Unlike other regions in China,PM2.5concentrations in Yunnan's border cities exhibit a distinct seasonal pattern,with significantly higher levels in spring compared to other seasons.To obtain direct evidence of ...Unlike other regions in China,PM2.5concentrations in Yunnan's border cities exhibit a distinct seasonal pattern,with significantly higher levels in spring compared to other seasons.To obtain direct evidence of the impact of cross-border transport of biomass burning emissions on air quality in Yunnan,observations based on continuous lidar network measurements and manual PM2.5sampling were carried out in spring 2024 in Yunnan.The source and transport pathways of PM2.5in Yunnan were analyzed by combining ground-based observation data,satellite remote sensing fire-point data,model simulations and backward trajectory analysis.The significant positive correlation between PM2.5and CO concentrations in spring 2024 in Yunnan Province indicates typical biomass burning characteristics.Apparent pollution transport and settling events were observed with lidars.The good agreement of the spatial distribution of PM2.5and K+ concentrations also provide visual evidence of the impact of biomass burning emissions on the border cities of Yunnan.Cluster analysis and data assimilation results show that high concentration air mass from biomass burning of the South and Southeast Asia is an important cause of the surge in PM2.5in border cities.Notably,eastern Myanmar represents the dominant potential source of PM2.5for Yunnan's border cities in spring,with emissions from Myanmar's biomass burning contributing over 20μg/m3 to local PM2.5levels.展开更多
Selenium(Se),an essential trace element,plays a critical role in protecting the toxicity of methylmercury(MeHg).However,its detoxification mechanism for alleviating MeHg-induced damage remains largely unexplored.This ...Selenium(Se),an essential trace element,plays a critical role in protecting the toxicity of methylmercury(MeHg).However,its detoxification mechanism for alleviating MeHg-induced damage remains largely unexplored.This study focused on the antagonistic effects of Se supplementation on the toxic responses induced by MeHg pretreatment in Caenorhabditis elegans.Our results showed that following a 20 h pre-exposure to MeHg,4 h exposure to Se effectively and rapidly antagonized the reproductive and neurological impairments induced by MeHg.Meanwhile,we found that the total Hg content decreased from 166±46.0 to 109±18.7µg/g after the addition of Se.Apart from inhibiting the bioaccumulation of Hg,Se supplementation reduced MeHg-induced reactive oxygen species(ROS)and promoted mitochondrial fusion to improve mitochondrial quality.In addition,MeHg-induced autophagy could be alleviated by increasing lysosome activity after the addition of Se.Further studies revealed that Se supplementation modulated the expression of gss-1 and gst-4,regulating glutathione(GSH)synthesis and elevated MeHg-decreased GSH content from 45.5%to 79.7%.These findings suggested that Se recovered MeHg-induced reproductive and neurological damage by modulating mitochondrial function and GSH synthesis,providing valuable insights for developing novel therapeutic strategies against MeHg toxicity.展开更多
1.Background,Polyolefins were first commercialized in the 1930s by Imperial Chemical Industries(ICI)and were applied as underwater cable coatings.After almost a century of development,polyolefins have become one of th...1.Background,Polyolefins were first commercialized in the 1930s by Imperial Chemical Industries(ICI)and were applied as underwater cable coatings.After almost a century of development,polyolefins have become one of the most widely used synthetic polymers,accounting for almost half of all global plastics production[1].Due to their many superior properties,they have found many everyday applications,but their annual production and widespread usage in single-use packaging have made them a major component of post-consumer plastic waste[2].Polyolefins are indispensable in the modern chemical industry and society,and their global market size is expected to grow rapidly in the foreseeable future.However,the current linear production and consumption of polyolefins is unsustainable and has created a serious environmental burden.Traditional recycling of polyolefins is performed via either mechanical recycling or pyrolysis.展开更多
The Schottky barrier height(SBH),which serves as a pivotal determinant of charge carrier injection efficiency in electronic devices,critically governs electrical behavior at metal/semiconductor interfaces.However,pron...The Schottky barrier height(SBH),which serves as a pivotal determinant of charge carrier injection efficiency in electronic devices,critically governs electrical behavior at metal/semiconductor interfaces.However,pronounced metal-induced gap states at metal contact interfaces induce Fermi-level pinning,which constrains the controllability of the SBH and ultimately degrades device performance.In this work,atomic models of metal/GaN interfaces with diverse metal terminations are constructed on the basis of first-principles calculations.The interfacial electrical properties,including binding energies,charge density differences,and SBHs,are systematically investigated.The computational SBH results are further validated using the experimental current-voltage characteristics of fabricated metal-GaN Schottky diodes.For n-type SBHs of different metals,these calculation results reveal a robust linear correlation with metal work functions,yielding a moderate pinning factor(S≈0.31)that aligns closely with experimental and empirical values.These findings establish a theoretical foundation for SBH engineering at metal/GaN interfaces and offer valuable insights for the design of high-performance GaN-based devices.展开更多
The Yangtze River Delta(YRD)region has witnessed a consistent decrease in NO2,CO,and PM2.5 from 2016 to 2023.However,ozone has exhibited fluctuating patterns.Quantifying ozone contributions from emissions,both w...The Yangtze River Delta(YRD)region has witnessed a consistent decrease in NO2,CO,and PM2.5 from 2016 to 2023.However,ozone has exhibited fluctuating patterns.Quantifying ozone contributions from emissions,both within and outside the YRD,is essential for understanding city-cluster-scale ozone pollution(CCSOP).To address these concerns,a comprehensive approach combining Kolmogorov-Zurbenko filtering,Empirical Orthogonal Function,Absolute Principal Component Score,andMultiple Linear Regression methods(KZ-EOF-APCs-MLR)was employed to quantify the impacts of meteorological factors,local and non-local emission contributions of ozone(LECO and NECO).Emission changes were identified as the predominant factor shaping annual fluctuations in ambient ozone.Notably,during the previous andmiddle stages of the COVID-19 pandemic(from2017 to 2021),emissions reductions led to a marked decrease in YRD ozone levels(-7.01μg/m3),with a pronounced rebound post-pandemic(2022 to 2023)(+8.04μg/m3).Seasonally,the emissioninduced ozone exhibited fluctuating upward trend during autumn and winter,suggesting a transition of ozone pollution towards colder seasons.Spatially,high LECO concentrated in the eastern YRD(EYRD)across spring,autumn,and winter,becoming prominent in the central YRD(CYRD)during summer.During CCSOP,the CYRD exhibited the highest LECO and exceedance frequency(20.82μg/m3 and 45.27%).LECO explained a large portion of ozone variability during CCSOP,particularly in the EYRD,while NECO showed less explanatory power but consistently high contributions(148.05±15.52μg/m3).These findings offer valuable insights for a deeper understanding of the evolving patterns of ozone pollution and the issue of CCSOP in the YRD.展开更多
