Background: India has scaled up ART programme very rapidly. Though there are reports on retention of patients in the national programme, data on transfer out patients within the ART centers are scanty in India. Method...Background: India has scaled up ART programme very rapidly. Though there are reports on retention of patients in the national programme, data on transfer out patients within the ART centers are scanty in India. Methods: This is a retrospective study of patients receiving antiretroviral treatment between January 2006 and July 2013. The patients who were transferred out from the ART center at National AIDS Research Institute in Pune were included in the study. The data on whether they reached the respective ART centers were collected either by making telephonic calls to the patients and/or to the respective ART centers. Results: Of the total 3015 patients ever started on treatment from the ART center, 158 (5.24%) were transferred out to other ART centers. Of these, 123 (77.8%) patients reached other centres and they were “transferred in”. However, 15 (9.5%) did not reach to respective ART centers and information could not be obtained for 20 (12.7%) transferred out patients. The analysis showed that those who were not living with their partners were 4.53 times more likely to not to reach the preferred ART centre after taking transfer [OR, 95% CI: (1.24 - 16.51), p = 0.022]. Conclusion: Our data suggest that significant number of transfer out patients is lost in HIV treatment cascade. Considering the total PLHIV on treatment in the country, this group adds significantly to the burden of lost to follow up patients. It is important to strengthen the system of tracking the transfer out patients in the programme which will help in patching an important leak in the cascade of HIV care.展开更多
OBJECTIVE:To investigate the effect of—Xiaoyi Yusi decoction(XYYSD,消异育嗣汤),a Traditional Chinese Medicine(TCM),on in vitro fertilization and embryo transfer(IVF-ET)in patients with endometriosis,and to study the ...OBJECTIVE:To investigate the effect of—Xiaoyi Yusi decoction(XYYSD,消异育嗣汤),a Traditional Chinese Medicine(TCM),on in vitro fertilization and embryo transfer(IVF-ET)in patients with endometriosis,and to study the mechanism underpinning the action.METHODS:Women who underwent IVF-ET were divided into three groups by simple randomization:the treatment(n=32;with TCM treatment),patient(n=28;with endometriosis alone),and control(n=33;with male factor alone)groups.The luteal phase short-acting gonadotropin-releasing hormone agonist prolonged protocol was used in all three groups.To compare the changes in TCM scores and reproductive outcomes before and after TCM intervention in patients with endometriosis,partial least-squares discriminant analysis was used to analyze the follicular fluid samples of each group and screen and compare metabolites using the MetaboA nalyst software.RESULTS:The clinical data indicated that following TCM intervention,kidney deficiency and blood stasis symptom patterns improved dramatically in patients with endometriosis and that their clinical pregnancy rate increased significantly(71.9%vs 57.1%,P<0.05).Metabolomics showed that the two groups of samples were separated before and after TCM intervention.After TCM intervention,the intervention group was close to the control group,indicating that the TCM had a certain effect.Pathway analysis revealed that after TCM intervention,the metabolism of glycerin phospholipid,pyruvate,and citric acid was regulated.CONCLUSIONS:Through the pyruvate and glycerophospholipid metabolism pathways and tricarboxylic acid cycle,the TCM XYYSD successfully improved kidney deficiency and blood stasis symptom pattern,as well as the clinical reproductive outcomes of patients with endometriosis-related infertility.展开更多
Objective:To investigate the effect of abnormal ovarian granulosa cell metabolism on in vitro fertilization and embryo transfer(IVF-ET)outcomes in obese polycystic ovary syndrome(PCOS)patients.Methods:Patients with PC...Objective:To investigate the effect of abnormal ovarian granulosa cell metabolism on in vitro fertilization and embryo transfer(IVF-ET)outcomes in obese polycystic ovary syndrome(PCOS)patients.Methods:Patients with PCOS who met the study criteria were screened according to the inclusion criteria.A total of 32 patients with obese PCOS were recruited into the study group,and 39 patients with non-obese PCOS were recruited into the control group.The general data(age,body mass index,and years of infertility),insulin resistance index(HOMA-IR),follicle-stimulating hormone(FSH),luteinizing hormone(LH),granulosa cell mitochondrial function,and IVF-ET outcome of patients in the study group and control group were retrospectively analyzed.Results:The differences in age and years of infertility between the study group and the control group were insignificant(P>0.05),and the body mass index(BMI)of the study group and control group was 30.5±1.24 kg/m2 and 22.3±1.12 kg/m2,respectively,in which the difference was statistically significant(P<0.05);the HOMA-IR of the study group was significantly higher than that of the control group(P<0.05);the reactive oxygen species(ROS)in the study group was significantly higher than that in the control group(P<0.05),and the ATP content in the study group was significantly lower than that in the control group(P<0.05);comparing the FSH and LH levels between the two groups,the difference was not statistically significant(P>0.05);the rate of IVF-ET failure was significantly higher in the study group than in the control group.Conclusion:PCOS is a complex endocrine disorder,and obesity is one of the independent risk factors for the development of PCOS.展开更多
Fluorescent probes based on intramolecular charge transfer(ICT) have obvious advantages for accurate quantitative analysis.To obtain high-performance ratiometric probes requires distinct photophysical properties durin...Fluorescent probes based on intramolecular charge transfer(ICT) have obvious advantages for accurate quantitative analysis.To obtain high-performance ratiometric probes requires distinct photophysical properties during recognition reaction process,which is closely related to their ICT characteristics.1,8-Naphthalimide is known as a typical fluorophore with desirable ICT property when functionalized with an electron-donating moiety at the para-position of the naphthalene chromophore.Although the photophysical properties of para-substituted 1,8-naphthalimide have been well studied,its meta-substituted counterpart has not been fully evaluated since the meta-position is conventionally thought to be weakly conjugated.Herein,combined experimental and theoretical studies are performed which consistently indicate that stronger charge transfer(CT) is exhibited by the meta-amino substituted 1,8-naphthalimide(m-NH_(2)) compared to the para-amino substituted one(p-NH_(2)).The ratiometric response of fluorescence with significant changes in wavelength and intensity upon acetylation(m-NAc and p-NAc) can be attributed to the larger ICT and stronger-NH_(2) vibrations.This observation is further demonstrated by deuterium oxide experiments,viscosity experiments and quantum chemical calculations.The practical application of meta-amino-1,8-naphthalimide ICT-based probes is also confirmed.This research is expected to bring an in-depth understanding of π-conjugated systems with ICT characteristics,and facilitates the design of sensitive ICT fluorescent probes with meta-amino substitution.展开更多
