The aerosolization and diffusion of radioactive materials caused by chemical explosions represent a typical nuclear accident scenario that poses severe radioactive hazards to human health and the environment.This stud...The aerosolization and diffusion of radioactive materials caused by chemical explosions represent a typical nuclear accident scenario that poses severe radioactive hazards to human health and the environment.This study examines the diffusion of plutonium aerosol generated by a chemical explosion within a typical representative underground facility.The state of explosion products following a single-point detonation of explosives was simulated.Subsequently,a numerical simulation of plutonium aerosol diffusion using the discrete phase model(DPM)was conducted based on the outcomes of the chemical explosion simulation.The simulation results indicate that plutonium aerosols diffuse throughout underground facilities after a chemical explosion;small particle size aerosols primarily accumulate in the upper part of the room after the accident;the concentrations of plutonium aerosol in the room and tunnel are significantly higher than those in the other areas;and the temporal variations in aerosol concentration in each area were quantified.Based on the particle concentration distribution and the effective dose computation approach,the study computes the internal irradiation dose received by personnel in seven areas over various time periods post-accident.Recommendations for emergency decision-making were derived from these calculations.These findings provide important theoretical insight and practical engineering application value for understanding the diffusion of radioactive aerosol in confined spaces following chemical explosions and for evaluating personnel radiation dose.展开更多
Methanol steam reforming(MSR)represents a promising route for hydrogen production,leveraging the high energy density and liquid-phase storage advantages of methanol.Copper-based catalysts have become indispensable for...Methanol steam reforming(MSR)represents a promising route for hydrogen production,leveraging the high energy density and liquid-phase storage advantages of methanol.Copper-based catalysts have become indispensable for MSR due to their cost-effectiveness,exceptional catalytic activity,and tunable selectivity.However,persistent challenges such as thermal sintering,undesirable CO byproduct formation,diminished low-temperature reactivity,and long-term catalyst deactivation limit their broad industrial deployment.This review comprehensively examines the mechanistic pathways of MSR over Cu-based catalysts,with particular focus on differentiating catalyst formulations optimized for high-temperature(>200°C)versus low-temperature(<200°C)operation.It highlights the decisive influence of Cu nanoparticle size,electronic structure,and crystal structure on catalytic performance.Cutting-edge design strategies,including multi-element engineering,innovative synthesis techniques,and deactivation mitigation,are critically evaluated to elucidate mechanistic connections between atomic-scale structure and catalytic performance enhancement.Finally,industrial applications of commercial Cu/ZnO/Al_(2)O_(3)variants and their scalability challenges are discussed,alongside prospective strategies for catalyst innovation and engineering to advance next-generation hydrogen production.展开更多
Extreme cold weather seriously harms human thermoregulatory system,necessitating high-performance insulating garments to maintain body temperature.However,as the core insulating layer,advanced fibrous materials always...Extreme cold weather seriously harms human thermoregulatory system,necessitating high-performance insulating garments to maintain body temperature.However,as the core insulating layer,advanced fibrous materials always struggle to balance mechanical properties and thermal insulation,resulting in their inability to meet the demands for both washing resistance and personal protection.Herein,inspired by the natural spring-like structures of cucumber tendrils,a superelastic and washable micro/nanofibrous sponge(MNFS)based on biomimetic helical fibers is directly prepared utilizing multiple-jet electrospinning technology for high-performance thermal insulation.By regulating the conductivity of polyvinylidene fluoride solution,multiple-jet ejection and multiple-stage whipping of jets are achieved,and further control of phase separation rates enables the rapid solidification of jets to form spring-like helical fibers,which are directly entangled to assemble MNFS.The resulting MNFS exhibits superelasticity that can withstand large tensile strain(200%),1000 cyclic tensile or compression deformations,and retain good resilience even in liquid nitrogen(-196℃).Furthermore,the MNFS shows efficient thermal insulation with low thermal conductivity(24.85 mW m^(-1)K^(-1)),close to the value of dry air,and remains structural stability even after cyclic washing.This work offers new possibilities for advanced fibrous sponges in transportation,environmental,and energy applications.展开更多
Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surf...Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surface wettability,insufficient interfacial contact,and unfavorable energy level alignment at the PTAA/perovskite interface.Here,we report a highly effective interfacial engineering strategy employing the ionic liquid 1,3-dimethylimidazolium dimethyl phosphate(DMIMPH)as a multifunctional interfacial modifier.The incorporation of DMIMPH improves PTAA wettability,promoting the growth of high-quality perovskite films with enhanced interfacial contact.Concurrently,DMIMPH effectively tunes the energy levels of PTAA,enhances its electrical conductivity,and passivates interfacial defects with more efficient hole extraction and charge transport.Moreover,its interaction with residual PbI_(2) modulates perovskite crystallization kinetics,yielding highly crystalline perovskite films with enlarged grain sizes,reduced PbI_(2) residue,and suppressed trap densities.As a result,PTAA-based p-i-n PSCs employing this approach achieve a record certified power conversion efficiency(PCE)of 24.52%,with a champion efficiency of 25.12%—the highest certified value for PTAA-based perovskite devices to date.Impressively,the DMIMPH-modified PSCs without encapsulation maintained 87.48%of their initial efficiency after 1600 h in air.This strategy offers an effective pathway for advancing the performance and stability of polymer-based inverted PSCs.展开更多
