Using the outputs from 16 chemistry-climate models(CCMs), the trends of lower- to mid-stratospheric water vapor(WV) during the period 1980–2005 were studied. Comparisons were made between the CCM results and European...Using the outputs from 16 chemistry-climate models(CCMs), the trends of lower- to mid-stratospheric water vapor(WV) during the period 1980–2005 were studied. Comparisons were made between the CCM results and European Centre for Medium-Range Weather Forecasts(ECMWF) Interim Reanalysis(ERA-Interim).The results of most of the CCMs, and those based on ERA-Interim, showed the trends of lower- to mid-stratospheric WV during the period 1980–2005 to be positive, with the extent of the trend increasing with altitude. The trend of lower- to mid-stratospheric WV in the ensemble mean of the CCMs was 0.03 ppmv per decade,which was about twice as large as that based on ERA-Interim. The authors also used a state-of-the-art general circulation model to evaluate the impacts of greenhouse gas(GHG) concentration increases and ozone depletion on stratospheric WV. The simulation results showed that the increases of lower- to mid-stratospheric WV affected by the combined effects of GHG and ozone changes happened mainly via warming of the tropopause and enhancement of the Brewer-Dobson circulation(BDC), with the former being the greater contributor.GHG increase led to a higher and warmer tropopause with stronger BDC, which in turn led to more WV entering the stratosphere; while ozone depletion led to a higher and cooler tropopause, which caused the decreases of lowerto mid-stratospheric WV, despite also causing stronger BDC.展开更多
Due to the significant changes they bring to high latitude stratospheric temperature and wind,stratospheric sudden warmings(SSWs)can have an impact on the propagation and energy distribution of gravity waves(GWs).The ...Due to the significant changes they bring to high latitude stratospheric temperature and wind,stratospheric sudden warmings(SSWs)can have an impact on the propagation and energy distribution of gravity waves(GWs).The variation characteristics of GWs during SSWs have always been an important issue.Using temperature data from January to March in 2014−2016,provided by the Constellation Observing System for Meteorology,Ionosphere and Climate(COSMIC)mission,we have analyzed global GW activity at 15−40 km in the Northern Hemisphere during SSW events.During the SSWs that we studied,the stratospheric temperature rose in one or two longitudinal regions in the Northern Hemisphere;the areas affected extended to the east of 90°W.During these SSWs,the potential energy density(E_(p)of GWs expanded and covered a larger range of longitude and altitude,exhibiting an eastward and downward extension.The E_(p)usually increased,while partially filtered by the eastward zonal winds.When zonal winds weakened or turned westward,E_(p)began to strengthen.After SSWs,the E_(p)usually decreased.These observations can serve as a reference for analyzing the interaction mechanism between SSWs and GWs in future work.展开更多
Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redo...Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.展开更多
We derive the potential energy of gravity waves(GWs)in the upper troposphere and stratosphere at 45°S-45°N from December 2019 to November 2022 by using temperature profiles retrieved from the Constellation O...We derive the potential energy of gravity waves(GWs)in the upper troposphere and stratosphere at 45°S-45°N from December 2019 to November 2022 by using temperature profiles retrieved from the Constellation Observing System for Meteorology,Ionosphere,and Climate-2(COSMIC-2)satellite.Owing to the dense sampling of COSMIC-2,in addition to the strong peaks of gravity wave potential energy(GWPE)above the Andes and Tibetan Plateau,we found weak peaks above the Rocky,Atlas,Caucasus,and Tianshan Mountains.The land-sea contrast is responsible for the longitudinal variations of the GWPE in the lower and upper stratosphere.At 40°N/S,the peaks were mainly above the topographic regions during the winter.At 20°N/S,the peaks were a slight distance away from the topographic regions and might be the combined effect of nontopographic GWs and mountain waves.Near the Equator,the peaks were mainly above the regions with the lowest sea level altitude and may have resulted from convection.Our results indicate that even above the local regions with lower sea level altitudes compared with the Andes and Tibetan Plateau,the GWPE also exhibits fine structures in geographic distributions.We found that dissipation layers above the tropopause jet provide the body force to generate secondary waves in the upper stratosphere,especially during the winter months of each hemisphere and at latitudes of greater than 20°N/S.展开更多
P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phas...P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.展开更多
New results presented in the 2023 MRE HP Special Volume clearly demonstrate the cross-disciplinary synergistic progress in high-pressure physics and chemistry.The prevalence of pressure-induced crystal chemistry of cl...New results presented in the 2023 MRE HP Special Volume clearly demonstrate the cross-disciplinary synergistic progress in high-pressure physics and chemistry.The prevalence of pressure-induced crystal chemistry of clathrate-like host-guest cages in borides,^(1,2)nitrides,^(3)and hydrides^(4)has led to exotic compositions and physical properties.展开更多