Objective:Advanced maternal age is associated with reduced ovarian reserve and lower oocyte quality.Whether body mass index(BMI)further influences assisted reproductive technology(ART)outcomes in this population remai...Objective:Advanced maternal age is associated with reduced ovarian reserve and lower oocyte quality.Whether body mass index(BMI)further influences assisted reproductive technology(ART)outcomes in this population remains unclear.Methods:This retrospective study analyzed 222 patients aged≥37 years who underwentin vitro fertilization or intracytoplasmic sperm injection with embryo transfer(IVF/ICSI-ET)at the First Affiliated Hospital of Xiamen University between January 2019 and December 2023.Patients were classified by BMI as underweight(<18.5 kg/m^(2);n=13),normal(18.5-24.9 kg/m^(2);n=154),or overweight(>24.9 kg/m^(2);n=55).Controlled ovarian stimulation protocols were individualized according to ovarian reserve.Laboratory and clinical outcomes were compared across groups,and multivariable logistic regression was used to identify factors associated with clinical pregnancy and live birth.Results:BMI,total gonadotropin dose,and use of IVFvs.ICSI differed among groups(allP<0.05).However,oocyte retrieval rate,metaphase II(MII)oocyte rate,cleavage rate,available embryo rate,high-quality embryo rate,biochemical pregnancy rate,clinical pregnancy rate,live birth rate,and miscarriage rate showed no significant differences(allP>0.05).In multivariable analysis,age,infertility duration,and progesterone level on the day of human chorionic gonadotropin(hCG)trigger were independent predictors of clinical pregnancy.Moreover,age and progesterone level on the hCG day were independently associated predictors of live birth(allP<0.05).Conclusions:Among women aged≥37 years,higher BMI did not significantly affect key laboratory or pregnancy outcomes after IVF/ICSI-ET.Clinical results were mainly influenced by age,infertility duration,and progesterone level on the hCG trigger day.展开更多
Objective:To assess whether personalized embryo transfer guided by endometrial receptivity array(ERA)improves implantation and pregnancy rates in women with implantation failure.Methods:This retrospective case-control...Objective:To assess whether personalized embryo transfer guided by endometrial receptivity array(ERA)improves implantation and pregnancy rates in women with implantation failure.Methods:This retrospective case-control study was conducted on women with previous implantation failure.The women were divided into two groups,i.e,women who underwent ERA and those who underwent embryo transfer without ERA testing.ERA was performed using Igenomix.ERA results were interpreted as receptive or non-receptive.Women underwent frozen embryo transfer on the 6th day of progesterone(P+5).The primary outcomes were implantation rate,clinical pregnancy rate,abortion rate,and negative pregnancy rate.Results:This study included 229 women with previous implantation failure,with 154 in the ERA group and 75 in the no ERA group.The mean age of the women of the ERA group was(32.2±4.1)years,and that of the no ERA group was(31.5±4.8)years.Women in the ERA group had a higher implantation rate(60.4%)and clinical pregnancy rate(57.1%)compared to those in the no ERA group(48.0%and 46.7%,respectively).In addition,implantation rate of the nonreceptive ERA group was higher than the no ERA group(65%vs.48%),and clinical pregnancy rate was also higher in the non-receptive ERA group than the no ERA group(65%vs.47%).The abortion rate of the no ERA group was 9%and that of the non-receptive ERA group was 10%.52%no ERA group women and 35%non-receptive ERA group women had negative pregnancy results.Conclusions:Women who have undergone personalised embryo transfer guided by ERA have a higher clinical pregnancy rate than women who have not after previous implantation failure.展开更多
A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,...A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,γ-difluoro-and γ-monofluoro-vinylacetic acids without stepwise acidification,exhibiting good functional group tolerance,broad scope,and facile scalability.Mechanism studies support that thiol plays the role of the hydrogen relay,which s a hydrogen atom through HAT and then outputs a proton via PT.This strategy also takes full advantage of formate for photocatalytic carboxylation reaction in a step-and atomeconomical way.展开更多
This study investigates the enhancement of convective heat transfer in a serpentine pipe using ferrofluid flow influenced by dual non-uniform magnetic sources.The primary objective is to improve thermal performance in...This study investigates the enhancement of convective heat transfer in a serpentine pipe using ferrofluid flow influenced by dual non-uniform magnetic sources.The primary objective is to improve thermal performance in compact cooling systems,such as those used in heat exchangers.A two-dimensional,steady-state Computational Fluid Dynamic(CFD)model is developed in ANSYS Fluent to simulate the behavior of an incompressible ferrofluid under applied constant heat flux and magnetic fields.The magnetic force is modeled using the Kelvin force,which acts on magnetized nanoparticles in response to spatially varying electromagnetic fields generated by two strategically positioned current-carrying wires.The effects of magnetic field strength,quantified by the magnetic number(Mn),on flow behavior and temperature distribution are thoroughly analyzed.The results indicate that increasing Mn leads to higher Nusselt numbers,demonstrating enhanced convective heat transfer.Secondary vortices induced by magnetic forcing improve fluid mixing,particularly in curved regions of the pipe.A mesh-independence study and model validation with benchmark data support the reliability of the numerical framework.This work highlights the potential of magnetic-field-assisted thermal control in energy-efficient cooling applications and provides a foundation for the further development of advanced ferrofluid-based heat transfer systems.展开更多
In this study,we meticulously designed a layered carbon-based catalytic material to induce the degradation of a series of organic pollutants by activating peroxymonosulfate(PMS) in the PMS-based advanced oxidation pro...In this study,we meticulously designed a layered carbon-based catalytic material to induce the degradation of a series of organic pollutants by activating peroxymonosulfate(PMS) in the PMS-based advanced oxidation processes(AOPs).Results indicated that the silicon and oxygen elements from the montmorillonite were incorporated into the catalyst matrix to form the Si-O-C structure.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array,achieving over 90 % removal rate of most pollutants within 60 min.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array.The salt bridge system confirmed that pollutants can provide electrons to the Si-O-C/PMS system,and we verified that the electron transfer process(ETP) mechanism was the main pathway for the degradation of pollutants in the Si-O-C/PMS system via the open-circuit potential analysis.In combination with the structural properties of different pollutants,we discovered that electron-donating pollutants can supply more electrons to the Si-O-C/PMS system,thereby enhancing the ETP process.The findings of this study are anticipated to advance the development and practical application of layered carbonaceous materials-based catalysts and support the design and implementation of nanoconfined catalysts in the field of AOPs.展开更多
The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for syn...The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for synthesizing thioesters primarily rely on the acylation of thiols,which produces substantial waste and requires malodorous,unstable sulfur sources.In this work,we introduce a photocatalyzed hydrogen transfer strategy that enables a three-component synthesis of thioesters using abundant primary alcohols,easily available alkenes and elemental sulfur under mild conditions.This protocol demonstrates broad applicability and high chemo-and regioselectivity for both primary alcohols and alkenes,highlighting the advantage and potential of photo-mediated hydrogen transfer in facilitating multicomponent reactions using primary alcohol and elemental sulfur feedstocks.展开更多
The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightfor...The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.展开更多
Cirrus clouds play a crucial role in the energy balance of the Earth-atmosphere system.We investigated the spatiotemporal variations of cirrus over the South China Sea(SCS)using satellite data(MOD08,MYD08,CALIPSO)and ...Cirrus clouds play a crucial role in the energy balance of the Earth-atmosphere system.We investigated the spatiotemporal variations of cirrus over the South China Sea(SCS)using satellite data(MOD08,MYD08,CALIPSO)and reanalysis data(MERRA-2)from March 2007 to February 2015(eight years).The horizontal distribution reveals lower cirrus fraction values in the northern SCS and higher values in the southern region,with minima observed in March and April and maxima sequentially occurring in August(northern SCS,NSCS),September(middle SCS,MSCS),and December(southern SCS,SSCS).Vertically,the cirrus fraction peaks in summer and reaches its lowest levels in spring.Opaque cirrus dominates during summer in the NSCS and MSCS,comprising 53.6%and 55.9%,respectively,while the SSCS exhibits a higher frequency of opaque cirrus relative to other cloud types.Subvisible cirrus clouds have the lowest frequency year-round,whereas thin cirrus is most prominent in winter in the NSCS(46.3%)and in spring in the MSCS(45.3%).A case study from September 2021 further explores the influence of ice crystal habits on brightness temperature(BT)over the SCS.Simulations utilizing five ice crystal shapes from the ARTS DDA(Atmospheric Radiative Transfer Simulator Discrete Dipole Approximation)database and the RTTOV 12.4 radiative transfer model reveal that the 8-column-aggregate shape best represents BT in the NSCS and SSCS,while the large-block-aggregate shape performs better in the SSCS.展开更多
