 7 days and on the 7th day post-irradiation, inferior vena cavablood was collected. The serum was separated, and TNF-a, IL-1, IL-2, 11_-6, and IL-8 protein levels were determined. RESULTS： Inflammatory response factors were found in the serum of each group. However, levels in ZSG-treated groups were significantly lower than in the saline-treated group （P〈0.05）. CONCLUSION： ZSG may prevent the development of radiation esophagitis, perhaps by inhibiting the generation and release of the inflammatory re- sponse factors TNF-a, IL-1, IL-2, IL-6, and IL-8.
基金financially supported by the National Natural Science Foundation of China (No.21575165)
文摘An electrochemical sensor for doxycycline hyclate(DC)detection with high sensitivity and good selectivity is reported.The sensor was fabricated by electro-polymerization of molecularly imprinted polymers(MIPs)in the presence of DC onto multi-walled carbon nanotubes modified glassy carbon electrode(MWCNTs/GCE).The MWCNTs can significantly increase the current response of the sensor,leading to enhanced sensitivity.The MIPs provide selective recognition sites for DC detection.The experimental parameters,such as the polymer monomer concentration,supporting electrolyte pH,the time for electro-polymerization and the incubation time of the sensor with DC were optimized.Under optimized experimental conditions,the sensor displayed a linear range of 0.05μmol/L-0.5μmol/L towards DC detection,with the detection limit of 1.3×10^-2μmol/L.The sensor was successfully applied for recovery test of DC in human serum samples.
基金supported by Chinese Academy of Sciences(Grant No.2018PS0011)100 Talent Plan of Chinese Academy of Sciences+4 种基金Natural Science Foundation of China(Grant No.61971405)the Department of Science and Technology(GoI)for support through the Project Nos.DST FILE NO.YSS/2015/001712,DST 11-IFAPH-07 and DST FILE NO.DST/TMD/SERI/HUBthe financial support from Equipment Research Program(Grant No.6140721050215)the Ontario Ministry of Research and Innovation(ER15-11-123)the Natural Science and Engineering Council of Canada(RGPIN-2019-05994).
文摘As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an attractive route for generating efficient electrocatalysts with high mass transport capabilities.Herein,we report an efficient hard templating pathway to design and synthesize three-dimensional(3-D)mesoporous ternary nickel iron nitride(Ni3FeN).The as-synthesized electrocatalyst shows good OER performance in an alkaline solution with low overpotential(259 mV)and a small Tafel slope(54 mV dec?1),giving superior performance to IrO2 and RuO2 catalysts.The highly active contact area,the hierarchical porosity,and the synergistic effect of bimetal atoms contributed to the improved electrocatalytic performance toward OER.In a practical rechargeable Zn–air battery,mesoporous Ni3FeN is also shown to deliver a lower charging voltage and longer lifetime than RuO2.This work opens up a new promising approach to synthesize active OER electrocatalysts for energy-related devices.
基金financial support from NSFC(51602332)the National Key Research and Development Program of China(2016YFB0700204)+4 种基金Science and Technology Commission of Shanghai Municipality(15520720400,16DZ2260603)Equipment Research Program(6140721050215)the National 1000 Youth Talents program of Chinafinancial support from Ningbo 3315 programDST Solar Energy Harnessing Centre(DST/TMD/SERI/HUB/1(C)),DST Materials for Energy Storage program,Ministry of Electronics and Information Technology(India)(Project ID:ELE1819353MEITNAK)
文摘Nitrogen-doped carbon materials with a large specific surface area,high conductivity,and adjustable microstructures have many prospects for energy-related applications.This is especially true for N-doped nanocarbons used in the electrocatalytic oxygen reduction reaction(ORR)and supercapacitors.Here,we report a low-cost,environmentally friendly,large-scale mechanochemical method of preparing N-doped porous carbons(NPCs)with hierarchical micro-mesopores and a large surface area via ball-milling polymerization followed by pyrolysis.The optimized NPC prepared at 1000°C(NPC-1000)offers excellent ORR activity with an onset potential(Eonset)and half-wave potential(E1/2)of 0.9 and 0.82 V,respectively(vs.a reversible hydrogen electrode),which are only approximately 30 mV lower than that of Pt/C.The rechargeable Zn–air battery assembled using NPC-1000 and the NiFe-layered double hydroxide as bifunctional ORR and oxygen evolution reaction electrodes offered superior cycling stability and comparable discharge performance to RuO2 and Pt/C.Moreover,the supercapacitor electrode equipped with NPC prepared at 800℃ exhibited a high specific capacity(431 F g^−1 at 10 mV s^−1),outstanding rate,performance,and excellent cycling stability in an aqueous 6-M KOH solution.This work demonstrates the potential of the mechanochemical preparation method of porous carbons,which are important for energy conversion and storage.