The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects,radiative transfer,and microphysical processes.However,previous studies have been mostly concerned with clouds,with...The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects,radiative transfer,and microphysical processes.However,previous studies have been mostly concerned with clouds,with limited studies on fog,particularly those that examine the combined influences of all key physical processes and their roles during fog evolution.As such,this study aims to conduct a comprehensive investigation by examining the relationships between relative dispersion and other microphysical variables,as well as the underlying microphysical and dynamic processes,based on field fog campaigns in polluted and clean conditions.In polluted fog,droplet concentrations are higher,leading to smaller droplets and increased dispersion.The correlation between dispersion and droplet volume-mean radius is positive in the polluted fog,but shifts to negative in clean fog.We attribute the difference to various microphysical processes like aerosol activation,condensation,collision-coalescence,and entrainment-mixing.In polluted fog,high aerosol concentrations,low supersaturations,and strong turbulence(entrainment-mixing)provide suitable conditions for the simultaneous occurrence of droplet condensation and aerosol activation,resulting in a positive correlation between dispersion and volume-mean radius,especially during the fog formation stage.In contrast,during the mature stage in clean fog,condensation is dominant with weak aerosol activation leading to a negative correlation between relative dispersion and volume-mean radius.The collision-coalescence process is more active in the mature stage,increasing radii and leading to the negative correlation between dispersion and volume-mean radius.This result sheds new light on understanding the relative dispersion and mechanisms in fog under different aerosol backgrounds.展开更多
Biochar and zero-valent iron are promising materials for the removal of trichloroethylene(TCE)from groundwater,but further research is still required on the synergistic mechanism and hydraulic performance in the perme...Biochar and zero-valent iron are promising materials for the removal of trichloroethylene(TCE)from groundwater,but further research is still required on the synergistic mechanism and hydraulic performance in the permeable reactive barriers(PRBs)with biochar-iron composites.In this work,biochar-iron composites were synthesized by two different methods,and subjected to the microscopic analysis,batch experiments and the PRB’s model tests.The results indicated that the removal rates of TCE on biochar-iron composites reached above 90%,and the optimal removal conditions were the initial pH of 6.0 and a biochar/iron mass ratio of 5:1.The removal of TCE on biochar-iron composites followed the pseudo-second-order and Freundlich models,and the maximum adsorption capacity of TCE was 25.95 mg/g.The adsorption of biochar and dechlorination of nZVI dominated the removal of TCE.Biochar significantly enhanced the dechlorination of TCE on nZVI through modifying the electrochemical characteristics to lower its corrosion potential of nZVI,promote direct electron transfer,and improve electronic transfer capability.M-5BC-1nZVI exhibited excellent hydraulic performance for maintaining an adequate permeability coefficient(10^(−6)to 10^(−5)m/s).展开更多
During geothermal resource exploitation,the potential deterioration of mechanical properties in high-temperature granite subjected to cooling poses a significant safety concern.To address this,the present study invest...During geothermal resource exploitation,the potential deterioration of mechanical properties in high-temperature granite subjected to cooling poses a significant safety concern.To address this,the present study investigates the coupled thermo-mechanical behavior of granite during heating and cooling through a combination of laboratory tests and finite difference method analysis.Initial investigations involve X-ray diffraction,thermal expansion test,thermogravimetric analysis,and uniaxial compression test.Results show the significant variations of granite properties under different thermal conditions,attributed to temperature gradients,water evaporation,and mineral phase transitions.Subsequently,a model considering temperature-dependent parameters and real-time cooling rates was employed to simulate linear heating and nonlinear cooling processes.Simulation results indicate that the thermal cracking predominantly occurs during the heating stage,with tensile failure as the primary mode.Additionally,a faster real-time cooling rate at higher temperatures intensifies the thermal cracking behavior in granite.This study effectively elucidates the thermomechanical coupling behavior of granite during heating and cooling processes,providing insights into the mechanisms of mechanical property changes with rising or decreasing temperatures.展开更多