Extreme ozone pollution events(EOPEs)are associated with synoptic weather patterns(SWPs)and pose severe health and ecological risks.However,a systematic investigation of themeteorological causes,transport pathways,and...Extreme ozone pollution events(EOPEs)are associated with synoptic weather patterns(SWPs)and pose severe health and ecological risks.However,a systematic investigation of themeteorological causes,transport pathways,and source contributions to historical EOPEs is still lacking.In this paper,the K-means clustering method is applied to identify six dominant SWPs during the warm season in the Yangtze River Delta(YRD)region from 2016 to 2022.It provides an integrated analysis of the meteorological factors affecting ozone pollution in Hefei under different SWPs.Using the WRF-FLEXPART model,the transport pathways(TPPs)and geographical sources of the near-surface air masses in Hefei during EOPEs are investigated.The results reveal that Hefei experienced the highest ozone concentration(134.77±42.82μg/m3),exceedance frequency(46 days(23.23%)),and proportion of EOPEs(21 instances,47.7%)under the control of peripheral subsidence of typhoon(Type 5).Regional southeast winds correlated with the ozone pollution in Hefei.During EOPEs,a high boundary layer height,solar radiation,and temperature;lowhumidity and cloud cover;and pronounced subsidence airflow occurred over Hefei and the broader YRD region.The East-South(E_S)patterns exhibited the highest frequency(28 instances,65.11%).Regarding the TPPs and geographical sources of the near-surface air masses during historical EOPEs.The YRD was the main source for land-originating air masses under E_S patterns(50.28%),with Hefei,southern Anhui,southern Jiangsu,and northern Zhejiang being key contributors.These findings can help improve ozone pollution early warning and control mechanisms at urban and regional scales.展开更多
As a significant city in the Yangtze River Delta regions,Hefei has experienced rapid changes in the sources of air pollution due to its high-speed economic development and urban expansion.However,there has been limite...As a significant city in the Yangtze River Delta regions,Hefei has experienced rapid changes in the sources of air pollution due to its high-speed economic development and urban expansion.However,there has been limited research in recent years on the spatial-temporal distribution and emission of its atmospheric pollutants.To address this,this study conducted mobile observations of urban roads using the Mobile-DOAS instrument from June 2021 to May 2022.The monitoring results exhibit a favourable consistent with TROPOMI satellite data and ground monitoring station data.Temporally,there were pronounced seasonal variations in air pollutants.Spatially,high concentration of HCHO and NO2were closely associated with traffic congestion on roadways,while heightened SO2levels were attributed to winter heating and industrial emissions.The study also revealed that with the implementation of road policies,the average vehicle speed increased by 95.4%,while the NO concentration decreased by 54.4%.In the estimation of urban NOxemission flux,it was observed that in temporal terms,compared with inventory data,the emissions calculated viamobile measurements exhibitedmore distinct seasonal patterns,with the highest emission rate of 349 g/sec in winter and the lowest of 142 g/sec in summer.In spatial terms,the significant difference in emissions between the inner and outer ring roads also suggests the presence of the city’s primary NOxemission sources in the area between these two rings.This study offers data support for formulating the next phase of air pollution control measures in urban areas.展开更多
This study focuses on the spatiotemporal distribution,urban-rural variations,and driving factors of ammonia Vertical Column Densities(VCDs)in China’s Yangtze River Delta region(YRD)from 2008 to 2020.Utilizing data fr...This study focuses on the spatiotemporal distribution,urban-rural variations,and driving factors of ammonia Vertical Column Densities(VCDs)in China’s Yangtze River Delta region(YRD)from 2008 to 2020.Utilizing data from the Infrared Atmospheric Sounding Interfer-ometer(IASI),Generalized Additive Models(GAM),and the GEOS-Chem chemical transport model,we observed a significant increase of NH3VCDs in the YRD between 2014 and 2020.The spatial distribution analysis revealed higher NH3concentrations in the northern part of the YRD region,primarily due to lower precipitation,alkaline soil,and intensive agricul-tural activities.NH3VCDs in the YRD region increased significantly(65.18%)from 2008 to 2020.The highest growth rate occurs in the summer,with an annual average growth rate of 7.2%during the period from 2014 to 2020.Agricultural emissions dominated NH3VCDs during spring and summer,with high concentrations primarily located in the agricultural areas adjacent to densely populated urban zones.Regions within several large urban areas have been discovered to exhibit relatively stable variations in NH3VCDs.The rise in NH3VCDs within the YRD region was primarily driven by the reduction of acidic gases like SO2,as emphasized by GAM modeling and sensitivity tests using the GEOS-Chem model.The concentration changes of acidic gases contribute to over 80%of the interannual variations in NH3VCDs.This emphasizes the crucial role of environmental policies targeting the reduction of these acidic gases.Effective emission control is urgent tomitigate environmental hazards and secondary particulate matter,especially in the northern YRD.展开更多
Electrocatalytic conversion of carbon dioxide(CO2)offers an effective method of CO2fixation to mitigate global warming and the energy crisis.However,for supported Ni single-atom catalysts(SACs),which are among t...Electrocatalytic conversion of carbon dioxide(CO2)offers an effective method of CO2fixation to mitigate global warming and the energy crisis.However,for supported Ni single-atom catalysts(SACs),which are among the most promising candidates for this application,the relationship between Ni coordination structure and catalytic properties is still under strong debate.Here,we fabricated a series of Ni SACs through precise-engineering of anchor sites on nitrogen-doped carbon(NC)followed by Ni atom anchoring using atomic layer deposition.Among them,a Ni1/NC SAC,with a coordination number(CN)of four but less pyridinic nitrogen(Npyri),achieved over 90%faradaic efϐiciency for CO at potentials from-0.7 to-1.0 V and a mass activity of 6.5 A/mgNi at-0.78 V along with high stability,outperforming other Ni SACs with lower CN and more Npyri.Theoretical calculations of various three and four-coordinated Ni1-NxCy structures revealed a linear correlation between the reaction Gibbs free energy for the potential-limiting step and the highest occupied molecular orbital(HOMO)position of Ni-3d orbitals,therein the four-coordinated Ni1-N1C3with the highest HOMO position is identified as the active site for the electrocatalytic CO2-to-CO process,in line with the experimental results.展开更多
The occurrence of extreme weather events is becoming more frequent due to global climate change.A long-lasting dust outbreak in the spring of 2023 was triggered by Mongolia cyclones and cold fronts in the dust source ...The occurrence of extreme weather events is becoming more frequent due to global climate change.A long-lasting dust outbreak in the spring of 2023 was triggered by Mongolia cyclones and cold fronts in the dust source areas.In this study,we illustrate the spatial distribution,the transport path of the dust and its influence on the air quality of downstream cities utilizing ground-based and space-borne measurements.Results indicate a more complicated pollution,coexisting of polluted dust stage S1 and pure dust stage S2.In S1,the aerosol was characterized by a dual-layer vertical structure—high extinction coefficient of nearly 1.0 km−1with a low particle depolarized ratio(PDR)of1300µg/m3.PM10 positively correlated with trace gases in S1 while varying inversely with the pollution gases in S2.The results help to shed light on the classification of different types of dust and also be useful in developing an effective strategy to forecast air pollution in downstream areas.展开更多