The representation of the Arctic stratospheric circulation and the quasi-biennial oscillation(QBO)during the period 1981–2019 in a 40-yr Chinese global reanalysis dataset(CRA-40)is evaluated by comparing two widely u...The representation of the Arctic stratospheric circulation and the quasi-biennial oscillation(QBO)during the period 1981–2019 in a 40-yr Chinese global reanalysis dataset(CRA-40)is evaluated by comparing two widely used reanalysis datasets,ERA-5 and MERRA-2.CRA-40 demonstrates a comparable performance with ERA-5 and MERRA-2 in characterizing the winter and spring circulation in the lower and middle Arctic stratosphere.Specifically,differences in the climatological polar-mean temperature and polar night jet among the three reanalyses are within±0.5 K and±0.5 m s^(–1),respectively.The onset dates of the stratospheric sudden warming and stratospheric final warming events at 10 hPa in CRA-40,together with the dynamics and circulation anomalies during the onset process of warming events,are nearly identical to the other two reanalyses with slight differences.By contrast,the CRA-40 dataset demonstrates a deteriorated performance in describing the QBO below 10 hPa compared to the other two reanalysis products,manifested by the larger easterly biases of the QBO index,the remarkably weaker amplitude of the QBO,and the weaker wavelet power of the QBO period.Such pronounced biases are mainly concentrated in the period 1981–98 and largely reduced by at least 39%in 1999–2019.Thus,particular caution is needed in studying the QBO based on CRA-40.All three reanalyses exhibit greater disagreement in the upper stratosphere compared to the lower and middle stratosphere for both the polar region and the tropics.展开更多
Utilizing the European Centre for Medium-Range Weather Forecast(ECMWF)Reanalysis v5(ERA5),for the first time,we have confirmed close links among Sudden Stratospheric Warmings(SSWs)in the Northern Hemisphere(NH),the po...Utilizing the European Centre for Medium-Range Weather Forecast(ECMWF)Reanalysis v5(ERA5),for the first time,we have confirmed close links among Sudden Stratospheric Warmings(SSWs)in the Northern Hemisphere(NH),the polar vortices,and stratospheric Planetary Waves(PWs)by analyzing and comparing their trends.Interestingly,within overall increasing trends,the duration and strength of SSWs exhibit increasing and decreasing trends before and after the winter of 2002,respectively.To reveal possible physical mechanisms driving these trends,we analyzed the long-term trends of the winter(from December to February)polar vortices and of stratospheric PWs with zonal wave number 1.Notably,our results show that in all three time periods(the entire period of 41winters,1980 to 2020,and the two subperiods—1980-2002 and 2002-2020)enhancing SSWs were always accompanied by weakening winter polar vortices and strengthening polar PWs like Stationary Planetary Waves(SPWs)and 16-day waves,and vice versa.This is the first proof,based on ERA5 long-term trend data,that weakening polar vortices and enhancing stratospheric PWs(especially SPWs)could cause an increase in SSWs.展开更多
MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical str...MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical strength,etc.This review begins by presenting MXenes,providing insights into their structural characteristics,synthesis methods,and surface functional groups.The review covers a thorough analysis of MXene surface properties,including surface chemistry and termination group impacts.The properties of MXenes are influenced by their synthesis,which can be fluorine-based or fluorinedependent.Fluorine-based synthesis techniques involve etching with fluorine-based reagents,mainly including HF or LiF/HCl,while fluorine-free methods include electrochemical etching,chemical vapor deposition(CVD),alkaline etching,Lewis acid-based etching,etc.These techniques result in the emergence of functional groups such as-F,-O,-OH,-Cl,etc.on the MXenes surface,depending on the synthesis method used.Properties of MXenes,such as electrical conductivity,electronic properties,catalytic activity,magnetic properties,mechanical strength,and chemical and thermal stability,are examined,and the role of functional groups in determining these properties is explored.The review delves into the diverse applications of MXenes,encompassing supercapacitors,battery materials,hydrogen storage,fuel cells,electromagnetic interference(EMI) shielding,pollutant removal,water purification,flexible electronics,sensors,additive manufacturing,catalysis,biomedical and healthcare fields,etc.Finally,this article outlines the challenges and opportunities in the current and future development of MXenes research,addressing various aspects such as synthesis scalability,etching challenges,and multifunctionality,and exploring novel applications.The review concludes with future prospects and conclusions envisioning the impact of MXenes on future technologies and innovation.展开更多