Background:Immune-mediated inflammatory disease(IMID)and cancer share underlying mechanisms.We aimed to comprehensively evaluate the associations between IMIDs and cancers from global,population and genetic perspectiv...Background:Immune-mediated inflammatory disease(IMID)and cancer share underlying mechanisms.We aimed to comprehensively evaluate the associations between IMIDs and cancers from global,population and genetic perspectives.Methods:A triangulation framework was employed to assess the association between IMIDs and cancers,using the Global Burden of Disease Study(2012-2021)to analyse six IMIDs and 33 cancers.The UK Biobank(UKBB)prospective cohort was subsequently used to validate these associations,with hazard ratios(HRs)and 95%confidence intervals(CIs)estimated by Cox proportional hazards models.Causal inference based on genetic instruments was performed in the FinnGen and UKBB to assess the potential causal effects between IMIDs and cancers.Results:IMIDs were positively associated with the occurrence of cancers from a global perspective.Moreover,170 specific IMID-cancer pairs revealed statistically significant associations.A total of 20 pairs of specific IMID-cancer associations were further confirmed in the UKBB cohort.Among these,the five most pronounced associations included atopic dermatitis with Hodgkin lymphoma(HR=12.56,95%CI:1.76-89.59),with ovarian cancer(HR=5.65,95%CI:1.41-22.65)and with non-Hodgkin lymphoma(HR=5.11,95%CI:1.91-13.63);rheumatoid arthritis with Hodgkin lymphoma(HR=3.85,95%CI:1.11-13.32);and psoriasis with Hodgkin lymphoma(HR=3.43,95%CI:1.69-6.96).Additionally,a positive causal association between rheumatoid arthritis and Hodgkin lymphoma(inverse variance weighted OR=1.31,95%CI:1.10-1.57)was observed.Conclusions:This study provides comprehensive evidence of the relationships between IMIDs and cancers from global,population and genetic perspectives and identifies 20 pairs of specific IMID-cancer associations,thereby contributing to advancements in cancer prevention and control.展开更多
The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective ...The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner.In this review,we investigate the development of industrialwaste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste.We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification,in which the active components,pore size,and phase structure can be altered.The review will discuss the potential of using industrial solid wastes,these modified materials,or synthesized materials from raw waste precursors for the removal of air pollutants,including SO_(2),NO_(x),Hg^(0),H_(2)S,VOCs,and CO_(2).The challenges still need to be addressed to realize this potential and the prospects for future research fully.The suggestions for future directions include determining the optimal composition of these materials,calculating the real reaction rate and turnover frequency,developing effective treatment methods,and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.展开更多
Single-pixel imaging(SPI)enables efficient sensing in challenging conditions.However,the requirement for numerous samplings constrains its practicality.We address the challenge of high-quality SPI reconstruction at ul...Single-pixel imaging(SPI)enables efficient sensing in challenging conditions.However,the requirement for numerous samplings constrains its practicality.We address the challenge of high-quality SPI reconstruction at ultra-low sampling rates.We develop an alternative optimization with physics and a data-driven diffusion network(APD-Net).It features alternative optimization driven by the learned task-agnostic natural image prior and the task-specific physics prior.During the training stage,APD-Net harnesses the power of diffusion models to capture data-driven statistics of natural signals.In the inference stage,the physics prior is introduced as corrective guidance to ensure consistency between the physics imaging model and the natural image probability distribution.Through alternative optimization,APD-Net reconstructs data-efficient,high-fidelity images that are statistically and physically compliant.To accelerate reconstruction,initializing images with the inverse SPI physical model reduces the need for reconstruction inference from 100 to 30 steps.Through both numerical simulations and real prototype experiments,APD-Net achieves high-quality,full-color reconstructions of complex natural images at a low sampling rate of 1%.In addition,APD-Net’s tuning-free nature ensures robustness across various imaging setups and sampling rates.Our research offers a broadly applicable approach for various applications,including but not limited to medical imaging and industrial inspection.展开更多
Aqueous Zn-ion batteries(AZIBs)have been regarded as promising alternatives to Li-ion batteries due to their advantages,such as low cost,high safety,and environmental friendliness.However,AZIBs face significant challe...Aqueous Zn-ion batteries(AZIBs)have been regarded as promising alternatives to Li-ion batteries due to their advantages,such as low cost,high safety,and environmental friendliness.However,AZIBs face significant challenges in limited stability and lifetime owing to zinc dendrite growth and serious side reactions caused by water molecules in the aqueous electrolyte during cycling.To address these issues,a new eutectic electrolyte based on Zn(ClO_(4))_(2)·6H_(2)O-N-methylacetamide(ZN)is proposed in this work.Compared with aqueous electrolyte,the ZN eutectic electrolyte containing organic N-methylacetamide could regulate the solvated structure of Zn^(2+),effectively suppressing zinc dendrite growth and side reactions.As a result,the Zn//NH4 V4 O10 full cell with the eutectic ZN-1-3 electrolyte demonstrates significantly enhanced cycling stability after 1000 cycles at 1 A g^(-1).Therefore,this study not only presents a new eutectic electrolyte for zinc-ion batteries but also provides a deep understanding of the influence of Zn^(2+)solvation structure on the cycle stability,contributing to the exploration of novel electrolytes for high-performance AZIBs.展开更多
Dear Editor,This letter focuses on the fact that small objects with few pixels disappear in feature maps with large receptive fields, as the network deepens, in object detection tasks. Therefore, the detection of dens...Dear Editor,This letter focuses on the fact that small objects with few pixels disappear in feature maps with large receptive fields, as the network deepens, in object detection tasks. Therefore, the detection of dense small objects is challenging.展开更多