Converting CO2to methanol presents a crucial pathway for achieving carbon neutrality,yet designing highly active and selective nano catalysts remain challenging.In this work,we report a combined density functional ...Converting CO2to methanol presents a crucial pathway for achieving carbon neutrality,yet designing highly active and selective nano catalysts remain challenging.In this work,we report a combined density functional theory and microkinetic study screening 26 transition metal single atoms(Sc-Zn,Y-Cd,Ta-Au)atomically dispersed in MoS2nanosheet(M1-MoS2)for CO2hydrogenation to methanol.Among these,Ni1-MoS2was identified as a promising candidate,exhibiting excellent stability and hydrogen dissociation capability.The reaction proceeds through a dissociative hydrogenation mechanism via key intermediates including*COOH,*C(OH)2,*CH(OH)2,*CHOH,and*CH2OH.Microkinetic simulations reveal that Ni1-MoS2significantly outperforms the experimentally validated Pt1-MoS2,demonstrating a 26.76-fold enhancement in formation rate and high selectivity under industrial relevant conditions(210℃,8 bar CO2,24 bar H2).This work not only highlights Ni1-MoS2as a highly efficient and cost-effective catalyst but also provides a mechanistic and kinetic framework for accelerating the design of single-atom catalysts for CO2conversion.展开更多
Zika virus(ZIKV)infection is associated with severe neurological complications such as congenital microcephaly,yet no safe and effective vaccine is currently available.A critical challenge in ZIKV vaccine development ...Zika virus(ZIKV)infection is associated with severe neurological complications such as congenital microcephaly,yet no safe and effective vaccine is currently available.A critical challenge in ZIKV vaccine development arises from cross-reactive,non-or sub-neutralizing antibodies,which may enhance dengue virus(DENV)infection through antibody-dependent enhancement(ADE).Herein,we report a vaccine strategy utilizing Mi3 nanoparticles to display the envelope(E)protein domain Ⅲ(EDⅢ)of ZIKV,which induces protective immunity against ZIKV infection in murine models.Compared to an EDⅢ subunit vaccine,the Mi3-EDⅢ nanoparticle vaccine elicited significantly higher antibody responses and stronger cell-mediated immune responses.In C57BL/6 mice,maternal immunization with Mi3-EDⅢ protected the neonates against ZIKV-caused symptoms,including body weight loss,neurological abnormalities,retardation of brain development,and mortality.In interferon-α/β receptor knockout(Ifnar1-/-)C57BL/6 mice,Mi3-EDⅢ immunization conferred effective protection against lethal ZIKV challenge.Notably,unlike ZIKV convalescent sera,Mi3-EDⅢ immune sera did not enhance DENV infection in human chronic myelogenous leukemia K562 cells,suggesting the absence of ADE-prone antibody induction.Our results demonstrate that Mi3-EDⅢ is a promising vaccine candidate against ZIKV infection and warrants further development.展开更多
The development of straightforward and environmentally friendly techniques for synthesizing organophosphorus compounds with C(sp²)—P bonds would be of great value for the advancement of synthetic chemistry.An el...The development of straightforward and environmentally friendly techniques for synthesizing organophosphorus compounds with C(sp²)—P bonds would be of great value for the advancement of synthetic chemistry.An electrochemically driven dienylation strategy of arylphosphine oxides with allenylsilanes is reported for the efficient synthesis of dienyl phosphorus compounds.A wide range of dienyl organophosphorus compounds with various functional group tolerance were facilely obtained in moderate to great yield.Mechanistic studies indicate that the desired C(sp²)-P bond is constructed through the radical addition process between the phosphoryl radical and the allene carbon.展开更多
The transport and thermoelectric properties together with annealing of the new layered Bi-chalcogenide LaOBiHgS3are studied.On the transport part,the insulating behavior of the as-grown sample is evidently depresse...The transport and thermoelectric properties together with annealing of the new layered Bi-chalcogenide LaOBiHgS3are studied.On the transport part,the insulating behavior of the as-grown sample is evidently depressed by post annealing.A hump-like abnormality appears around 170 K.The thermoelectric performance of the sample is observably improved by the annealing,mainly because of the enhanced electrical conductance.The present results suggest that the physical properties of LaOBiHgS3are sensitive to post annealing and the possible micro adjustments that follow,indicating the layered Bi-chalcogenide family to be an ideal platform for designing novel functional materials.展开更多
Nanoplastics are emerging contaminants that may co-exist with organochlorine pesticides and adversely affect invertebrates in the environment.However,the impact of environmental aging on the combined toxicity of nanop...Nanoplastics are emerging contaminants that may co-exist with organochlorine pesticides and adversely affect invertebrates in the environment.However,the impact of environmental aging on the combined toxicity of nanoplastics and organochlorine pesticides remains unclear.This study investigated the effects of aging on the combined toxicity of polystyrene nanoplastics(PS NPs)and chlordane against Caenorhabditis elegans.The results showed that photo-aging altered the physicochemical properties of PS NPs and promoted the combined toxicity of PS NPs and chlordane to nematodes by reducing survival rate,body length and enhancing germline apoptosis.Additionally,combined exposure of nematodes to aged PS NPs and chlordane significantly increased reactive oxygen species production and intestinal permeability,suggesting that aging enhances combined toxicity through oxidative stress and intestinal damage.Moreover,aging increased chlordane contents in nematodes without promoting PS NPs accumulation,potentially leading to increased combined toxicity of PS NPs and chlordane.Notably,aging significantly increased the accumulation of PS NPs in the posterior intestine of the nematode during co-exposure,which may be responsible for the most sensitive and highest degree of change in germline apoptosis.These observations emphasize the significance of accounting for environmental aging as well as the accumulation and distribution of nanoplastics in organisms when assessing the combined effects of nanoplastics and coexisting pollutants.展开更多
HCLS1-associated protein X-1(HAX1)is a multifunctional mitochondrial protein involved in the regulation of apoptosis,a crucial process of programmed cell death,and mRNA processing.Despite its significance,limited stru...HCLS1-associated protein X-1(HAX1)is a multifunctional mitochondrial protein involved in the regulation of apoptosis,a crucial process of programmed cell death,and mRNA processing.Despite its significance,limited structural data is available for HAX1,hindering a comprehensive understanding of its biological function.Notably,the caseinolytic mitochondrial matrix peptidase chaperone subunit B(CLPB)has been identified as an interacting partner of HAX1,yet the biophysical properties and binding affinity governing their interaction remain poorly defined.In this study,we present a thorough biophysical characterization of full-length human HAX1 and CLPB,accomplished through recombinant expression and purification.By employing size exclusion chromatography,dynamic light scattering,and circular dichroism spectroscopy,we successfully established their biophysical properties,revealing contrasting structural features,with CLPB displaying a-helical content and HAX1 exhibiting a disordered nature.Moreover,we employed solutionstate nuclear magnetic resonance(NMR)spectroscopy to probe their binding affinity.Our findings demonstrate the formation of stable multimeric complexes between HAX1 and CLPB,and we quantified a dissociation constant in the low range of micro-molar for their high affinity interaction.These results lay the foundation for further in-depth investigations into the dynamics and energetics governing the HAX1-CLPB interaction,ultimately contributing to a comprehensive understanding of their functional mechanisms.展开更多