Rechargeable lithium-sulfur(Li-S)batteries,featuring high energy density,low cost,and environmental friendliness,have been dubbed as one of the most promising candidates to replace current commercial rechargeable Li-i...Rechargeable lithium-sulfur(Li-S)batteries,featuring high energy density,low cost,and environmental friendliness,have been dubbed as one of the most promising candidates to replace current commercial rechargeable Li-ion batteries.However,their practical deployment has long been plagued by the infamous“shuttle effect”of soluble Li polysulfides(LiPSs)and the rampant growth of Li dendrites.Therefore,it is important to specifically elucidate the solvation structure in the Li-S system and systematically summarize the feasibility strategies that can simultaneously suppress the shuttle effect and the growth of Li dendrites for practical applications.This review attempts to achieve this goal.In this review,we first introduce the importance of developing Li-S batteries and highlight the key challenges.Then,we revisit the working principles of Li-S batteries and underscore the fundamental understanding of LiPSs.Next,we summarize some representative characterization techniques and theoretical calculations applied to characterize the solvation structure of LiPSs.Afterward,we overview feasible designing strategies that can simultaneously suppress the shuttle effect of soluble LiPSs and the growth of Li dendrites.Finally,we conclude and propose personal insights and perspectives on the future development of Li-S batteries.We envisage that this timely review can provide some inspiration to build better Li-S batteries for promoting practical applications.展开更多
Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehe...Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehensive overview of recent advancements in the plasma-enabled synthesis of life’s building blocks, charting the complex environmental parameters believed to have surrounded life’s inception. This discussion elaborates on the fundamental mechanisms of discharge plasmas and their likely role in fostering conditions necessary for the origin of life on early Earth. We consider a variety of chemical reactions facilitated by plasma, specifically the synthesis of vital organic molecules - amino acids, nucleobases, sugars, and lipids. Further, we delve into the impact of plasmas on prebiotic chemical evolution. We expect this review to open new horizons for future investigations in plasma-related prebiotic chemistry that could offer valuable insights for unraveling the mysteries of life's origin.展开更多
Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with th...Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with the continuous development of material systems and modification strategies,researchers have gradually found that D-band center theory is usually effective for large metal particle systems,but for small metal particle systems or semiconductors,such as single atom systems,the opposite conclusion to the D-band center theory is often obtained.To solve the issue above,here we propose a bonding and anti-bonding orbitals stable electron intensity difference(BASED)theory for surface chemistry.The newly-proposed BASED theory can not only successfully explain the abnormal phenomena of D-band center theory,but also exhibits a higher accuracy for prediction of adsorption energy and bond length of intermediates on active sites.Importantly,a new phenomenon of the spin transition state in the adsorption process is observed based on the BASED theory,where the active center atom usually yields an unstable high spin transition state to enhance its adsorption capability in the adsorption process of intermediates when their distance is about 2.5Å.In short,the BASED theory can be considered as a general principle to understand catalytic mechanism of intermediates on surfaces.展开更多
Downward transport of stratospheric air into the troposphere(identified as stratospheric intrusions)could potentially modify the radiation budget and chemical of the Earth's surface atmosphere.As the highest and l...Downward transport of stratospheric air into the troposphere(identified as stratospheric intrusions)could potentially modify the radiation budget and chemical of the Earth's surface atmosphere.As the highest and largest plateau on earth,the Tibetan Plateau including the Himalayas couples to global climate,and has attracted widespread attention due to rapid warming and cryospheric shrinking.Previous studies recognized strong stratospheric intrusions in the Himalayas but are poorly understood due to limited direct evidences and the complexity of the meteorological dynamics of the third pole.Cosmogenic^(35)S is a radioactive isotope predominately produced in the lower stratosphere and has been demonstrated as a sensitive chemical tracer to detect stratospherically sourced air mass in the planetary boundary layer.Here,we report 6-month(April–September 2018)observation of^(35)S in atmospheric sulfate aerosols(^(35)SO_(4)^(2-))collected from a remote site in the Himalayas to reveal the stratospheric intrusion phenomenon as well as its