In recent years,with the rapid advancement of artificial intelligence,object detection algorithms have made significant strides in accuracy and computational efficiency.Notably,research and applications of Anchor-Free...In recent years,with the rapid advancement of artificial intelligence,object detection algorithms have made significant strides in accuracy and computational efficiency.Notably,research and applications of Anchor-Free models have opened new avenues for real-time target detection in optical remote sensing images(ORSIs).However,in the realmof adversarial attacks,developing adversarial techniques tailored to Anchor-Freemodels remains challenging.Adversarial examples generated based on Anchor-Based models often exhibit poor transferability to these new model architectures.Furthermore,the growing diversity of Anchor-Free models poses additional hurdles to achieving robust transferability of adversarial attacks.This study presents an improved cross-conv-block feature fusion You Only Look Once(YOLO)architecture,meticulously engineered to facilitate the extraction ofmore comprehensive semantic features during the backpropagation process.To address the asymmetry between densely distributed objects in ORSIs and the corresponding detector outputs,a novel dense bounding box attack strategy is proposed.This approach leverages dense target bounding boxes loss in the calculation of adversarial loss functions.Furthermore,by integrating translation-invariant(TI)and momentum-iteration(MI)adversarial methodologies,the proposed framework significantly improves the transferability of adversarial attacks.Experimental results demonstrate that our method achieves superior adversarial attack performance,with adversarial transferability rates(ATR)of 67.53%on the NWPU VHR-10 dataset and 90.71%on the HRSC2016 dataset.Compared to ensemble adversarial attack and cascaded adversarial attack approaches,our method generates adversarial examples in an average of 0.64 s,representing an approximately 14.5%improvement in efficiency under equivalent conditions.展开更多
Air-permeable and ultrathin conductive electrodes are essential for next-generation soft electronics,including breathable wearables,on-skin devices and biointegrated electronics.However,conventional metallization stra...Air-permeable and ultrathin conductive electrodes are essential for next-generation soft electronics,including breathable wearables,on-skin devices and biointegrated electronics.However,conventional metallization strategies,such as sputtering and ink-printing,often suffer from severe vertical charge leakage due to the porous and ultrathin characteristics of nanofibrous networks,leading to device short-circuiting,operational failure and limited vertical integration.Here,we present a solvent-selective dissolutionassisted transfer printing strategy to achieve surface-confined metallization of ultrathin,lightweight,and gas-permeable nanofibrous networks,enabling lateral conductivity while maintaining vertical insulation.This transfer printing process facilitates not only the rapid formation of conductive patterns on the surface of nanofibrous networks but also mechanical reinforcement through solvent evaporation-induced interlocked fiber-fiber welding.Meanwhile,the strategy preserves the high permeability of the nanofibrous networks and imparts a unique combination of surface conductivity(2Ωcm)and vertical insulativity(10^(11)Ωcm).The resulting anisotropic conductive networks enable low-voltage wearable heaters,high-sensitive pressure sensors,and ultralight temperature sensors.A pressure-temperature dual-modal sensing patch is further fabricated for intelligent grasping classification.The proposed surface-confined metallization strategy enables rapid fabrication of an anisotropic conductive network as a building block to construct air-permeable,ultrathin and lightweight wearable electronics.展开更多
Accurate assessment of seismic landslide susceptibility is crucial for disaster prevention and emergency decision-making.Although machine learning methods have been widely applied in this field,they exhibit a strong d...Accurate assessment of seismic landslide susceptibility is crucial for disaster prevention and emergency decision-making.Although machine learning methods have been widely applied in this field,they exhibit a strong dependence on large quantities of highquality samples,resulting in significantly low prediction accuracy of existing studies under data-scarce or crossregional prediction scenarios,which fail to meet practical application requirements.To address this issue,this study proposes an intelligent prediction model integrating transfer learning and a sampling optimization strategy,aiming to enhance the accuracy and applicability of seismic landslide susceptibility assessment.The model first improves the sample collection method through the sampling optimization strategy to enhance the precision and representativeness of training samples.This not only ensures the accuracy of origin area training but also further strengthens the model's predictive ability in the target area.Subsequently,it incorporates Transfer Component Analysis(TCA)to overcome the differences in environmental characteristics between the origin area and target area,and couples TCA with the Light GBM algorithm to construct the TCA-Light GBM model,realizing the assessment of seismic landslide susceptibility in sample-free areas.Validated through case studies of the Jiuzhaigou and Luding earthquakes,the results demonstrate that the proposed TCALight GBM transfer learning method exhibits excellent applicability in seismic landslide susceptibility prediction.After optimization with the TCA algorithm,the model's prediction performance in the target domain is significantly improved,with the AUC value increasing from 0.719 to 0.827,representing an increase of approximately 15.02%.This indicates that TCA technology can effectively alleviate the feature distribution discrepancy between the source domain and target domain,enhancing the model's generalization ability.The method is particularly suitable for scenarios with data scarcity and cross-regional prediction and can provide reliable technical support for the emergency response and risk prevention and control of seismic hazards.展开更多
Co-assembling chiral molecules with achiral compounds via non-covalent interactions like areneperfluoroarene(AP) interactions offers an effective approach for fabricating chiral functional materials.Herein,chiral mole...Co-assembling chiral molecules with achiral compounds via non-covalent interactions like areneperfluoroarene(AP) interactions offers an effective approach for fabricating chiral functional materials.Herein,chiral molecules L/D-PF1 and L/D-PF2 with pyrene groups were synthesized and its chiroptical properties upon co-assembly with achiral compound octafluoronaphthalene(OFN) through AP interaction were systemically studied.The co-assembly of L/D-PF1/OFN and L/D-PF2/OFN exhibited distinct chiroptical properties such as circular dichroism(CD) and circularly polarized luminescence(CPL) signals.Chirality transfer from the chirality center of L/D-PF1 and L/D-PF2 to the achiral OFN and chiral amplification were successfully achieved.Besides,no significant CPL signal was observed in the self-assembly of L/DPF1 or L/D-PF2 while co-assembly with OFN exhibited obvious CPL amplification induced by AP interaction.Notably,a reversal CD signal and CPL signal could be observed in L/D-PF2/OFN when the molar ratio changed from 1:1 to 1:2 while not found in L/D-PF1/OFN,indicating that that minor structural changes of molecules could cause large changes in assembly.In addition,a series of computational calculations were conducted to verify the AP interaction between L-PF1/L-PF2 and OFN.This work demonstrated that arene-perfluoroarene interaction could drive chiral transfer,chiral amplification and chiral inversion and provided a new method for the preparation of chiroptical materials.展开更多
Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organ...Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organic coordination catalysts showed satisfactory ability of TH in the secondary alcohols,but most of them could not effectively employ the cheaper primary alcohols as hydrogen donors.Furthermore,they commonly contained high metal contents,which also led to low catalytic efficiency in significant measure.In this work,we constructed a novel magnesium single-atom catalyst(Mg-NC)with merely 0.37 wt%Mg by means of a combined self-assembly and pyrolysis strategy.The characterization results indicated that Mg was atomically dispersed and it was coordinated with four pyridinic-N in Mg-NC.Due to the obvious electron transfer from Mg to its coordinated pyridinic-N,Mg–N_(4)active centers displayed high Lewis acid-base strength with abundant content,which brought remarkable catalytic activity.When Mg-NC was used for the TH of 5-hydroxymethylfurfural(HMF)in ethanol(EtOH),2,5-bis(hydroxymethyl)furan(BHMF)yield was up to 96.3%with high productivity of 19.85 molBHMF mol_(Mg)^(−1)h^(−1)at 150°C for 5 h.More interestingly,the process of TH over Mg-NC in EtOH was proved to proceed via the hydrogen radical mechanism.Additionally,Mg-NC exhibited powerful catalytic universality;it could not only utilize other primary alcohols(such as n-propanol and n-butanol)as hydrogen donors,but also catalyze the TH of other carbonyl compounds(such as furfural,5-methylfurfural,benzaldehyde,cyclohexanone,and levulinic acid).Overall,this work offered some important clues and references to reinforce the hydrogen-supplying ability of primary alcohols in the TH of various biomass-derived carbonyl compounds to high-value fine chemicals.展开更多
Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sust...Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sustainable development.Despite significant progress in various electrochemical systems,the regulatory mechanisms of PDE in energy and mass transfer and the lifespan extension of electrolysis systems,particularly in water electrolysis(WE)for hydrogen production,remain insufficiently explored.Therefore,there is an urgent need for a deeper understanding of the unique contributions of PDE in mass transfer enhancement,microenvironment regulation,and hydrogen production optimization,aiming to achieve low-energy consumption,high catalytic activity,and long-term stability in the generation of target products.Here,this review critically examines the microenvironmental effects of PDE on energy and mass transfer,the electrode degradation mechanisms in the lifespan extension of electrolysis systems,and the key factors in enhancing WE for hydrogen production,providing a comprehensive summary of current research progress.The review focuses on the complex regulatory mechanisms of frequency,duty cycle,amplitude,and other factors in hydrogen evolution reaction(HER)performance within PDE strategies,revealing the interrelationships among them.Finally,the potential future directions and challenges for transitioning from laboratory studies to industrial applications are proposed.展开更多
Van der Waals(vdW)heterostructures have attracted much attention due to their distinctive optical,electrical,and thermal properties,demonstrating promising potential in areas such as photocatalysis,ultrafast photonics...Van der Waals(vdW)heterostructures have attracted much attention due to their distinctive optical,electrical,and thermal properties,demonstrating promising potential in areas such as photocatalysis,ultrafast photonics,and free electron radiation devices.Particularly,they are promising platforms for studying thermionic emission.It is illustrated that using vdW heterostructure-based thermionic emission can enhance heat transfer in vacuum devices.As a proof of concept,the approach is demonstrated to offer a promising solution for the long-standing overheating issue in X-ray tubes.Specifically,it is shown that the saturated target temperature of a 2000 W X-ray tube can be reduced from around 1200℃ to 490℃.Additionally,it is also demonstrated that by reducing the height of the Schottky barrier formed in the vdW heterostructures,the thermionic cooling performance can be enhanced.The findings pave the way for the development of high-power X-ray tubes.展开更多
Triclosan(TCS) poses harmful risks to ecosystems and human health owing to its endocrine-disrupting effects.Therefore,developing an efficient and sustainable technology to degrade TCS is urgently needed.Herein,cobalt ...Triclosan(TCS) poses harmful risks to ecosystems and human health owing to its endocrine-disrupting effects.Therefore,developing an efficient and sustainable technology to degrade TCS is urgently needed.Herein,cobalt oxyhydroxide @covalent organic frameworks(CoOOH@COFs) S-scheme heterojunction was synthesized,which combined the visible-light-driven photocatalysis and peroxymonosulfate(PMS) activation to synergistically generate abundant reactive oxygen species(ROSs) for TCS degradation.The degradation efficiency of TCS reached 100 % within 8 min in the Vis-CoOOH@COFs/PMS system,and the reaction rate constant was 0.456 min^(-1),which was nearly 1.90 and 2.85 times that of single Co OOH and COFs,and2.36 times that under dark condition,respectively.The density functional theory(DFT) calculations confirmed the energy band bending of CoOOH@COFs and S-scheme charge transport from COFs to Co OOH.Both experimental and theoretical analyses indicated that Co OOH@COFs in photocatalytic-PMS activation systems synergistically facilitated photo-generated carrier separation,enhanced interfacial electron transfer,accelerated PMS activation,and generated multiple ROSs.In particular,photogenerated electrons(e^(-))accelerated the Co(Ⅲ)/Co(Ⅱ) redox cycle,while the PMS captured the e-,which significantly decreased the charge combination of Co OOH@COFs.Radicals(O_(2)^(·-),^(·)OH,and SO_(4)^(·-)) and non-radicals(such as ^(1)O_(2),h^(+),and e^(-)) were both presented in the Vis-CoOOH@COFs/PMS system,with O_(2)^(-) playing a dominant role in TCS degradation.Furthermore,the pathway of TCS degradation and toxicity of intermediates were explored by DFT calculation and transformation product identification.Importantly,the environmentally friendly CoOOH@COFs S-scheme heterojunction exhibited excellent stability and reusability.In conclusion,this study innovatively designed an S-scheme heterojunction in the photocatalytic-PMS activation system,providing guidance and theoretical support for efficient and eco-friendly wastewater treatment.展开更多
文摘Background: India has scaled up ART programme very rapidly. Though there are reports on retention of patients in the national programme, data on transfer out patients within the ART centers are scanty in India. Methods: This is a retrospective study of patients receiving antiretroviral treatment between January 2006 and July 2013. The patients who were transferred out from the ART center at National AIDS Research Institute in Pune were included in the study. The data on whether they reached the respective ART centers were collected either by making telephonic calls to the patients and/or to the respective ART centers. Results: Of the total 3015 patients ever started on treatment from the ART center, 158 (5.24%) were transferred out to other ART centers. Of these, 123 (77.8%) patients reached other centres and they were “transferred in”. However, 15 (9.5%) did not reach to respective ART centers and information could not be obtained for 20 (12.7%) transferred out patients. The analysis showed that those who were not living with their partners were 4.53 times more likely to not to reach the preferred ART centre after taking transfer [OR, 95% CI: (1.24 - 16.51), p = 0.022]. Conclusion: Our data suggest that significant number of transfer out patients is lost in HIV treatment cascade. Considering the total PLHIV on treatment in the country, this group adds significantly to the burden of lost to follow up patients. It is important to strengthen the system of tracking the transfer out patients in the programme which will help in patching an important leak in the cascade of HIV care.