We report the magnetic and transport properties of EuBi2 single crystal. EuBi2 exhibits complex magnetic behavior at low temperatures. In both the in-plane and out-of-plane directions, three antiferromagnetic(AF...We report the magnetic and transport properties of EuBi2 single crystal. EuBi2 exhibits complex magnetic behavior at low temperatures. In both the in-plane and out-of-plane directions, three antiferromagnetic(AFM) transitions have been observed at TN1~18.9 K, TN2~7.0 K, and TN3~3.1 K. Among them, the transitions at TN2 and TN3 represent the canted AFM orders with ferromagnetic components. As the magnetic field increases, the transition at TN3 is rapidly suppressed to disappearance. However, the transitions at TN1 and TN2 persist until high fields and their signatures can also be reflected in the resistivity and specific heat. Above the magnetic transition temperature TN1, the resistivity of EuBi2 increases linearly with temperature, exhibiting the strange-metal behavior. In the magnetically ordered region below TN1, EuBi2 exhibits the weak antilocalization(WAL) effect and large magnetoresistance(475% at 1.8 K and 14 T). It is suggested that the magnetic ordering significantly enhances the spin–orbital coupling interaction and induces the WAL effect.展开更多
The variation of the effective mass m*of carrier is often overlooked in experimental studies on quantum oscillations and Kohler's rule.Here,we report the magnetotransport properties of La3Sc Bi5and reveal...The variation of the effective mass m*of carrier is often overlooked in experimental studies on quantum oscillations and Kohler's rule.Here,we report the magnetotransport properties of La3Sc Bi5and reveal the changing m*in it.The temperature and magnetic field dependence of m*follows the power-law scaling behavior at low temperature and leads to the failure of conventional analysis,which should not be ignored.In the analysis of the thermal factor and Dingle plot of de Haas-van Alphen oscillation in La3ScBi5,satisfactory fitting results can be obtained after considering the correction of m*.We have also applied this method to Sr1-yMn1-zSb2,solving the remaining fitting problem in previous reports.Moreover,the magnetoresistance(MR)of La3ScBi5has been found to violate Kohler's rule.Although the extended Kohler's rule is applicable to high-temperature MR data,it does not scale the low-temperature data well.We further modified the extended Kohler's rule by introducing m*,and subsequently scaled the low-temperature MR data well.Our study emphasizes the importance of considering the variation of m*in the analysis of quantum oscillations and Kohler's rule,and provides a method for extracting the temperature and magnetic field dependence of m*through quantum oscillations,which is very beneficial for the data analysis of other materials in the future.展开更多
Oxygen deficiency is known to critically influence the superconductivity of La3Ni2O7-δ.However,precise control of oxygen content to mitigate such deficiencies remains a significant challenge.In this work,we ...Oxygen deficiency is known to critically influence the superconductivity of La3Ni2O7-δ.However,precise control of oxygen content to mitigate such deficiencies remains a significant challenge.In this work,we synthesized high-oxygencontent La3Ni2O7+δpolycrystals via high-pressure oxygen annealing with the oxygen stoichiometry(δ)successfully tuned by varying the amount of KClO4.The obtained samples La3Ni2O7.16and La3Ni2O7.38exhibit metallic behavior at ambient pressure.We further conducted a comprehensive investigation into the pressure-induced superconductivity and atomic structure.STEM imaging revealed large-area bilayer-phase stacking in La3Ni2O7.16,while La3Ni2O7.38showed noticeable intergrowth with other Ruddlesden-Popper(R-P)phases.Notably,the critical pressure in La3Ni2O7.16is substantially reduced,though its critical temperature(Tc)is lower than that of as-grown samples.In contrast,only a weak superconducting signal was detected in higher oxygen content sample La3Ni2O7.38likely due to the intergrowth with other R-P phases,nonnegligible interstitial oxygen,or an increased fraction of the tetragonal phase.Our findings provide a viable pathway for optimizing nickelate superconductivity and offer insights into the fundamental mechanisms governing superconductivity in these materials.展开更多
Developing sustainable and efficient methods for the transformation of 1,3-dicarbonyl compounds and alkene functionalization represents a pivotal endeavor for advancing the frontiers of synthetic organic chemistry.Her...Developing sustainable and efficient methods for the transformation of 1,3-dicarbonyl compounds and alkene functionalization represents a pivotal endeavor for advancing the frontiers of synthetic organic chemistry.Herein,an electrochemically driven functionalization reaction of 1,3-dicarbonyl compounds and alkenes is reported,which enables the efficient construction of α-alkylated 1,3-dicarbonyl compounds.This protocol avoids additional chemical oxidantseductants,proceeds under mild and environmentally benign conditions,and exhibits excellent functional group tolerance,furnishing a diverse array of target products in moderate to good yields.Mechanistic studies indicate that electrochemically generated 1,3-dicarbonyl radicals add to alkenes,followed by single-electron transfer(SET)oxidation and nucleophilic alcohol quenching,thereby realizing efficient alkene functionalization.展开更多
基金supported by the National Key Research and Development Program of China(Nos.2022YFC3704000 and 2022YFC3700400)the National Natural Science Foundation of China(Nos.42305149 and 42575144).
摘要Unlike other regions in China,PM2.5concentrations in Yunnan's border cities exhibit a distinct seasonal pattern,with significantly higher levels in spring compared to other seasons.To obtain direct evidence of the impact of cross-border transport of biomass burning emissions on air quality in Yunnan,observations based on continuous lidar network measurements and manual PM2.5sampling were carried out in spring 2024 in Yunnan.The source and transport pathways of PM2.5in Yunnan were analyzed by combining ground-based observation data,satellite remote sensing fire-point data,model simulations and backward trajectory analysis.The significant positive correlation between PM2.5and CO concentrations in spring 2024 in Yunnan Province indicates typical biomass burning characteristics.Apparent pollution transport and settling events were observed with lidars.The good agreement of the spatial distribution of PM2.5and K+ concentrations also provide visual evidence of the impact of biomass burning emissions on the border cities of Yunnan.Cluster analysis and data assimilation results show that high concentration air mass from biomass burning of the South and Southeast Asia is an important cause of the surge in PM2.5in border cities.Notably,eastern Myanmar represents the dominant potential source of PM2.5for Yunnan's border cities in spring,with emissions from Myanmar's biomass burning contributing over 20μg/m3 to local PM2.5levels.