Sonodynamic therapy(SDT)as an emerging modality for malignant tumors mainly involves in sonosensitizers and low-intensity ultrasound(US),which can safely penetrate the tissue without significant attenuation.SDT not on...Sonodynamic therapy(SDT)as an emerging modality for malignant tumors mainly involves in sonosensitizers and low-intensity ultrasound(US),which can safely penetrate the tissue without significant attenuation.SDT not only has the advantages including high precision,non-invasiveness,and minimal side effects,but also overcomes the limitation of low penetration of light to deep tumors.The cytotoxic reactive oxygen species can be produced by the utilization of sonosensitizers combined with US and kill tumor cells.However,the underlying mechanism of SDT has not been elucidated,and its unsatisfactory efficiency retards its further clinical application.Herein,we shed light on the main mechanisms of SDT and the types of sonosensitizers,including organic sonosensitizers and inorganic sonosensitizers.Due to the development of nanotechnology,many novel nanoplatforms are utilized in this arisen field to solve the barriers of sonosensitizers and enable continuous innovation.This review also highlights the potential advantages of nanosonosensitizers and focus on the enhanced efficiency of SDT based on nanosonosensitizers with monotherapy or synergistic therapy for deep tumors that are difficult to reach by traditional treatment,especially orthotopic cancers.展开更多
Drug-eluting magnesium(Mg)alloy stents have a slower degradation rate and lower restenosis rate compared with uncoated stents,demonstrating good clinical efficacy.However,the release of anti-hyperplasia drugs from coa...Drug-eluting magnesium(Mg)alloy stents have a slower degradation rate and lower restenosis rate compared with uncoated stents,demonstrating good clinical efficacy.However,the release of anti-hyperplasia drugs from coatings delays endothelial tissue repair,thus leading to late stent thrombosis.To address these issues,a dual self-healed coating with various biological properties was fabricated on magnesium fluoride/polydopamine(MgF_(2)/PDA)-treated Mg alloys by spraying-assisted layer-by-layer(LBL)self-assembly of chitosan(CS),gallic acid(GA),and 3-aminobenzeneboronic acid-modified hyaluronic acid(HA-ABBA).The LBL coating,approximately 1.50μm thick,exhibited a uniform morphology with good adhesion strength(~1065 mN).The annual corrosion rate(Pi)of LBL samples was~1400 times slower than that of the Mg substrate,due to the physical barrier function provided by MgF_(2)/PDA layers and the dual self-healed ability of LBL layers.The rapid self-healing ability(with a healing period of~4 h under dynamic/static conditions)resulted from the synergistic interplay between the recombination of diverse chemical bonds within the LBL coating and the coordination of LBL-released GA with Mg2+,as corroborated by computer simulations.Compared with the drug-eluting coatings,the LBL sample demonstrated substantial advantages in anti-oxidation,anti-denaturation of fibrinogen,anti-platelet adhesion,anti-inflammation,anti-hyperplasia,and promoted-endothelialization.These benefits effectively address the limitations associated with drug-eluting coatings.展开更多
Herein,a series of manganese oxide catalysts with different valences(Mn_(3)O_(4),Mn_(2)O_(3),and MnO_(2))were designed and synthesized for the synthesis of ethylene urea(EU)from ethylenediamine(EDA)and carbon dioxide(...Herein,a series of manganese oxide catalysts with different valences(Mn_(3)O_(4),Mn_(2)O_(3),and MnO_(2))were designed and synthesized for the synthesis of ethylene urea(EU)from ethylenediamine(EDA)and carbon dioxide(CO_(2)).With a maximal EDA conversion of 82%and EU selectivity of 99%at 160℃ for 2 h,Mn_(2)O_(3) catalysts had the best catalytic activity among them,which was superior to the reported catalysts.In the following order:Mn_(2)O_(3)>MnO_(2)>Mn_(3)O_(4),the catalytic activity for the synthesis of EU from CO_(2) and EDA decreased.Further characterization showed the Mn_(2)O_(3) catalyst possessed a greater Mn^(3+)/Mn4+ratio and more surface oxygen vacancies than the MnO_(2) and Mn_(3)O_(4),which improved its capacity to adsorb and activate CO_(2) and EDA.After four recycling runs,the EDA conversion slightly declined from 82%to 56%on Mn_(2)O_(3) catalyst,while no obvious change in EU selectivity was observed.The loss of surface Ov contents and Mn^(3+)proportion were concluded as main reasons for the decrease in catalytic activity over Mn_(2)O_(3) catalyst.This work demonstrated a metal oxide catalyst that was efficient in producing EU from CO_(2) and EDA.展开更多
文摘The aerosolization and diffusion of radioactive materials caused by chemical explosions represent a typical nuclear accident scenario that poses severe radioactive hazards to human health and the environment.This study examines the diffusion of plutonium aerosol generated by a chemical explosion within a typical representative underground facility.The state of explosion products following a single-point detonation of explosives was simulated.Subsequently,a numerical simulation of plutonium aerosol diffusion using the discrete phase model(DPM)was conducted based on the outcomes of the chemical explosion simulation.The simulation results indicate that plutonium aerosols diffuse throughout underground facilities after a chemical explosion;small particle size aerosols primarily accumulate in the upper part of the room after the accident;the concentrations of plutonium aerosol in the room and tunnel are significantly higher than those in the other areas;and the temporal variations in aerosol concentration in each area were quantified.Based on the particle concentration distribution and the effective dose computation approach,the study computes the internal irradiation dose received by personnel in seven areas over various time periods post-accident.Recommendations for emergency decision-making were derived from these calculations.These findings provide important theoretical insight and practical engineering application value for understanding the diffusion of radioactive aerosol in confined spaces following chemical explosions and for evaluating personnel radiation dose.