基金the financial support from the Science and Technology Commission of Shanghai Municipality(19ZR1479500)the National Natural Science Foundation of China(52072389)the Program of Shanghai Academic Research Leader(20XD1424300)for financial support。
文摘Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline.However,the additional utilization of a reductant and/or the operation at the elevating temperature causes the over-growth and agglomeration of Pt clusters,thus losing the high catalytic performance.Herein,we report that V dopant not only favors self-reducing Pt clusters on Ni Fe layered double hydroxide(LDH)(Pt/NiFeV)at room temperature,but also regulates interfacial charge redistribution to enhance the water-splitting performance.Experimental and theoretical studies reveal that V dopant into Ni Fe LDH triggers more electrons to transfer to adjacent Fe atoms,thus leading to a higher reducing ability compared to that without V-doping.When used as water-splitting electrocatalyst,V doping promotes electron loss of Pt clusters in Pt/Ni Fe V,optimizing the free energy of hydrogen adsorption and proton recombination kinetics at the cathode.Meanwhile,it also moves the d-band center of Ni away from the Fermi level to optimize the adsorption of*OH intermediates and facilitate the desorption of oxygen molecules at the anode.Thereby,Pt/Ni Fe V exhibits much higher bifunctional performance than V-free Pt/Ni Fe LDH toward both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).This work can spark inspiration of designing other bifunctional electrocatalysts for energy conversion and storage.
基金supported by programs for the 973 National Basic Research Program of China (2014CB138505)the Open Foundation of State Key Laboratory of Animal Nutrition (2004DA115184F1415)
文摘Background： Resveratrol, an important phyto-antioxidant commonly found in grapes, mulberry, and other plants,has a variety of functions including anti-aging, anti-cancer and anti-inflammatory activities. In the current study, we investigated the beneficial effects of resveratrol on in vitro porcine oocyte maturation under heat stress（HS）. The effect of resveratrol, melatonin and their combination on alleviating HS was compared according to the maturation rate of oocytes and the development competence of embryos after parthenogenetic activation（PA）.Results： Supplementation with resveratrol（2.0 μmol/L） not only improved the nuclear maturation but also raised the blastocyst rate of porcine embryos＇ PA from oocytes that underwent HS by increasing their glutathione（GSH）level, reducing reactive oxygen species（ROS） and up-regulating the expression of Sirtuin 1（SIRT1）. It was also found that melatonin（10^-7mol/L） and the combination of resveratrol（2.0 μmol/L） plus melatonin（10^-7mol/L） exhibited more potent effects than resveratrol alone regarding their protective activities on oocyte maturation under HS.Conclusions： This study compared the efficiencies of resveratrol, melatonin and their combination for protecting porcine oocytes from heat stress. The mechanisms are attributed to the fact that each treatment may have different ability to regulate the synthesis of steroid hormones and the expression of mature related genes.
基金supported by the National Natural Science Foundation of China(No.21575165)。
文摘This article describes a fast and simple electrochemical assay for detecting cell concentration.After cell death,the membrane of cells will be broken,and DNA molecules contained in the cells will be released,but this does not happen in living cells.Sodium molybdate can react with the phosphate backbone of the released DNA molecules to form phosphomolybdate precipitation and produces a corresponding redox current.The higher the concentration of DNA,the stronger the intensity of the current generated.Sodium molybdate solution and centrifuged cell supernatant were added onto the glassy carbon electrode to determine the cell concentration by measuring the current intensity.The cell viability,which means the ratio of living cells to the total cells,can also be determined by this method.This assay has the advantages of high sensitivity,low detection limit,and wide detection range.In addition,this method was successfully applied to the detection of cell concentration in human serum,which has potential clinical applications.
基金supported by the National Natural Science Foundation of China,No.61977006.