基金supported by the National Key Research and Development Program of China(No.2023YFC3708303)Anhui Provincial Natural Science Foundation(No.2308085UM08)the National Natural Science Foundation of China(No.22376200).
摘要Selenium(Se),an essential trace element,plays a critical role in protecting the toxicity of methylmercury(MeHg).However,its detoxification mechanism for alleviating MeHg-induced damage remains largely unexplored.This study focused on the antagonistic effects of Se supplementation on the toxic responses induced by MeHg pretreatment in Caenorhabditis elegans.Our results showed that following a 20 h pre-exposure to MeHg,4 h exposure to Se effectively and rapidly antagonized the reproductive and neurological impairments induced by MeHg.Meanwhile,we found that the total Hg content decreased from 166±46.0 to 109±18.7µg/g after the addition of Se.Apart from inhibiting the bioaccumulation of Hg,Se supplementation reduced MeHg-induced reactive oxygen species(ROS)and promoted mitochondrial fusion to improve mitochondrial quality.In addition,MeHg-induced autophagy could be alleviated by increasing lysosome activity after the addition of Se.Further studies revealed that Se supplementation modulated the expression of gss-1 and gst-4,regulating glutathione(GSH)synthesis and elevated MeHg-decreased GSH content from 45.5%to 79.7%.These findings suggested that Se recovered MeHg-induced reproductive and neurological damage by modulating mitochondrial function and GSH synthesis,providing valuable insights for developing novel therapeutic strategies against MeHg toxicity.
基金supported by National Key Research and Development Program of China(2021YFA1501700)National Natural Science Foundation of China(U25A20249,U25D9008,and 22301294)+1 种基金Natural Science Foundation of Anhui Province,China(2308085Y35 and 2023AH030002)Chinese Academy of Sciences(CAS)Project for Young Scientists in Basic Research(YSBR-094)。
摘要1.Background,Polyolefins were first commercialized in the 1930s by Imperial Chemical Industries(ICI)and were applied as underwater cable coatings.After almost a century of development,polyolefins have become one of the most widely used synthetic polymers,accounting for almost half of all global plastics production[1].Due to their many superior properties,they have found many everyday applications,but their annual production and widespread usage in single-use packaging have made them a major component of post-consumer plastic waste[2].Polyolefins are indispensable in the modern chemical industry and society,and their global market size is expected to grow rapidly in the foreseeable future.However,the current linear production and consumption of polyolefins is unsustainable and has created a serious environmental burden.Traditional recycling of polyolefins is performed via either mechanical recycling or pyrolysis.
基金supported by the National Natural Science Foundation of China(Grants 52302046,62474001,51727901 and L2424216)Guangdong Basic and Applied Basic Research Foundation(Grants 2022A1515110149 and 2024A1515011764)+4 种基金the Basic Research Program of Jiangsu(Grant BK20230268)the Knowledge Innovation Program of Wuhan-Shuguang Project(Grant 2023010201020262)the Universities Collaborative Innovation Project of Anhui Province(Grant GXXT-2023-001)supported by Hubei Province“Chutian Talent Plan”Science and Technology Innovation Team Projectthe support from the Anhui Province Engineering Research Center for Advanced Power Electronics and Energy Conversion(APEEC)。
摘要The Schottky barrier height(SBH),which serves as a pivotal determinant of charge carrier injection efficiency in electronic devices,critically governs electrical behavior at metal/semiconductor interfaces.However,pronounced metal-induced gap states at metal contact interfaces induce Fermi-level pinning,which constrains the controllability of the SBH and ultimately degrades device performance.In this work,atomic models of metal/GaN interfaces with diverse metal terminations are constructed on the basis of first-principles calculations.The interfacial electrical properties,including binding energies,charge density differences,and SBHs,are systematically investigated.The computational SBH results are further validated using the experimental current-voltage characteristics of fabricated metal-GaN Schottky diodes.For n-type SBHs of different metals,these calculation results reveal a robust linear correlation with metal work functions,yielding a moderate pinning factor(S≈0.31)that aligns closely with experimental and empirical values.These findings establish a theoretical foundation for SBH engineering at metal/GaN interfaces and offer valuable insights for the design of high-performance GaN-based devices.
基金supported by the National Natural Science Foundation of China(Nos.U19A2044,42105132,42030609,41975037)the National Key Research and Development Programof China(No.2022YFC3700303).
摘要The Yangtze River Delta(YRD)region has witnessed a consistent decrease in NO2,CO,and PM2.5 from 2016 to 2023.However,ozone has exhibited fluctuating patterns.Quantifying ozone contributions from emissions,both within and outside the YRD,is essential for understanding city-cluster-scale ozone pollution(CCSOP).To address these concerns,a comprehensive approach combining Kolmogorov-Zurbenko filtering,Empirical Orthogonal Function,Absolute Principal Component Score,andMultiple Linear Regression methods(KZ-EOF-APCs-MLR)was employed to quantify the impacts of meteorological factors,local and non-local emission contributions of ozone(LECO and NECO).Emission changes were identified as the predominant factor shaping annual fluctuations in ambient ozone.Notably,during the previous andmiddle stages of the COVID-19 pandemic(from2017 to 2021),emissions reductions led to a marked decrease in YRD ozone levels(-7.01μg/m3),with a pronounced rebound post-pandemic(2022 to 2023)(+8.04μg/m3).Seasonally,the emissioninduced ozone exhibited fluctuating upward trend during autumn and winter,suggesting a transition of ozone pollution towards colder seasons.Spatially,high LECO concentrated in the eastern YRD(EYRD)across spring,autumn,and winter,becoming prominent in the central YRD(CYRD)during summer.During CCSOP,the CYRD exhibited the highest LECO and exceedance frequency(20.82μg/m3 and 45.27%).LECO explained a large portion of ozone variability during CCSOP,particularly in the EYRD,while NECO showed less explanatory power but consistently high contributions(148.05±15.52μg/m3).These findings offer valuable insights for a deeper understanding of the evolving patterns of ozone pollution and the issue of CCSOP in the YRD.
基金supported by the National Natural Science Foundation of China(Nos.U19A2044,42105132,42030609,and 41975037)the National Key Research and Development Programof China(No.2022YFC3700303).