基金supported by the National Natural Science Foundation of China(No.22208374)the Excellent Youth Scientist Award Foundation of Shandong Province(No.ZR2024YQ009)+2 种基金the Distinguished Young Scholars of the National Natural Science Foundation of China(No.22322814)CNPC Innovation Found(2022DQ02-0607)the Fundamental Research Funds for the Central Universities(No.24CX07006A).
文摘Methanol steam reforming(MSR)represents a promising route for hydrogen production,leveraging the high energy density and liquid-phase storage advantages of methanol.Copper-based catalysts have become indispensable for MSR due to their cost-effectiveness,exceptional catalytic activity,and tunable selectivity.However,persistent challenges such as thermal sintering,undesirable CO byproduct formation,diminished low-temperature reactivity,and long-term catalyst deactivation limit their broad industrial deployment.This review comprehensively examines the mechanistic pathways of MSR over Cu-based catalysts,with particular focus on differentiating catalyst formulations optimized for high-temperature(>200°C)versus low-temperature(<200°C)operation.It highlights the decisive influence of Cu nanoparticle size,electronic structure,and crystal structure on catalytic performance.Cutting-edge design strategies,including multi-element engineering,innovative synthesis techniques,and deactivation mitigation,are critically evaluated to elucidate mechanistic connections between atomic-scale structure and catalytic performance enhancement.Finally,industrial applications of commercial Cu/ZnO/Al_(2)O_(3)variants and their scalability challenges are discussed,alongside prospective strategies for catalyst innovation and engineering to advance next-generation hydrogen production.
基金supported by Young Elite Scientists Sponsorship Program by China Association for Science and Technology(No.2022QNRC001)the National Natural Science Foundation of China(No.52273053)the Chenguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission(No.21CGA41)。
文摘Extreme cold weather seriously harms human thermoregulatory system,necessitating high-performance insulating garments to maintain body temperature.However,as the core insulating layer,advanced fibrous materials always struggle to balance mechanical properties and thermal insulation,resulting in their inability to meet the demands for both washing resistance and personal protection.Herein,inspired by the natural spring-like structures of cucumber tendrils,a superelastic and washable micro/nanofibrous sponge(MNFS)based on biomimetic helical fibers is directly prepared utilizing multiple-jet electrospinning technology for high-performance thermal insulation.By regulating the conductivity of polyvinylidene fluoride solution,multiple-jet ejection and multiple-stage whipping of jets are achieved,and further control of phase separation rates enables the rapid solidification of jets to form spring-like helical fibers,which are directly entangled to assemble MNFS.The resulting MNFS exhibits superelasticity that can withstand large tensile strain(200%),1000 cyclic tensile or compression deformations,and retain good resilience even in liquid nitrogen(-196℃).Furthermore,the MNFS shows efficient thermal insulation with low thermal conductivity(24.85 mW m^(-1)K^(-1)),close to the value of dry air,and remains structural stability even after cyclic washing.This work offers new possibilities for advanced fibrous sponges in transportation,environmental,and energy applications.
基金supported by the Research Projects of the Department of Education of Guangdong Province 2024ZDZX3079The financial support from the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515011677)+4 种基金the Scientific and Technical Innovation Council of Shenzhen(20220812165832002)the Research Projects of Department of Education of Guangdong Province-2023GCZX015the Innovation Team Project of Guangdong(2022KCXTD055)the China Postdoctoral Science Foundation(Certificate Number:2024M763441)is gratefully acknowledgedsupported by the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20250031 and Research Projects of the Department of Education of Guangdong Province 2023GCZX015。
文摘Despite the intrinsic durability of polymeric hole transport materials,poly-triarylamines(PTAA)-based inverted perovskite solar cells(PSCs)have lagged behind their counterparts in efficiency,primarily due to poor surface wettability,insufficient interfacial contact,and unfavorable energy level alignment at the PTAA/perovskite interface.Here,we report a highly effective interfacial engineering strategy employing the ionic liquid 1,3-dimethylimidazolium dimethyl phosphate(DMIMPH)as a multifunctional interfacial modifier.The incorporation of DMIMPH improves PTAA wettability,promoting the growth of high-quality perovskite films with enhanced interfacial contact.Concurrently,DMIMPH effectively tunes the energy levels of PTAA,enhances its electrical conductivity,and passivates interfacial defects with more efficient hole extraction and charge transport.Moreover,its interaction with residual PbI_(2) modulates perovskite crystallization kinetics,yielding highly crystalline perovskite films with enlarged grain sizes,reduced PbI_(2) residue,and suppressed trap densities.As a result,PTAA-based p-i-n PSCs employing this approach achieve a record certified power conversion efficiency(PCE)of 24.52%,with a champion efficiency of 25.12%—the highest certified value for PTAA-based perovskite devices to date.Impressively,the DMIMPH-modified PSCs without encapsulation maintained 87.48%of their initial efficiency after 1600 h in air.This strategy offers an effective pathway for advancing the performance and stability of polymer-based inverted PSCs.
基金supported by the Chinese National Natural Science Foundation under Grant Nos.(41975181,42325503,42375197,42575207,42205090)Y.LIU is supported by the U.S.Department of Energy’s Atmospheric System Research(ASR)program.