potential impacts in this region.Throughout the sampling campaign,the^(35)SO_(4)^(2-)concentrations show an average of 1,070±980 atoms/m^(3).In springtime,the average is 1,620±730 atoms/m^(3),significantly higher than the global existing data measured so far.The significant enrichments of^(35)SO_(4)^(2-)measured in this study verified the hypothesis that the Himalayas is a global hot spot of stratospheric intrusions,especially during the springtime as a consequence of its unique geology and atmospheric couplings.In combined with the ancillary evidences,e.g.,oxygen-17 anomaly in sulfate and modeling results,we found that the stratospheric intrusions have a profound impact on the surface ozone concentrations over the study region,and potentially have the ability to constrain how the mechanisms of sulfate oxidation are affected by a change in plateau atmospheric properties and conditions.This study provides new observational constraints on stratospheric intrusions in the Himalayas,which would further provide additional information for a deeper understanding on the environment and climatic changes over the Tibetan Plateau.展开更多
The undesirable capacity loss after first cycle is universal among layered cathode materials,which results in the capacity and energy decay.The key to resolving this obstacle lies in understanding the effect and origi...The undesirable capacity loss after first cycle is universal among layered cathode materials,which results in the capacity and energy decay.The key to resolving this obstacle lies in understanding the effect and origin of specific active Li sites during discharge process.In this study,focusing on Ah-level pouch cells for reliability,an ultrahigh initial Coulombic efficiency(96.1%)is achieved in an archetypical Li-rich layered oxide material.Combining the structure and electrochemistry analysis,we demonstrate that the achievement of high-capacity reversibility is a kinetic effect,primarily related to the sluggish Li mobility during oxygen reduction.Activating oxygen reduction through small density would induce the oxygen framework contraction,which,according to Pauli repulsion,imposes a great repulsive force to hinder the transport of tetrahedral Li.The tetrahedral Li storage upon deep oxygen reduction is experimentally visualized and,more importantly,contributes to 6%Coulombic efficiency enhancement as well as 10%energy density improvement for pouch cells,which shows great potentials breaking through the capacity and energy limitation imposed by intercalation chemistry.展开更多
Physical chemistry experiments are an important branch of chemical experiments.In view of problems and shortcomings in physical chemistry experiment teaching of food quality and safety major in Chengdu University,the ...Physical chemistry experiments are an important branch of chemical experiments.In view of problems and shortcomings in physical chemistry experiment teaching of food quality and safety major in Chengdu University,the teaching methods of physical chemistry experiment course of food quality and safety major were explored and practiced,aiming to arouse students enthusiasm for experiments and cultivate their ability of independent learning,comprehensive thinking and independent problem solving.展开更多
Rechargeable magnesium batteries(RMBs),as a low-cost,high-safety and high-energy storage technology,have attracted tremendous attention in large-scale energy storage applications.However,the key anode/electrolyte inte...Rechargeable magnesium batteries(RMBs),as a low-cost,high-safety and high-energy storage technology,have attracted tremendous attention in large-scale energy storage applications.However,the key anode/electrolyte interfacial issues,including surface passivation,uneven Mg plating/stripping,and pulverization after cycling still result in a large overpotential,short cycling life,poor power density,and possible safety hazards of cells,severely impeding the commercial development of RMBs.In this review,a concise overview of recently advanced strategies to address these anode/electroyte interfacial issues is systematically classified and summarized.The design of magnesiophilic substrates,construction of artificial SEI layers,and modification of electrolyte are important and effective strategies to improve the uniformity/kinetics of Mg plating/stripping and achieve the stable anode/electrolyte interface.The key opportunities and challenges in this field are advisedly put forward,and the insights into future directions for stabilizing Mg metal anodes and the anode/electrolyte interface are highlighted.This review provides important references fordeveloping the high-performance and high-safety RMBs.展开更多