基金the National Natural Science Fund Project:A Theoretical Study of Renal Reproduction Based on in vitro Fertilization Follicular Fluid Differential Protein-metabolite Global Regulatory Network(No.81874484)。
文摘OBJECTIVE:To investigate the effect of—Xiaoyi Yusi decoction(XYYSD,消异育嗣汤),a Traditional Chinese Medicine(TCM),on in vitro fertilization and embryo transfer(IVF-ET)in patients with endometriosis,and to study the mechanism underpinning the action.METHODS:Women who underwent IVF-ET were divided into three groups by simple randomization:the treatment(n=32;with TCM treatment),patient(n=28;with endometriosis alone),and control(n=33;with male factor alone)groups.The luteal phase short-acting gonadotropin-releasing hormone agonist prolonged protocol was used in all three groups.To compare the changes in TCM scores and reproductive outcomes before and after TCM intervention in patients with endometriosis,partial least-squares discriminant analysis was used to analyze the follicular fluid samples of each group and screen and compare metabolites using the MetaboA nalyst software.RESULTS:The clinical data indicated that following TCM intervention,kidney deficiency and blood stasis symptom patterns improved dramatically in patients with endometriosis and that their clinical pregnancy rate increased significantly(71.9%vs 57.1%,P<0.05).Metabolomics showed that the two groups of samples were separated before and after TCM intervention.After TCM intervention,the intervention group was close to the control group,indicating that the TCM had a certain effect.Pathway analysis revealed that after TCM intervention,the metabolism of glycerin phospholipid,pyruvate,and citric acid was regulated.CONCLUSIONS:Through the pyruvate and glycerophospholipid metabolism pathways and tricarboxylic acid cycle,the TCM XYYSD successfully improved kidney deficiency and blood stasis symptom pattern,as well as the clinical reproductive outcomes of patients with endometriosis-related infertility.
基金Baoding Science and Technology Program Project(Grant No.2241ZF120)Hebei Health Care Commission Scientific Research Funding Project(Grant No.20170827)+1 种基金Funding Project of Affiliated Hospital of Hebei University(Grant No.2016Q016)Funding Project of Affiliated Hospital of Hebei University(No.2022QC66).
文摘Objective:To investigate the effect of abnormal ovarian granulosa cell metabolism on in vitro fertilization and embryo transfer(IVF-ET)outcomes in obese polycystic ovary syndrome(PCOS)patients.Methods:Patients with PCOS who met the study criteria were screened according to the inclusion criteria.A total of 32 patients with obese PCOS were recruited into the study group,and 39 patients with non-obese PCOS were recruited into the control group.The general data(age,body mass index,and years of infertility),insulin resistance index(HOMA-IR),follicle-stimulating hormone(FSH),luteinizing hormone(LH),granulosa cell mitochondrial function,and IVF-ET outcome of patients in the study group and control group were retrospectively analyzed.Results:The differences in age and years of infertility between the study group and the control group were insignificant(P>0.05),and the body mass index(BMI)of the study group and control group was 30.5±1.24 kg/m2 and 22.3±1.12 kg/m2,respectively,in which the difference was statistically significant(P<0.05);the HOMA-IR of the study group was significantly higher than that of the control group(P<0.05);the reactive oxygen species(ROS)in the study group was significantly higher than that in the control group(P<0.05),and the ATP content in the study group was significantly lower than that in the control group(P<0.05);comparing the FSH and LH levels between the two groups,the difference was not statistically significant(P>0.05);the rate of IVF-ET failure was significantly higher in the study group than in the control group.Conclusion:PCOS is a complex endocrine disorder,and obesity is one of the independent risk factors for the development of PCOS.
基金financially supported by National Key Research and Development Programs (Nos.2022YFD1700403 and 2023YFD1700303)National Natural Science Foundation of China (Nos.12274128 and 12250003)+2 种基金Shanghai Rising-Star Program (No.21QA1402600)the support of NYU-ECNU Center for Computational Chemistry at NYU Shanghaithe University of Bath and the Open Research Fund of the School of Chemistry and Chemical Engineering,Henan Normal University (No.2020ZD01) for support。
文摘Fluorescent probes based on intramolecular charge transfer(ICT) have obvious advantages for accurate quantitative analysis.To obtain high-performance ratiometric probes requires distinct photophysical properties during recognition reaction process,which is closely related to their ICT characteristics.1,8-Naphthalimide is known as a typical fluorophore with desirable ICT property when functionalized with an electron-donating moiety at the para-position of the naphthalene chromophore.Although the photophysical properties of para-substituted 1,8-naphthalimide have been well studied,its meta-substituted counterpart has not been fully evaluated since the meta-position is conventionally thought to be weakly conjugated.Herein,combined experimental and theoretical studies are performed which consistently indicate that stronger charge transfer(CT) is exhibited by the meta-amino substituted 1,8-naphthalimide(m-NH_(2)) compared to the para-amino substituted one(p-NH_(2)).The ratiometric response of fluorescence with significant changes in wavelength and intensity upon acetylation(m-NAc and p-NAc) can be attributed to the larger ICT and stronger-NH_(2) vibrations.This observation is further demonstrated by deuterium oxide experiments,viscosity experiments and quantum chemical calculations.The practical application of meta-amino-1,8-naphthalimide ICT-based probes is also confirmed.This research is expected to bring an in-depth understanding of π-conjugated systems with ICT characteristics,and facilitates the design of sensitive ICT fluorescent probes with meta-amino substitution.