文摘The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects,radiative transfer,and microphysical processes.However,previous studies have been mostly concerned with clouds,with limited studies on fog,particularly those that examine the combined influences of all key physical processes and their roles during fog evolution.As such,this study aims to conduct a comprehensive investigation by examining the relationships between relative dispersion and other microphysical variables,as well as the underlying microphysical and dynamic processes,based on field fog campaigns in polluted and clean conditions.In polluted fog,droplet concentrations are higher,leading to smaller droplets and increased dispersion.The correlation between dispersion and droplet volume-mean radius is positive in the polluted fog,but shifts to negative in clean fog.We attribute the difference to various microphysical processes like aerosol activation,condensation,collision-coalescence,and entrainment-mixing.In polluted fog,high aerosol concentrations,low supersaturations,and strong turbulence(entrainment-mixing)provide suitable conditions for the simultaneous occurrence of droplet condensation and aerosol activation,resulting in a positive correlation between dispersion and volume-mean radius,especially during the fog formation stage.In contrast,during the mature stage in clean fog,condensation is dominant with weak aerosol activation leading to a negative correlation between relative dispersion and volume-mean radius.The collision-coalescence process is more active in the mature stage,increasing radii and leading to the negative correlation between dispersion and volume-mean radius.This result sheds new light on understanding the relative dispersion and mechanisms in fog under different aerosol backgrounds.
基金supported by the National Key R&D Program of China(No.2023YFC3707900)the National Natural Science Foundation of China(No.51978157).
文摘Biochar and zero-valent iron are promising materials for the removal of trichloroethylene(TCE)from groundwater,but further research is still required on the synergistic mechanism and hydraulic performance in the permeable reactive barriers(PRBs)with biochar-iron composites.In this work,biochar-iron composites were synthesized by two different methods,and subjected to the microscopic analysis,batch experiments and the PRB’s model tests.The results indicated that the removal rates of TCE on biochar-iron composites reached above 90%,and the optimal removal conditions were the initial pH of 6.0 and a biochar/iron mass ratio of 5:1.The removal of TCE on biochar-iron composites followed the pseudo-second-order and Freundlich models,and the maximum adsorption capacity of TCE was 25.95 mg/g.The adsorption of biochar and dechlorination of nZVI dominated the removal of TCE.Biochar significantly enhanced the dechlorination of TCE on nZVI through modifying the electrochemical characteristics to lower its corrosion potential of nZVI,promote direct electron transfer,and improve electronic transfer capability.M-5BC-1nZVI exhibited excellent hydraulic performance for maintaining an adequate permeability coefficient(10^(−6)to 10^(−5)m/s).
基金National Natural Science Foundation of China,Grant/Award Number:52104120Hunan Provincial Key Laboratory of Key Technology on Hydropower Development,Grant/Award Number:PKLHD202303。
文摘During geothermal resource exploitation,the potential deterioration of mechanical properties in high-temperature granite subjected to cooling poses a significant safety concern.To address this,the present study investigates the coupled thermo-mechanical behavior of granite during heating and cooling through a combination of laboratory tests and finite difference method analysis.Initial investigations involve X-ray diffraction,thermal expansion test,thermogravimetric analysis,and uniaxial compression test.Results show the significant variations of granite properties under different thermal conditions,attributed to temperature gradients,water evaporation,and mineral phase transitions.Subsequently,a model considering temperature-dependent parameters and real-time cooling rates was employed to simulate linear heating and nonlinear cooling processes.Simulation results indicate that the thermal cracking predominantly occurs during the heating stage,with tensile failure as the primary mode.Additionally,a faster real-time cooling rate at higher temperatures intensifies the thermal cracking behavior in granite.This study effectively elucidates the thermomechanical coupling behavior of granite during heating and cooling processes,providing insights into the mechanisms of mechanical property changes with rising or decreasing temperatures.
基金National Natural Science Foundation of China,Grant/Award Numbers:82404340,82273722,82373685,82204143CAMS Innovation Fund for Medical Science,Grant/Award Number:2021-I2M-1-067Open Research Fund Programme of Changzhou Institute for Advanced Study of Public Health,Nanjing Medical University,Grant/Award Number:CPHM202301。
文摘Background:Immune-mediated inflammatory disease(IMID)and cancer share underlying mechanisms.We aimed to comprehensively evaluate the associations between IMIDs and cancers from global,population and genetic perspectives.Methods:A triangulation framework was employed to assess the association between IMIDs and cancers,using the Global Burden of Disease Study(2012-2021)to analyse six IMIDs and 33 cancers.The UK Biobank(UKBB)prospective cohort was subsequently used to validate these associations,with hazard ratios(HRs)and 95%confidence intervals(CIs)estimated by Cox proportional hazards models.Causal inference based on genetic instruments was performed in the FinnGen and UKBB to assess the potential causal effects between IMIDs and cancers.Results:IMIDs were positively associated with the occurrence of cancers from a global perspective.Moreover,170 specific IMID-cancer pairs revealed statistically significant associations.A total of 20 pairs of specific IMID-cancer associations were further confirmed in the UKBB cohort.Among these,the five most pronounced associations included atopic dermatitis with Hodgkin lymphoma(HR=12.56,95%CI:1.76-89.59),with ovarian cancer(HR=5.65,95%CI:1.41-22.65)and with non-Hodgkin lymphoma(HR=5.11,95%CI:1.91-13.63);rheumatoid arthritis with Hodgkin lymphoma(HR=3.85,95%CI:1.11-13.32);and psoriasis with Hodgkin lymphoma(HR=3.43,95%CI:1.69-6.96).Additionally,a positive causal association between rheumatoid arthritis and Hodgkin lymphoma(inverse variance weighted OR=1.31,95%CI:1.10-1.57)was observed.Conclusions:This study provides comprehensive evidence of the relationships between IMIDs and cancers from global,population and genetic perspectives and identifies 20 pairs of specific IMID-cancer associations,thereby contributing to advancements in cancer prevention and control.