文摘Nowadays,smart wearable devices are used widely in the Social Internet of Things(IoT),which record human physiological data in real time.To protect the data privacy of smart devices,researchers pay more attention to federated learning.Although the data leakage problem is somewhat solved,a new challenge has emerged.Asynchronous federated learning shortens the convergence time,while it has time delay and data heterogeneity problems.Both of the two problems harm the accuracy.To overcome these issues,we propose an asynchronous federated learning scheme based on double compensation to solve the problem of time delay and data heterogeneity problems.The scheme improves the Delay Compensated Asynchronous Stochastic Gradient Descent(DC-ASGD)algorithm based on the second-order Taylor expansion as the delay compensation.It adds the FedProx operator to the objective function as the heterogeneity compensation.Besides,the proposed scheme motivates the federated learning process by adjusting the importance of the participants and the central server.We conduct multiple sets of experiments in both conventional and heterogeneous scenarios.The experimental results show that our scheme improves the accuracy by about 5%while keeping the complexity constant.We can find that our scheme converges more smoothly during training and adapts better in heterogeneous environments through numerical experiments.The proposed double-compensation-based federated learning scheme is highly accurate,flexible in terms of participants and smooth the training process.Hence it is deemed suitable for data privacy protection of smart wearable devices.
基金supported by the National Natural Science Foundation of China(22238013 and 22178393)Postdoctoral Science Foundation of Central South University(320808)+1 种基金Natural Science Foundation of Hunan Province(2023JJ40706)the High Performance Computing Center of Central South University。
文摘CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operation or storage,resulting in decreased catalytic performance.Herein,we report a efficient and stable BiIn@Cu-foam electrode through the in-situ regeneration of Bi^(0) active sites to renew the surface activation.The electronic structure of Bi site can be regulated by introducing In,thereby enhancing the adsorption strength of*OCHO.The optimized electrode exhibits over 90%FE_(formate)at a wide potential window(-0.9–-2.2 V),and formation rate for 3.15 mM cm^(-1)h^(-1).Especially,the electrode can maintain the high performance at continuously electrolysis for more than 300 h,or for more than 50 cycles,even repeated operation and storage for more than 2 years.This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.
基金the financial support by the National Natural Science Foundation of China(Nos.51573201,51501209,201675165 and 61901460)NSFC-Zhejiang Joint Fund for the Integration of Industrialization and Informatization(No.U1709205)+7 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA22000000)Scientific Instrument Developing Project of the Chinese Academy of Sciences(No.YZ201640)Science and Technology Major Project of Ningbo(Nos.2016S1002 and 2016B10038)International S&T Cooperation Program of Ningbo(No.2017D10016)China Postdoctoral Science Foundation(No.2019M653125)for financial supportthe Chinese Academy of Sciences for Hundred Talents ProgramChinese Central Government for Thousand Young Talents Program3315 Program of Ningbo。
文摘Graphene nanosheets are widely used in anti-corrosion polymeric coating as filler,owing to the excellent electrochemical inertness and barrier property.However,as the arrangement of graphene nanosheets is difficult to form a perfect layered structure,polymeric coating with graphene nanosheets usually needs micron-scale thickness to ensure the enhancement of corrosion protection.In this work,layer-by-layer stacked graphene nanocoatings were fabricated on stainless steel by self-assembly based on Marangoni effect.The anti-corrosion property of graphene coatings were studied through Tafel polarization curves,electrochemical impedance spectroscopy and accelerated corrosion test with extra applied voltage.The self corrosion current density of optimized three-layered graphene coated sample was one quarter of that of bare stainless steel.And the self corrosion potential of optimized sample is increased to-0.045 V.According to the results,graphene nanocoatings composed of layered nanosheets exhibits good anticorrosion property.Besides,the self-assembly method provide a promising approach to make layeredstructure coating for other researches about 2 D material nanosheets.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0540000)the National Key R&D Program of China(No.2018YFA0704000)+2 种基金the National Natural Science Foundation of China(Nos.22327901,22077098,U21A20392,21921004,and 82127802)the Knowledge Innovation Program of WuhanBasic Research(No.2022020801010137)support from the Youth Innovation Promotion Association and the Young Top-notch Talent Cultivation Program。
文摘As a promising imaging technology,the low sensitivity of fluorine-19 magnetic resonance imaging(^(19)F MRI)severely hinders its biomedical applications.Herein,we have developed an unprecedented rotaxanebased strategy to improve the sensitivity of^(19)F MRI agents.By threading the fluorinated macrocycle into2-blade pinwheel[2]rotaxanes,the^(19)F longitudinal relaxation rate R1was dramatically increased,resulting in a significant^(19)F MRI signal intensity enhancement of up to 79%.Through comparative molecular dynamics studies using a series of solution and solid-state^(1)H/^(19)F nuclear magnetic resonance(^(1)H/^(19)F NMR)and molecular dynamics simulations,it was found that the formation of mechanical bonds dramatically restricts the motion of the wheel fluorines and thus increasing the R1for higher^(19)F MRI sensitivity.Besides a novel strategy for improving^(19)F MRI sensitivity,this study has established^(19)F NMR/MRI as a valuable technology for monitoring the molecular dynamics of rotaxanes,which may shed new light on high-performance^(19)F MRI agents and molecular devices.