基金Natural Science Foundation of Xiamen(3502Z20227342)。
文摘Objective:Advanced maternal age is associated with reduced ovarian reserve and lower oocyte quality.Whether body mass index(BMI)further influences assisted reproductive technology(ART)outcomes in this population remains unclear.Methods:This retrospective study analyzed 222 patients aged≥37 years who underwentin vitro fertilization or intracytoplasmic sperm injection with embryo transfer(IVF/ICSI-ET)at the First Affiliated Hospital of Xiamen University between January 2019 and December 2023.Patients were classified by BMI as underweight(<18.5 kg/m^(2);n=13),normal(18.5-24.9 kg/m^(2);n=154),or overweight(>24.9 kg/m^(2);n=55).Controlled ovarian stimulation protocols were individualized according to ovarian reserve.Laboratory and clinical outcomes were compared across groups,and multivariable logistic regression was used to identify factors associated with clinical pregnancy and live birth.Results:BMI,total gonadotropin dose,and use of IVFvs.ICSI differed among groups(allP<0.05).However,oocyte retrieval rate,metaphase II(MII)oocyte rate,cleavage rate,available embryo rate,high-quality embryo rate,biochemical pregnancy rate,clinical pregnancy rate,live birth rate,and miscarriage rate showed no significant differences(allP>0.05).In multivariable analysis,age,infertility duration,and progesterone level on the day of human chorionic gonadotropin(hCG)trigger were independent predictors of clinical pregnancy.Moreover,age and progesterone level on the hCG day were independently associated predictors of live birth(allP<0.05).Conclusions:Among women aged≥37 years,higher BMI did not significantly affect key laboratory or pregnancy outcomes after IVF/ICSI-ET.Clinical results were mainly influenced by age,infertility duration,and progesterone level on the hCG trigger day.
文摘Objective:To assess whether personalized embryo transfer guided by endometrial receptivity array(ERA)improves implantation and pregnancy rates in women with implantation failure.Methods:This retrospective case-control study was conducted on women with previous implantation failure.The women were divided into two groups,i.e,women who underwent ERA and those who underwent embryo transfer without ERA testing.ERA was performed using Igenomix.ERA results were interpreted as receptive or non-receptive.Women underwent frozen embryo transfer on the 6th day of progesterone(P+5).The primary outcomes were implantation rate,clinical pregnancy rate,abortion rate,and negative pregnancy rate.Results:This study included 229 women with previous implantation failure,with 154 in the ERA group and 75 in the no ERA group.The mean age of the women of the ERA group was(32.2±4.1)years,and that of the no ERA group was(31.5±4.8)years.Women in the ERA group had a higher implantation rate(60.4%)and clinical pregnancy rate(57.1%)compared to those in the no ERA group(48.0%and 46.7%,respectively).In addition,implantation rate of the nonreceptive ERA group was higher than the no ERA group(65%vs.48%),and clinical pregnancy rate was also higher in the non-receptive ERA group than the no ERA group(65%vs.47%).The abortion rate of the no ERA group was 9%and that of the non-receptive ERA group was 10%.52%no ERA group women and 35%non-receptive ERA group women had negative pregnancy results.Conclusions:Women who have undergone personalised embryo transfer guided by ERA have a higher clinical pregnancy rate than women who have not after previous implantation failure.
基金supported by the National Natural Science Foundation of China (22472031,U24A20567,22032002)the 111 Project。
文摘A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,γ-difluoro-and γ-monofluoro-vinylacetic acids without stepwise acidification,exhibiting good functional group tolerance,broad scope,and facile scalability.Mechanism studies support that thiol plays the role of the hydrogen relay,which s a hydrogen atom through HAT and then outputs a proton via PT.This strategy also takes full advantage of formate for photocatalytic carboxylation reaction in a step-and atomeconomical way.
文摘This study investigates the enhancement of convective heat transfer in a serpentine pipe using ferrofluid flow influenced by dual non-uniform magnetic sources.The primary objective is to improve thermal performance in compact cooling systems,such as those used in heat exchangers.A two-dimensional,steady-state Computational Fluid Dynamic(CFD)model is developed in ANSYS Fluent to simulate the behavior of an incompressible ferrofluid under applied constant heat flux and magnetic fields.The magnetic force is modeled using the Kelvin force,which acts on magnetized nanoparticles in response to spatially varying electromagnetic fields generated by two strategically positioned current-carrying wires.The effects of magnetic field strength,quantified by the magnetic number(Mn),on flow behavior and temperature distribution are thoroughly analyzed.The results indicate that increasing Mn leads to higher Nusselt numbers,demonstrating enhanced convective heat transfer.Secondary vortices induced by magnetic forcing improve fluid mixing,particularly in curved regions of the pipe.A mesh-independence study and model validation with benchmark data support the reliability of the numerical framework.This work highlights the potential of magnetic-field-assisted thermal control in energy-efficient cooling applications and provides a foundation for the further development of advanced ferrofluid-based heat transfer systems.
基金supported by National Natural Science Foundation of China (Nos.52170086,22476116,52074176)Natural Science Foundation of Shandong Province (Nos.ZR2021ME013,ZR2024ME156,ZR2022QB250)。
文摘In this study,we meticulously designed a layered carbon-based catalytic material to induce the degradation of a series of organic pollutants by activating peroxymonosulfate(PMS) in the PMS-based advanced oxidation processes(AOPs).Results indicated that the silicon and oxygen elements from the montmorillonite were incorporated into the catalyst matrix to form the Si-O-C structure.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array,achieving over 90 % removal rate of most pollutants within 60 min.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array.The salt bridge system confirmed that pollutants can provide electrons to the Si-O-C/PMS system,and we verified that the electron transfer process(ETP) mechanism was the main pathway for the degradation of pollutants in the Si-O-C/PMS system via the open-circuit potential analysis.In combination with the structural properties of different pollutants,we discovered that electron-donating pollutants can supply more electrons to the Si-O-C/PMS system,thereby enhancing the ETP process.The findings of this study are anticipated to advance the development and practical application of layered carbonaceous materials-based catalysts and support the design and implementation of nanoconfined catalysts in the field of AOPs.
基金National Natural Science Foundation of China (Nos.22071185 and 22271224)the Fundamental Research Funds for the Central Universities (No.2042019kf0008)Wuhan University startup funding for financial support。
文摘The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for synthesizing thioesters primarily rely on the acylation of thiols,which produces substantial waste and requires malodorous,unstable sulfur sources.In this work,we introduce a photocatalyzed hydrogen transfer strategy that enables a three-component synthesis of thioesters using abundant primary alcohols,easily available alkenes and elemental sulfur under mild conditions.This protocol demonstrates broad applicability and high chemo-and regioselectivity for both primary alcohols and alkenes,highlighting the advantage and potential of photo-mediated hydrogen transfer in facilitating multicomponent reactions using primary alcohol and elemental sulfur feedstocks.
基金supported by Shaanxi Fundamental Science Research Project for Chemistry and Biology(23JHQ011)Natural Science Foundation of Shaanxi(2024JC-YBMS-115)Natural Science Basic Research Plan in Shaanxi Province of China(2025JC-YBMS-141)。
文摘The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.