摘要Extreme ozone pollution events(EOPEs)are associated with synoptic weather patterns(SWPs)and pose severe health and ecological risks.However,a systematic investigation of themeteorological causes,transport pathways,and source contributions to historical EOPEs is still lacking.In this paper,the K-means clustering method is applied to identify six dominant SWPs during the warm season in the Yangtze River Delta(YRD)region from 2016 to 2022.It provides an integrated analysis of the meteorological factors affecting ozone pollution in Hefei under different SWPs.Using the WRF-FLEXPART model,the transport pathways(TPPs)and geographical sources of the near-surface air masses in Hefei during EOPEs are investigated.The results reveal that Hefei experienced the highest ozone concentration(134.77±42.82μg/m3),exceedance frequency(46 days(23.23%)),and proportion of EOPEs(21 instances,47.7%)under the control of peripheral subsidence of typhoon(Type 5).Regional southeast winds correlated with the ozone pollution in Hefei.During EOPEs,a high boundary layer height,solar radiation,and temperature;lowhumidity and cloud cover;and pronounced subsidence airflow occurred over Hefei and the broader YRD region.The East-South(E_S)patterns exhibited the highest frequency(28 instances,65.11%).Regarding the TPPs and geographical sources of the near-surface air masses during historical EOPEs.The YRD was the main source for land-originating air masses under E_S patterns(50.28%),with Hefei,southern Anhui,southern Jiangsu,and northern Zhejiang being key contributors.These findings can help improve ozone pollution early warning and control mechanisms at urban and regional scales.
基金supported by the National Natural Science Foundation of China(Nos.U19A2044,42105132,42030609,41975037,and 42105133)the National Key Research and Development Program of China(No.2022YFC3703502)+1 种基金the Plan for Anhui Major Provincial Science&Technology Project(No.202203a07020003)Hefei Ecological Environment Bureau Project(No.2020BFFFD01804).
摘要As a significant city in the Yangtze River Delta regions,Hefei has experienced rapid changes in the sources of air pollution due to its high-speed economic development and urban expansion.However,there has been limited research in recent years on the spatial-temporal distribution and emission of its atmospheric pollutants.To address this,this study conducted mobile observations of urban roads using the Mobile-DOAS instrument from June 2021 to May 2022.The monitoring results exhibit a favourable consistent with TROPOMI satellite data and ground monitoring station data.Temporally,there were pronounced seasonal variations in air pollutants.Spatially,high concentration of HCHO and NO2were closely associated with traffic congestion on roadways,while heightened SO2levels were attributed to winter heating and industrial emissions.The study also revealed that with the implementation of road policies,the average vehicle speed increased by 95.4%,while the NO concentration decreased by 54.4%.In the estimation of urban NOxemission flux,it was observed that in temporal terms,compared with inventory data,the emissions calculated viamobile measurements exhibitedmore distinct seasonal patterns,with the highest emission rate of 349 g/sec in winter and the lowest of 142 g/sec in summer.In spatial terms,the significant difference in emissions between the inner and outer ring roads also suggests the presence of the city’s primary NOxemission sources in the area between these two rings.This study offers data support for formulating the next phase of air pollution control measures in urban areas.
基金supported by the Joint Funds of the National Natural Science Foundation of China(No.U21A2027)the New Cornerstone Science Foundation through the XPLORER PRIZE(2023-1033).
摘要This study focuses on the spatiotemporal distribution,urban-rural variations,and driving factors of ammonia Vertical Column Densities(VCDs)in China’s Yangtze River Delta region(YRD)from 2008 to 2020.Utilizing data from the Infrared Atmospheric Sounding Interfer-ometer(IASI),Generalized Additive Models(GAM),and the GEOS-Chem chemical transport model,we observed a significant increase of NH3VCDs in the YRD between 2014 and 2020.The spatial distribution analysis revealed higher NH3concentrations in the northern part of the YRD region,primarily due to lower precipitation,alkaline soil,and intensive agricul-tural activities.NH3VCDs in the YRD region increased significantly(65.18%)from 2008 to 2020.The highest growth rate occurs in the summer,with an annual average growth rate of 7.2%during the period from 2014 to 2020.Agricultural emissions dominated NH3VCDs during spring and summer,with high concentrations primarily located in the agricultural areas adjacent to densely populated urban zones.Regions within several large urban areas have been discovered to exhibit relatively stable variations in NH3VCDs.The rise in NH3VCDs within the YRD region was primarily driven by the reduction of acidic gases like SO2,as emphasized by GAM modeling and sensitivity tests using the GEOS-Chem model.The concentration changes of acidic gases contribute to over 80%of the interannual variations in NH3VCDs.This emphasizes the crucial role of environmental policies targeting the reduction of these acidic gases.Effective emission control is urgent tomitigate environmental hazards and secondary particulate matter,especially in the northern YRD.
摘要Electrocatalytic conversion of carbon dioxide(CO2)offers an effective method of CO2fixation to mitigate global warming and the energy crisis.However,for supported Ni single-atom catalysts(SACs),which are among the most promising candidates for this application,the relationship between Ni coordination structure and catalytic properties is still under strong debate.Here,we fabricated a series of Ni SACs through precise-engineering of anchor sites on nitrogen-doped carbon(NC)followed by Ni atom anchoring using atomic layer deposition.Among them,a Ni1/NC SAC,with a coordination number(CN)of four but less pyridinic nitrogen(Npyri),achieved over 90%faradaic efϐiciency for CO at potentials from-0.7 to-1.0 V and a mass activity of 6.5 A/mgNi at-0.78 V along with high stability,outperforming other Ni SACs with lower CN and more Npyri.Theoretical calculations of various three and four-coordinated Ni1-NxCy structures revealed a linear correlation between the reaction Gibbs free energy for the potential-limiting step and the highest occupied molecular orbital(HOMO)position of Ni-3d orbitals,therein the four-coordinated Ni1-N1C3with the highest HOMO position is identified as the active site for the electrocatalytic CO2-to-CO process,in line with the experimental results.
基金supported by the Innovation and Development Special Project of China Meteorological Administration(Nos.CXFZ2024J011 and CXFZ2024J057)the Key Lab.of Environmental Optics and Technology,CAS(No.2005DP173065-2021-07).
摘要The occurrence of extreme weather events is becoming more frequent due to global climate change.A long-lasting dust outbreak in the spring of 2023 was triggered by Mongolia cyclones and cold fronts in the dust source areas.In this study,we illustrate the spatial distribution,the transport path of the dust and its influence on the air quality of downstream cities utilizing ground-based and space-borne measurements.Results indicate a more complicated pollution,coexisting of polluted dust stage S1 and pure dust stage S2.In S1,the aerosol was characterized by a dual-layer vertical structure—high extinction coefficient of nearly 1.0 km−1with a low particle depolarized ratio(PDR)of1300µg/m3.PM10 positively correlated with trace gases in S1 while varying inversely with the pollution gases in S2.The results help to shed light on the classification of different types of dust and also be useful in developing an effective strategy to forecast air pollution in downstream areas.