基金supported by National Natural Science Foundation of China(Grant No.52270106 and 22266021)Yunnan Major Scientific and Technological Projects(grant No.202202AG050005)Yunnan Fundamental Research Projects(grant No.202201AT070116).
文摘The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner.In this review,we investigate the development of industrialwaste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste.We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification,in which the active components,pore size,and phase structure can be altered.The review will discuss the potential of using industrial solid wastes,these modified materials,or synthesized materials from raw waste precursors for the removal of air pollutants,including SO_(2),NO_(x),Hg^(0),H_(2)S,VOCs,and CO_(2).The challenges still need to be addressed to realize this potential and the prospects for future research fully.The suggestions for future directions include determining the optimal composition of these materials,calculating the real reaction rate and turnover frequency,developing effective treatment methods,and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.
基金upported by the National Natural Science Foundation of China(Grant No.62305184)the Major Key Project of Pengcheng Laboratory(Grant No.PCL2024A1)+1 种基金the Basic and Applied Basic Research Foundation of Guangdong Province(Grant No.2023A1515012932)the Science,Technology and Innovation Commission of Shenzhen Municipality(Grant No.WDZC20220818100259004).
文摘Single-pixel imaging(SPI)enables efficient sensing in challenging conditions.However,the requirement for numerous samplings constrains its practicality.We address the challenge of high-quality SPI reconstruction at ultra-low sampling rates.We develop an alternative optimization with physics and a data-driven diffusion network(APD-Net).It features alternative optimization driven by the learned task-agnostic natural image prior and the task-specific physics prior.During the training stage,APD-Net harnesses the power of diffusion models to capture data-driven statistics of natural signals.In the inference stage,the physics prior is introduced as corrective guidance to ensure consistency between the physics imaging model and the natural image probability distribution.Through alternative optimization,APD-Net reconstructs data-efficient,high-fidelity images that are statistically and physically compliant.To accelerate reconstruction,initializing images with the inverse SPI physical model reduces the need for reconstruction inference from 100 to 30 steps.Through both numerical simulations and real prototype experiments,APD-Net achieves high-quality,full-color reconstructions of complex natural images at a low sampling rate of 1%.In addition,APD-Net’s tuning-free nature ensures robustness across various imaging setups and sampling rates.Our research offers a broadly applicable approach for various applications,including but not limited to medical imaging and industrial inspection.
基金supported by the Natural Science Foundation of Henan Province(No.242300420021)the Major Science and Technology Projects of Henan Province(No.221100230200)+4 种基金the Open Fund of State Key Laboratory of Advanced Refractories(No.SKLAR202210)the Key Science and Technology Program of Henan Province(No.232102241020)the Undergraduate Innovation and Entrepreneurship Training Program of Henan Province(No.S202310464012)the Ph.D.Research Startup Foundation of Henan University of Science and Technology(No.400613480015)the Postdoctoral Research Startup Foundation of Henan University of Science and Technology(No.400613554001).
文摘Aqueous Zn-ion batteries(AZIBs)have been regarded as promising alternatives to Li-ion batteries due to their advantages,such as low cost,high safety,and environmental friendliness.However,AZIBs face significant challenges in limited stability and lifetime owing to zinc dendrite growth and serious side reactions caused by water molecules in the aqueous electrolyte during cycling.To address these issues,a new eutectic electrolyte based on Zn(ClO_(4))_(2)·6H_(2)O-N-methylacetamide(ZN)is proposed in this work.Compared with aqueous electrolyte,the ZN eutectic electrolyte containing organic N-methylacetamide could regulate the solvated structure of Zn^(2+),effectively suppressing zinc dendrite growth and side reactions.As a result,the Zn//NH4 V4 O10 full cell with the eutectic ZN-1-3 electrolyte demonstrates significantly enhanced cycling stability after 1000 cycles at 1 A g^(-1).Therefore,this study not only presents a new eutectic electrolyte for zinc-ion batteries but also provides a deep understanding of the influence of Zn^(2+)solvation structure on the cycle stability,contributing to the exploration of novel electrolytes for high-performance AZIBs.
基金supported in part by the National Science Foundation of China(52371372)the Project of Science and Technology Commission of Shanghai Municipality,China(22JC1401400,21190780300)the 111 Project,China(D18003)
文摘Dear Editor,This letter focuses on the fact that small objects with few pixels disappear in feature maps with large receptive fields, as the network deepens, in object detection tasks. Therefore, the detection of dense small objects is challenging.