基金supported by the National Natural Science Foundation of China(Grant Nos.42027804,41775026,and 41075012)。
文摘Cirrus clouds play a crucial role in the energy balance of the Earth-atmosphere system.We investigated the spatiotemporal variations of cirrus over the South China Sea(SCS)using satellite data(MOD08,MYD08,CALIPSO)and reanalysis data(MERRA-2)from March 2007 to February 2015(eight years).The horizontal distribution reveals lower cirrus fraction values in the northern SCS and higher values in the southern region,with minima observed in March and April and maxima sequentially occurring in August(northern SCS,NSCS),September(middle SCS,MSCS),and December(southern SCS,SSCS).Vertically,the cirrus fraction peaks in summer and reaches its lowest levels in spring.Opaque cirrus dominates during summer in the NSCS and MSCS,comprising 53.6%and 55.9%,respectively,while the SSCS exhibits a higher frequency of opaque cirrus relative to other cloud types.Subvisible cirrus clouds have the lowest frequency year-round,whereas thin cirrus is most prominent in winter in the NSCS(46.3%)and in spring in the MSCS(45.3%).A case study from September 2021 further explores the influence of ice crystal habits on brightness temperature(BT)over the SCS.Simulations utilizing five ice crystal shapes from the ARTS DDA(Atmospheric Radiative Transfer Simulator Discrete Dipole Approximation)database and the RTTOV 12.4 radiative transfer model reveal that the 8-column-aggregate shape best represents BT in the NSCS and SSCS,while the large-block-aggregate shape performs better in the SSCS.
文摘In recent years,with the rapid advancement of artificial intelligence,object detection algorithms have made significant strides in accuracy and computational efficiency.Notably,research and applications of Anchor-Free models have opened new avenues for real-time target detection in optical remote sensing images(ORSIs).However,in the realmof adversarial attacks,developing adversarial techniques tailored to Anchor-Freemodels remains challenging.Adversarial examples generated based on Anchor-Based models often exhibit poor transferability to these new model architectures.Furthermore,the growing diversity of Anchor-Free models poses additional hurdles to achieving robust transferability of adversarial attacks.This study presents an improved cross-conv-block feature fusion You Only Look Once(YOLO)architecture,meticulously engineered to facilitate the extraction ofmore comprehensive semantic features during the backpropagation process.To address the asymmetry between densely distributed objects in ORSIs and the corresponding detector outputs,a novel dense bounding box attack strategy is proposed.This approach leverages dense target bounding boxes loss in the calculation of adversarial loss functions.Furthermore,by integrating translation-invariant(TI)and momentum-iteration(MI)adversarial methodologies,the proposed framework significantly improves the transferability of adversarial attacks.Experimental results demonstrate that our method achieves superior adversarial attack performance,with adversarial transferability rates(ATR)of 67.53%on the NWPU VHR-10 dataset and 90.71%on the HRSC2016 dataset.Compared to ensemble adversarial attack and cascaded adversarial attack approaches,our method generates adversarial examples in an average of 0.64 s,representing an approximately 14.5%improvement in efficiency under equivalent conditions.
基金supported by the National Natural Science Foundation of China(22434007,22104021,52303075,22404102)the Taishan Young Scholar Program of Shandong Province(tsqnz20231235)+2 种基金the Natural Science Foundation of Shandong Province(ZR2024QB338,ZR2023QB227)the Higher Education Institutions Youth Innovation Team Plan of Shandong Province(2024KJH046)the Shandong Postdoctora1 Science Foundation(SDCX-ZG-202400279)。
文摘Air-permeable and ultrathin conductive electrodes are essential for next-generation soft electronics,including breathable wearables,on-skin devices and biointegrated electronics.However,conventional metallization strategies,such as sputtering and ink-printing,often suffer from severe vertical charge leakage due to the porous and ultrathin characteristics of nanofibrous networks,leading to device short-circuiting,operational failure and limited vertical integration.Here,we present a solvent-selective dissolutionassisted transfer printing strategy to achieve surface-confined metallization of ultrathin,lightweight,and gas-permeable nanofibrous networks,enabling lateral conductivity while maintaining vertical insulation.This transfer printing process facilitates not only the rapid formation of conductive patterns on the surface of nanofibrous networks but also mechanical reinforcement through solvent evaporation-induced interlocked fiber-fiber welding.Meanwhile,the strategy preserves the high permeability of the nanofibrous networks and imparts a unique combination of surface conductivity(2Ωcm)and vertical insulativity(10^(11)Ωcm).The resulting anisotropic conductive networks enable low-voltage wearable heaters,high-sensitive pressure sensors,and ultralight temperature sensors.A pressure-temperature dual-modal sensing patch is further fabricated for intelligent grasping classification.The proposed surface-confined metallization strategy enables rapid fabrication of an anisotropic conductive network as a building block to construct air-permeable,ultrathin and lightweight wearable electronics.
文摘Accurate assessment of seismic landslide susceptibility is crucial for disaster prevention and emergency decision-making.Although machine learning methods have been widely applied in this field,they exhibit a strong dependence on large quantities of highquality samples,resulting in significantly low prediction accuracy of existing studies under data-scarce or crossregional prediction scenarios,which fail to meet practical application requirements.To address this issue,this study proposes an intelligent prediction model integrating transfer learning and a sampling optimization strategy,aiming to enhance the accuracy and applicability of seismic landslide susceptibility assessment.The model first improves the sample collection method through the sampling optimization strategy to enhance the precision and representativeness of training samples.This not only ensures the accuracy of origin area training but also further strengthens the model's predictive ability in the target area.Subsequently,it incorporates Transfer Component Analysis(TCA)to overcome the differences in environmental characteristics between the origin area and target area,and couples TCA with the Light GBM algorithm to construct the TCA-Light GBM model,realizing the assessment of seismic landslide susceptibility in sample-free areas.Validated through case studies of the Jiuzhaigou and Luding earthquakes,the results demonstrate that the proposed TCALight GBM transfer learning method exhibits excellent applicability in seismic landslide susceptibility prediction.After optimization with the TCA algorithm,the model's prediction performance in the target domain is significantly improved,with the AUC value increasing from 0.719 to 0.827,representing an increase of approximately 15.02%.This indicates that TCA technology can effectively alleviate the feature distribution discrepancy between the source domain and target domain,enhancing the model's generalization ability.The method is particularly suitable for scenarios with data scarcity and cross-regional prediction and can provide reliable technical support for the emergency response and risk prevention and control of seismic hazards.
基金financially supported by the National Natural Science Foundation of China (Nos.22171165 and 22371170)Natural Science Foundation of Shandong Province (No.ZR2022MB080)Scientific and Technological Frontiers in Project of Henan Province(No.242102110192)。
文摘Co-assembling chiral molecules with achiral compounds via non-covalent interactions like areneperfluoroarene(AP) interactions offers an effective approach for fabricating chiral functional materials.Herein,chiral molecules L/D-PF1 and L/D-PF2 with pyrene groups were synthesized and its chiroptical properties upon co-assembly with achiral compound octafluoronaphthalene(OFN) through AP interaction were systemically studied.The co-assembly of L/D-PF1/OFN and L/D-PF2/OFN exhibited distinct chiroptical properties such as circular dichroism(CD) and circularly polarized luminescence(CPL) signals.Chirality transfer from the chirality center of L/D-PF1 and L/D-PF2 to the achiral OFN and chiral amplification were successfully achieved.Besides,no significant CPL signal was observed in the self-assembly of L/DPF1 or L/D-PF2 while co-assembly with OFN exhibited obvious CPL amplification induced by AP interaction.Notably,a reversal CD signal and CPL signal could be observed in L/D-PF2/OFN when the molar ratio changed from 1:1 to 1:2 while not found in L/D-PF1/OFN,indicating that that minor structural changes of molecules could cause large changes in assembly.In addition,a series of computational calculations were conducted to verify the AP interaction between L-PF1/L-PF2 and OFN.This work demonstrated that arene-perfluoroarene interaction could drive chiral transfer,chiral amplification and chiral inversion and provided a new method for the preparation of chiroptical materials.