基金supported by the National Natural Science Foundation of China(22373092)the National Key Research and Development Program of China(2023YFA1509000)+2 种基金the Innovation Program for Quantum Science and Technology(2021ZD0303306)the Fundamental Research Funds for the Central Universities(WK2060000060)the robotic AI-Scientist platform of Chinese Academy of Science.
摘要Converting CO2to methanol presents a crucial pathway for achieving carbon neutrality,yet designing highly active and selective nano catalysts remain challenging.In this work,we report a combined density functional theory and microkinetic study screening 26 transition metal single atoms(Sc-Zn,Y-Cd,Ta-Au)atomically dispersed in MoS2nanosheet(M1-MoS2)for CO2hydrogenation to methanol.Among these,Ni1-MoS2was identified as a promising candidate,exhibiting excellent stability and hydrogen dissociation capability.The reaction proceeds through a dissociative hydrogenation mechanism via key intermediates including*COOH,*C(OH)2,*CH(OH)2,*CHOH,and*CH2OH.Microkinetic simulations reveal that Ni1-MoS2significantly outperforms the experimentally validated Pt1-MoS2,demonstrating a 26.76-fold enhancement in formation rate and high selectivity under industrial relevant conditions(210℃,8 bar CO2,24 bar H2).This work not only highlights Ni1-MoS2as a highly efficient and cost-effective catalyst but also provides a mechanistic and kinetic framework for accelerating the design of single-atom catalysts for CO2conversion.
基金supported by the National Natural Science Foundation of China(32300776,32370998)the Guangdong Basic and Applied Basic Research Project(2022A1515110460)+2 种基金the Foundation for Basic and Applied Basic Research of Guangzhou(2023A04J0106)the China Postdoctoral Science Foundation(2022M723165)the State Key Laboratory of Respiratory Disease(SKLRD-Z-202211).
摘要Zika virus(ZIKV)infection is associated with severe neurological complications such as congenital microcephaly,yet no safe and effective vaccine is currently available.A critical challenge in ZIKV vaccine development arises from cross-reactive,non-or sub-neutralizing antibodies,which may enhance dengue virus(DENV)infection through antibody-dependent enhancement(ADE).Herein,we report a vaccine strategy utilizing Mi3 nanoparticles to display the envelope(E)protein domain Ⅲ(EDⅢ)of ZIKV,which induces protective immunity against ZIKV infection in murine models.Compared to an EDⅢ subunit vaccine,the Mi3-EDⅢ nanoparticle vaccine elicited significantly higher antibody responses and stronger cell-mediated immune responses.In C57BL/6 mice,maternal immunization with Mi3-EDⅢ protected the neonates against ZIKV-caused symptoms,including body weight loss,neurological abnormalities,retardation of brain development,and mortality.In interferon-α/β receptor knockout(Ifnar1-/-)C57BL/6 mice,Mi3-EDⅢ immunization conferred effective protection against lethal ZIKV challenge.Notably,unlike ZIKV convalescent sera,Mi3-EDⅢ immune sera did not enhance DENV infection in human chronic myelogenous leukemia K562 cells,suggesting the absence of ADE-prone antibody induction.Our results demonstrate that Mi3-EDⅢ is a promising vaccine candidate against ZIKV infection and warrants further development.
摘要The development of straightforward and environmentally friendly techniques for synthesizing organophosphorus compounds with C(sp²)—P bonds would be of great value for the advancement of synthetic chemistry.An electrochemically driven dienylation strategy of arylphosphine oxides with allenylsilanes is reported for the efficient synthesis of dienyl phosphorus compounds.A wide range of dienyl organophosphorus compounds with various functional group tolerance were facilely obtained in moderate to great yield.Mechanistic studies indicate that the desired C(sp²)-P bond is constructed through the radical addition process between the phosphoryl radical and the allene carbon.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.51572001,11404002,and 11404003)the ‘211 Project’ of Anhui University,China(Grant No.J01001319J10113190007)
摘要The transport and thermoelectric properties together with annealing of the new layered Bi-chalcogenide LaOBiHgS3are studied.On the transport part,the insulating behavior of the as-grown sample is evidently depressed by post annealing.A hump-like abnormality appears around 170 K.The thermoelectric performance of the sample is observably improved by the annealing,mainly because of the enhanced electrical conductance.The present results suggest that the physical properties of LaOBiHgS3are sensitive to post annealing and the possible micro adjustments that follow,indicating the layered Bi-chalcogenide family to be an ideal platform for designing novel functional materials.
基金supported by the National Key Research and Development Program of China(No.2020YFC1808204)the National Natural Science Foundation of China(Nos.22206001 and U22A20406)the Scientific Research Foundation of Education Department of Anhui Province of China(No.KJ2021A0074).
摘要Nanoplastics are emerging contaminants that may co-exist with organochlorine pesticides and adversely affect invertebrates in the environment.However,the impact of environmental aging on the combined toxicity of nanoplastics and organochlorine pesticides remains unclear.This study investigated the effects of aging on the combined toxicity of polystyrene nanoplastics(PS NPs)and chlordane against Caenorhabditis elegans.The results showed that photo-aging altered the physicochemical properties of PS NPs and promoted the combined toxicity of PS NPs and chlordane to nematodes by reducing survival rate,body length and enhancing germline apoptosis.Additionally,combined exposure of nematodes to aged PS NPs and chlordane significantly increased reactive oxygen species production and intestinal permeability,suggesting that aging enhances combined toxicity through oxidative stress and intestinal damage.Moreover,aging increased chlordane contents in nematodes without promoting PS NPs accumulation,potentially leading to increased combined toxicity of PS NPs and chlordane.Notably,aging significantly increased the accumulation of PS NPs in the posterior intestine of the nematode during co-exposure,which may be responsible for the most sensitive and highest degree of change in germline apoptosis.These observations emphasize the significance of accounting for environmental aging as well as the accumulation and distribution of nanoplastics in organisms when assessing the combined effects of nanoplastics and coexisting pollutants.
基金supported by grants from the Special Foundation of President of the Chinese Academy of Sciences(Grant No.,YZJJ2020QN27,YZJJ2021QN33)Anhui Provincial Natural Science Foundation(Grant No.,2108085MC79).