An engineering system approach of 2-D cylindrical model of transient mass balance calculations of ozone and other concerned chemicals along with fourteen photolysis, ozone-generating and ozone-depleting chemical react...An engineering system approach of 2-D cylindrical model of transient mass balance calculations of ozone and other concerned chemicals along with fourteen photolysis, ozone-generating and ozone-depleting chemical reaction equations was developed, validated, and used for studying the ozone concentrations, distribution and peak of the layer, ozone depletion and total ozone abundance in the stratosphere. The calculated ozone concentrations and profile at both the Equator and a 60˚N location were found to follow closely with the measured data. The calculated average ozone concentration was within 1% of the measured average, and the deviation of ozone profiles was within 14%. The monthly evolution of stratospheric ozone concentrations and distribution above the Equator was studied with results discussed in details. The influences of slow air movement in both altitudinal and radial directions on ozone concentrations and profile in the stratosphere were explored and discussed. Parametric studies of the influences of gas diffusivities of ozone D<sub>O3</sub> and active atomic oxygen D<sub>O</sub> on ozone concentrations and distributions were also studied and delineated. Having both influences through physical diffusion and chemical reactions, the diffusivity (and diffusion) of atomic oxygen D<sub>O</sub> was found to be more sensitive and important than that of ozone D<sub>O3</sub> on ozone concentrations and distribution. The 2-D ozone model present in this paper for stratospheric ozone and its layer and depletion is shown to be robust, convenient, efficient, and executable for analyzing the complex ozone phenomena in the stratosphere. .展开更多
Integrating ideological and political theories teaching into the whole process of classroom teaching construction is a new requirement for implementing the fundamental task of cultivating people by virtue and playing ...Integrating ideological and political theories teaching into the whole process of classroom teaching construction is a new requirement for implementing the fundamental task of cultivating people by virtue and playing the role of collaborative education.In order to realize the seamless integration of inorganic and analytical chemistry courses and ideological and political education,this paper summarizes the current situation of ideological and political research on inorganic and analytical chemistry courses in three major databases in China(VIP,CNKI and Wanfang),and sorts out the knowledge points,ideological and political elements and educational goals according to the content of the course chapters,to provide a basic guarantee for the ideological and political education construction of the course.展开更多
Green analytical chemistry(GAC)focuses on mitigating the adverse effects of analytical activities on human safety,human health,and environment.In addition to the 12 principles of GAC,proper GAC tools should be develop...Green analytical chemistry(GAC)focuses on mitigating the adverse effects of analytical activities on human safety,human health,and environment.In addition to the 12 principles of GAC,proper GAC tools should be developed and employed to assess the greenness of different analytical assays.The 15 widely used GAC metrics,i.e.,national environmental methods index(NEMI),advanced NEMI,assessment of green profile(AGP),chloroform-oriented toxicity estimation scale(ChlorTox Scale),Analytical Eco-Scale,Green Certificate Modified Eco-Scale,analytical method greenness score(AMGS),green analytical procedure index(GAPI),ComplexGAPI,red-green-blue(RGB)additive color model,RGB 12 algorithm,analytical greenness calculator(AGREE),AGREE preparation(AGREEprep),HEXAGON,and blue applicability grade index(BAGI),are selected as the typical tools.This article comprehensively presents and elucidates the principles,characteristics,merits,and demerits of 15 widely used GAC tools.This review is helpful for researchers to use the current GAC metrics to assess the environmental sustainability of analytical assays.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos. 41225018 and 41305036)
文摘Using the outputs from 16 chemistry-climate models(CCMs), the trends of lower- to mid-stratospheric water vapor(WV) during the period 1980–2005 were studied. Comparisons were made between the CCM results and European Centre for Medium-Range Weather Forecasts(ECMWF) Interim Reanalysis(ERA-Interim).The results of most of the CCMs, and those based on ERA-Interim, showed the trends of lower- to mid-stratospheric WV during the period 1980–2005 to be positive, with the extent of the trend increasing with altitude. The trend of lower- to mid-stratospheric WV in the ensemble mean of the CCMs was 0.03 ppmv per decade,which was about twice as large as that based on ERA-Interim. The authors also used a state-of-the-art general circulation model to evaluate the impacts of greenhouse gas(GHG) concentration increases and ozone depletion on stratospheric WV. The simulation results showed that the increases of lower- to mid-stratospheric WV affected by the combined effects of GHG and ozone changes happened mainly via warming of the tropopause and enhancement of the Brewer-Dobson circulation(BDC), with the former being the greater contributor.GHG increase led to a higher and warmer tropopause with stronger BDC, which in turn led to more WV entering the stratosphere; while ozone depletion led to a higher and cooler tropopause, which caused the decreases of lowerto mid-stratospheric WV, despite also causing stronger BDC.