基金financially supported by the National Natural Science Foundation of China(U22A20421)the Qinglan Project of Jiangsu Province,the 533 Talent Program of Huaian City,and the College Students’Innovative Entrepreneurial Training Plan Program of Jiangsu Province(X202510323027).
文摘Endogenous hydrogen systems,consisting of metal–organic coordination catalysts and alcohols,have been widely applied for the transfer hydrogenation(TH)of biomass-derived carbonyl compounds in recent years.Metal-organic coordination catalysts showed satisfactory ability of TH in the secondary alcohols,but most of them could not effectively employ the cheaper primary alcohols as hydrogen donors.Furthermore,they commonly contained high metal contents,which also led to low catalytic efficiency in significant measure.In this work,we constructed a novel magnesium single-atom catalyst(Mg-NC)with merely 0.37 wt%Mg by means of a combined self-assembly and pyrolysis strategy.The characterization results indicated that Mg was atomically dispersed and it was coordinated with four pyridinic-N in Mg-NC.Due to the obvious electron transfer from Mg to its coordinated pyridinic-N,Mg–N_(4)active centers displayed high Lewis acid-base strength with abundant content,which brought remarkable catalytic activity.When Mg-NC was used for the TH of 5-hydroxymethylfurfural(HMF)in ethanol(EtOH),2,5-bis(hydroxymethyl)furan(BHMF)yield was up to 96.3%with high productivity of 19.85 molBHMF mol_(Mg)^(−1)h^(−1)at 150°C for 5 h.More interestingly,the process of TH over Mg-NC in EtOH was proved to proceed via the hydrogen radical mechanism.Additionally,Mg-NC exhibited powerful catalytic universality;it could not only utilize other primary alcohols(such as n-propanol and n-butanol)as hydrogen donors,but also catalyze the TH of other carbonyl compounds(such as furfural,5-methylfurfural,benzaldehyde,cyclohexanone,and levulinic acid).Overall,this work offered some important clues and references to reinforce the hydrogen-supplying ability of primary alcohols in the TH of various biomass-derived carbonyl compounds to high-value fine chemicals.
基金financially supported by the Key Research and Development Program of Heilongjiang Province(No.2024ZXJ03C06)National Natural Science Foundation of China(No.52476192,No.52106237)+1 种基金Natural Science Foundation of Heilongjiang Province(No.YQ2022E027)Technology Project of China Datang Technology Innovation Co.,Ltd(No.DTKC-2024-20610).
文摘Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sustainable development.Despite significant progress in various electrochemical systems,the regulatory mechanisms of PDE in energy and mass transfer and the lifespan extension of electrolysis systems,particularly in water electrolysis(WE)for hydrogen production,remain insufficiently explored.Therefore,there is an urgent need for a deeper understanding of the unique contributions of PDE in mass transfer enhancement,microenvironment regulation,and hydrogen production optimization,aiming to achieve low-energy consumption,high catalytic activity,and long-term stability in the generation of target products.Here,this review critically examines the microenvironmental effects of PDE on energy and mass transfer,the electrode degradation mechanisms in the lifespan extension of electrolysis systems,and the key factors in enhancing WE for hydrogen production,providing a comprehensive summary of current research progress.The review focuses on the complex regulatory mechanisms of frequency,duty cycle,amplitude,and other factors in hydrogen evolution reaction(HER)performance within PDE strategies,revealing the interrelationships among them.Finally,the potential future directions and challenges for transitioning from laboratory studies to industrial applications are proposed.
基金supported by National Natural Science Foundation of China(61921002 and 92163204)。
文摘Van der Waals(vdW)heterostructures have attracted much attention due to their distinctive optical,electrical,and thermal properties,demonstrating promising potential in areas such as photocatalysis,ultrafast photonics,and free electron radiation devices.Particularly,they are promising platforms for studying thermionic emission.It is illustrated that using vdW heterostructure-based thermionic emission can enhance heat transfer in vacuum devices.As a proof of concept,the approach is demonstrated to offer a promising solution for the long-standing overheating issue in X-ray tubes.Specifically,it is shown that the saturated target temperature of a 2000 W X-ray tube can be reduced from around 1200℃ to 490℃.Additionally,it is also demonstrated that by reducing the height of the Schottky barrier formed in the vdW heterostructures,the thermionic cooling performance can be enhanced.The findings pave the way for the development of high-power X-ray tubes.
文摘Triclosan(TCS) poses harmful risks to ecosystems and human health owing to its endocrine-disrupting effects.Therefore,developing an efficient and sustainable technology to degrade TCS is urgently needed.Herein,cobalt oxyhydroxide @covalent organic frameworks(CoOOH@COFs) S-scheme heterojunction was synthesized,which combined the visible-light-driven photocatalysis and peroxymonosulfate(PMS) activation to synergistically generate abundant reactive oxygen species(ROSs) for TCS degradation.The degradation efficiency of TCS reached 100 % within 8 min in the Vis-CoOOH@COFs/PMS system,and the reaction rate constant was 0.456 min^(-1),which was nearly 1.90 and 2.85 times that of single Co OOH and COFs,and2.36 times that under dark condition,respectively.The density functional theory(DFT) calculations confirmed the energy band bending of CoOOH@COFs and S-scheme charge transport from COFs to Co OOH.Both experimental and theoretical analyses indicated that Co OOH@COFs in photocatalytic-PMS activation systems synergistically facilitated photo-generated carrier separation,enhanced interfacial electron transfer,accelerated PMS activation,and generated multiple ROSs.In particular,photogenerated electrons(e^(-))accelerated the Co(Ⅲ)/Co(Ⅱ) redox cycle,while the PMS captured the e-,which significantly decreased the charge combination of Co OOH@COFs.Radicals(O_(2)^(·-),^(·)OH,and SO_(4)^(·-)) and non-radicals(such as ^(1)O_(2),h^(+),and e^(-)) were both presented in the Vis-CoOOH@COFs/PMS system,with O_(2)^(-) playing a dominant role in TCS degradation.Furthermore,the pathway of TCS degradation and toxicity of intermediates were explored by DFT calculation and transformation product identification.Importantly,the environmentally friendly CoOOH@COFs S-scheme heterojunction exhibited excellent stability and reusability.In conclusion,this study innovatively designed an S-scheme heterojunction in the photocatalytic-PMS activation system,providing guidance and theoretical support for efficient and eco-friendly wastewater treatment.