基金supported by the National Natural Science Foundation of China(Nos.U23A20573,U23A20140,22072154,and 22377127)Hebei Natural Science Foundation(B2024208046 and H2022423314)+2 种基金Huang jin tai plan project of Hebei provincial department of education(HJZD202512)S&T Program of Hebei,the Youth innovation Promotion Association of Chinese Academy of Sciences(No.2021048)the Beijing Nova Program(No.20230484352).
文摘Sonodynamic therapy(SDT)as an emerging modality for malignant tumors mainly involves in sonosensitizers and low-intensity ultrasound(US),which can safely penetrate the tissue without significant attenuation.SDT not only has the advantages including high precision,non-invasiveness,and minimal side effects,but also overcomes the limitation of low penetration of light to deep tumors.The cytotoxic reactive oxygen species can be produced by the utilization of sonosensitizers combined with US and kill tumor cells.However,the underlying mechanism of SDT has not been elucidated,and its unsatisfactory efficiency retards its further clinical application.Herein,we shed light on the main mechanisms of SDT and the types of sonosensitizers,including organic sonosensitizers and inorganic sonosensitizers.Due to the development of nanotechnology,many novel nanoplatforms are utilized in this arisen field to solve the barriers of sonosensitizers and enable continuous innovation.This review also highlights the potential advantages of nanosonosensitizers and focus on the enhanced efficiency of SDT based on nanosonosensitizers with monotherapy or synergistic therapy for deep tumors that are difficult to reach by traditional treatment,especially orthotopic cancers.
基金supported by the National Key Research and Development Program of China(No.2021YFC2400703)the Key Scientific and Technological Research Projects in Henan Province(Nos.232102311155 and 232102230106)Zhengzhou University Major Project Cultivation Special Project(No.125-32214076).
文摘Drug-eluting magnesium(Mg)alloy stents have a slower degradation rate and lower restenosis rate compared with uncoated stents,demonstrating good clinical efficacy.However,the release of anti-hyperplasia drugs from coatings delays endothelial tissue repair,thus leading to late stent thrombosis.To address these issues,a dual self-healed coating with various biological properties was fabricated on magnesium fluoride/polydopamine(MgF_(2)/PDA)-treated Mg alloys by spraying-assisted layer-by-layer(LBL)self-assembly of chitosan(CS),gallic acid(GA),and 3-aminobenzeneboronic acid-modified hyaluronic acid(HA-ABBA).The LBL coating,approximately 1.50μm thick,exhibited a uniform morphology with good adhesion strength(~1065 mN).The annual corrosion rate(Pi)of LBL samples was~1400 times slower than that of the Mg substrate,due to the physical barrier function provided by MgF_(2)/PDA layers and the dual self-healed ability of LBL layers.The rapid self-healing ability(with a healing period of~4 h under dynamic/static conditions)resulted from the synergistic interplay between the recombination of diverse chemical bonds within the LBL coating and the coordination of LBL-released GA with Mg2+,as corroborated by computer simulations.Compared with the drug-eluting coatings,the LBL sample demonstrated substantial advantages in anti-oxidation,anti-denaturation of fibrinogen,anti-platelet adhesion,anti-inflammation,anti-hyperplasia,and promoted-endothelialization.These benefits effectively address the limitations associated with drug-eluting coatings.
基金supported by the National Natural Science Foundation of China(No.22278041)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(No.2022-K78)+1 种基金Jiangsu Province Key Laboratory of Fine Petrochemical Engineering(No.KF2107)the Advanced Catalysis and Green Manufacturing Collab-orative Innovation Center(No.ACGM2022-10-07)。
文摘Herein,a series of manganese oxide catalysts with different valences(Mn_(3)O_(4),Mn_(2)O_(3),and MnO_(2))were designed and synthesized for the synthesis of ethylene urea(EU)from ethylenediamine(EDA)and carbon dioxide(CO_(2)).With a maximal EDA conversion of 82%and EU selectivity of 99%at 160℃ for 2 h,Mn_(2)O_(3) catalysts had the best catalytic activity among them,which was superior to the reported catalysts.In the following order:Mn_(2)O_(3)>MnO_(2)>Mn_(3)O_(4),the catalytic activity for the synthesis of EU from CO_(2) and EDA decreased.Further characterization showed the Mn_(2)O_(3) catalyst possessed a greater Mn^(3+)/Mn4+ratio and more surface oxygen vacancies than the MnO_(2) and Mn_(3)O_(4),which improved its capacity to adsorb and activate CO_(2) and EDA.After four recycling runs,the EDA conversion slightly declined from 82%to 56%on Mn_(2)O_(3) catalyst,while no obvious change in EU selectivity was observed.The loss of surface Ov contents and Mn^(3+)proportion were concluded as main reasons for the decrease in catalytic activity over Mn_(2)O_(3) catalyst.This work demonstrated a metal oxide catalyst that was efficient in producing EU from CO_(2) and EDA.
基金Project supported by the National Natural Science Foundation of China(No.51439005)the National Basic Research Program(973 Program)of China(No.2013CB035906)the National Natural Science Foundation of Innovation Group(No.51621092),China