基金supported by National Key Research&Development Program of China(Nos.2021YFA1201000,2021YFC2302400)Beijing Institute of Technology Research Fund Program for Young Scholars(No.XSQD-6120220072)+1 种基金National Natural Science Foundation of China(No.82371846)China Postdoctoral Science Foundation(No.2022M720438).
文摘The monkeypox virus(MPXV)outbreak,declared a Public Health Emergency of International Concern(PHEIC)by the World Health Organization(WHO)in 2022,continues to pose a significant threat due to the absence of vaccines or drugs for MPXV infection.In this study,we developed an mRNA vaccine that expressing the A29L antigen,a specific protein of the intracellular mature virus.Our vaccine utilizes a thermostable ionizable lipid nanoparticle(iLNP)platform and has been administered to mice.Our find-ings demonstrate that the MPXV A29L mRNA vaccine candidate induces robust cross-neutralizing immune responses against both vaccinia virus(VACV)and MPXV live virus.Furthermore,immunization with the vaccine candidate provided protection against the VACV challenge in mice.These findings underscore the potential of mRNA-LNP vaccines as safe and effective candidates against monkeypox epidemics.Given the current absence of specific interventions for MPXV infection,our study represents a significant step forward in developing a viable solution to combat this ongoing public health threat.
基金supported by the National Natural Science Foundation of China(No.21773297,No.21973108,and No.21921004 to Minghui Yang,No.21973109 to Hongwei Song)。
文摘The mode selectivity of the H+CH_(3)D→H_(2)+CH_(2)D reaction was studied using a recently developed ten-dimensional time-dependent wave packet method.The reaction dynamics are studied for the reactant CH_(3)D initially from the ground state,the CH_(3) symmetry and asymmetry stretching excitation,the CD stretching excitation and the fundamental and the first overtone of the CH_(3) bending mode.The calculated reaction probabilities show that exciting either of the CH_(3) stretching modes enhances the reactivity in the collision energy range below 1.0 eV,while the CD stretching excitation does not obviously prompt the reaction.Fundamental CH_(3) bending excitation has nearly no effect on promoting reactivity.However,a significant enhancement is observed for the first overtone excitation of the CH_(3) bending mode,resulting from the Fermi resonance between the fundamental state of the CH_(3) symmetry stretching mode and the first overtone state of the CH_(3) bending mode.
基金financial support by the National Natural Science Foundation of China(Nos.51573201,51501209 and 201675165)NSFC-Zhejiang Joint Fund for the Integration of Industrialization and Informatization(No.U1709205)+6 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA22000000)Scientific Instrument Developing Project of the Chinese Academy of Sciences(No.YZ201640)Science and Technology Major Project of Ningbo(Nos.2016S1002 and 2016B10038)International S&T Cooperation Program of Ningbo(No.2017D10016)for financial supportthe Chinese Academy of Sciences for Hundred Talents ProgramChinese Central Government for Thousand Young Talents Program3315 Program of Ningbo。
文摘The realization of good aqueous dispersibility of commercial graphene products composed of exfoliated graphene sheets is of significance for downstream applications.However,the tap density of commercial graphene powder is quite low(0.03-0.1 kg/m3),meaning that 1 kg graphene powder occupies about 10-30 m3 in volume during transportation.And,the available content of commercial graphene dispersion/slurry in aqueous medium cannot exceed 5 wt%,although the density is high(≈1050 kg/m3).In this work,a graphene monolith was prepared by oven-drying of graphene sheets prefunctionalized with poloxamer surfactants.Our graphene monoliths not only have a high density(1500 kg/m^3) and high graphene content(≈10 wt%),but also a full capability to be completely redispersed(≈100%) in water by bath sonication to obtain solubilized graphene sheets,whose lateral size and thickness are unchanged compared to as-exfoliated ones.Moreover,a simple empirical method was proposed to predict the redispersion capability of graphene monoliths using different poloxamers by contact angle measurements.Our results provide a universal approach to make exfoliated graphene-based products with better downstream availability and lower transportation cost.