摘要HCLS1-associated protein X-1(HAX1)is a multifunctional mitochondrial protein involved in the regulation of apoptosis,a crucial process of programmed cell death,and mRNA processing.Despite its significance,limited structural data is available for HAX1,hindering a comprehensive understanding of its biological function.Notably,the caseinolytic mitochondrial matrix peptidase chaperone subunit B(CLPB)has been identified as an interacting partner of HAX1,yet the biophysical properties and binding affinity governing their interaction remain poorly defined.In this study,we present a thorough biophysical characterization of full-length human HAX1 and CLPB,accomplished through recombinant expression and purification.By employing size exclusion chromatography,dynamic light scattering,and circular dichroism spectroscopy,we successfully established their biophysical properties,revealing contrasting structural features,with CLPB displaying a-helical content and HAX1 exhibiting a disordered nature.Moreover,we employed solutionstate nuclear magnetic resonance(NMR)spectroscopy to probe their binding affinity.Our findings demonstrate the formation of stable multimeric complexes between HAX1 and CLPB,and we quantified a dissociation constant in the low range of micro-molar for their high affinity interaction.These results lay the foundation for further in-depth investigations into the dynamics and energetics governing the HAX1-CLPB interaction,ultimately contributing to a comprehensive understanding of their functional mechanisms.
基金Project supported by the National Key Research and Development Program of China (Grant No. 2023YFA1406500)the National Natural Science Foundation of China (Grant Nos. 12474098, 12274388, 12174361, 12404191, 52102333, 12404043, and 12204004)the Natural Science Foundation of Anhui Province (Grant No. 2408085QA024)。
摘要We report the magnetic and transport properties of EuBi2 single crystal. EuBi2 exhibits complex magnetic behavior at low temperatures. In both the in-plane and out-of-plane directions, three antiferromagnetic(AFM) transitions have been observed at TN1~18.9 K, TN2~7.0 K, and TN3~3.1 K. Among them, the transitions at TN2 and TN3 represent the canted AFM orders with ferromagnetic components. As the magnetic field increases, the transition at TN3 is rapidly suppressed to disappearance. However, the transitions at TN1 and TN2 persist until high fields and their signatures can also be reflected in the resistivity and specific heat. Above the magnetic transition temperature TN1, the resistivity of EuBi2 increases linearly with temperature, exhibiting the strange-metal behavior. In the magnetically ordered region below TN1, EuBi2 exhibits the weak antilocalization(WAL) effect and large magnetoresistance(475% at 1.8 K and 14 T). It is suggested that the magnetic ordering significantly enhances the spin–orbital coupling interaction and induces the WAL effect.
基金supported by the National Key R&D Program of China(Grant Nos.2023YFA1406500,2024YFA1409002,and 2021YFA1400300)the National Natural Science Foundation of China(Grant Nos.12474098,12574042,12274388,12404043,12074425,and 12204004)+4 种基金the Natural Science Foundation of Anhui Province(Grant No.2408085QA024)the Science and Technology Projects in Guangzhou(Grant No.2023A04J1936)the Fundamental Research Funds for the Central Universities(Peking University)the Research Funds of Renmin University of China(Grant No.23XNKJ22)the Beijing National Laboratory for Condensed Matter Physics(Grant No.2023BNLCMPKF008)。
摘要The variation of the effective mass m*of carrier is often overlooked in experimental studies on quantum oscillations and Kohler's rule.Here,we report the magnetotransport properties of La3Sc Bi5and reveal the changing m*in it.The temperature and magnetic field dependence of m*follows the power-law scaling behavior at low temperature and leads to the failure of conventional analysis,which should not be ignored.In the analysis of the thermal factor and Dingle plot of de Haas-van Alphen oscillation in La3ScBi5,satisfactory fitting results can be obtained after considering the correction of m*.We have also applied this method to Sr1-yMn1-zSb2,solving the remaining fitting problem in previous reports.Moreover,the magnetoresistance(MR)of La3ScBi5has been found to violate Kohler's rule.Although the extended Kohler's rule is applicable to high-temperature MR data,it does not scale the low-temperature data well.We further modified the extended Kohler's rule by introducing m*,and subsequently scaled the low-temperature MR data well.Our study emphasizes the importance of considering the variation of m*in the analysis of quantum oscillations and Kohler's rule,and provides a method for extracting the temperature and magnetic field dependence of m*through quantum oscillations,which is very beneficial for the data analysis of other materials in the future.
基金Project supported by the National Key R&D Program of China(Grant No.2022YFA1403203)the National Natural Science Foundation of China(Grant Nos.12204007,12374133,12304162,and 12074002)+5 种基金the Key Scientific Research Foundation of the Education Department of Anhui Province(Grant No.2024AH050046)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302802)Quantum Science and TechnologyNational Science and Technology Major Project(Grant No.2024ZD0301300)the Major Basic Program of Natural Science Foundation of Shandong Province(Grant No.ZR2021ZD01)the Start-up Funding Program of Guangdong-Hong Kong-Macao Greater Bay Area Quantum Science Center(Grant No.QD2301003)Guangdong Provincial Quantum Science Strategic Initiative(Grant No.GDZX2401001)。
摘要Oxygen deficiency is known to critically influence the superconductivity of La3Ni2O7-δ.However,precise control of oxygen content to mitigate such deficiencies remains a significant challenge.In this work,we synthesized high-oxygencontent La3Ni2O7+δpolycrystals via high-pressure oxygen annealing with the oxygen stoichiometry(δ)successfully tuned by varying the amount of KClO4.The obtained samples La3Ni2O7.16and La3Ni2O7.38exhibit metallic behavior at ambient pressure.We further conducted a comprehensive investigation into the pressure-induced superconductivity and atomic structure.STEM imaging revealed large-area bilayer-phase stacking in La3Ni2O7.16,while La3Ni2O7.38showed noticeable intergrowth with other Ruddlesden-Popper(R-P)phases.Notably,the critical pressure in La3Ni2O7.16is substantially reduced,though its critical temperature(Tc)is lower than that of as-grown samples.In contrast,only a weak superconducting signal was detected in higher oxygen content sample La3Ni2O7.38likely due to the intergrowth with other R-P phases,nonnegligible interstitial oxygen,or an increased fraction of the tetragonal phase.Our findings provide a viable pathway for optimizing nickelate superconductivity and offer insights into the fundamental mechanisms governing superconductivity in these materials.
摘要Developing sustainable and efficient methods for the transformation of 1,3-dicarbonyl compounds and alkene functionalization represents a pivotal endeavor for advancing the frontiers of synthetic organic chemistry.Herein,an electrochemically driven functionalization reaction of 1,3-dicarbonyl compounds and alkenes is reported,which enables the efficient construction of α-alkylated 1,3-dicarbonyl compounds.This protocol avoids additional chemical oxidantseductants,proceeds under mild and environmentally benign conditions,and exhibits excellent functional group tolerance,furnishing a diverse array of target products in moderate to good yields.Mechanistic studies indicate that electrochemically generated 1,3-dicarbonyl radicals add to alkenes,followed by single-electron transfer(SET)oxidation and nucleophilic alcohol quenching,thereby realizing efficient alkene functionalization.