基金the National Science Foundation of Hunan Province,China(Grant No.2022JJ40471)the Research Foundation of the Education Bureau of Hunan Province,China(Grant No.22B0345)the Key Laboratory of Geospace Envi-ronment,Chinese Academy of Sciences,University of Science&Technology of China(Grant No.GE2023-01).
文摘Due to the significant changes they bring to high latitude stratospheric temperature and wind,stratospheric sudden warmings(SSWs)can have an impact on the propagation and energy distribution of gravity waves(GWs).The variation characteristics of GWs during SSWs have always been an important issue.Using temperature data from January to March in 2014−2016,provided by the Constellation Observing System for Meteorology,Ionosphere and Climate(COSMIC)mission,we have analyzed global GW activity at 15−40 km in the Northern Hemisphere during SSW events.During the SSWs that we studied,the stratospheric temperature rose in one or two longitudinal regions in the Northern Hemisphere;the areas affected extended to the east of 90°W.During these SSWs,the potential energy density(E_(p)of GWs expanded and covered a larger range of longitude and altitude,exhibiting an eastward and downward extension.The E_(p)usually increased,while partially filtered by the eastward zonal winds.When zonal winds weakened or turned westward,E_(p)began to strengthen.After SSWs,the E_(p)usually decreased.These observations can serve as a reference for analyzing the interaction mechanism between SSWs and GWs in future work.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(2021B1515120072)the Natural Science Foundation of China(22279096 and T2241003)the Fundamental Research Funds for the Central Universities(WUT:2023IVA094).
文摘Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.
基金the National Natural Science Foundation of China(Grant Nos.41831073,42174196,and 42374205)the Project of Stable Support for Youth Team in Basic Research Field,Chinese Academy of Sciences(CAS+4 种基金Grant No.YSBR-018)the Informatization Plan of CAS(Grant No.CAS-WX2021PY-0101)the Youth Cross Team Scientific Research project of the Chinese Academy of Sciences(Grant No.JCTD-2021-10)the Open Research Project of Large Research Infrastructures of CAS titled“Study on the Interaction Between Low-/Mid-Latitude Atmosphere and Ionosphere Based on the Chinese Meridian Project.”This work was also supported in part by the Specialized Research Fund and the Open Research Program of the State Key Laboratory of Space Weather.
文摘We derive the potential energy of gravity waves(GWs)in the upper troposphere and stratosphere at 45°S-45°N from December 2019 to November 2022 by using temperature profiles retrieved from the Constellation Observing System for Meteorology,Ionosphere,and Climate-2(COSMIC-2)satellite.Owing to the dense sampling of COSMIC-2,in addition to the strong peaks of gravity wave potential energy(GWPE)above the Andes and Tibetan Plateau,we found weak peaks above the Rocky,Atlas,Caucasus,and Tianshan Mountains.The land-sea contrast is responsible for the longitudinal variations of the GWPE in the lower and upper stratosphere.At 40°N/S,the peaks were mainly above the topographic regions during the winter.At 20°N/S,the peaks were a slight distance away from the topographic regions and might be the combined effect of nontopographic GWs and mountain waves.Near the Equator,the peaks were mainly above the regions with the lowest sea level altitude and may have resulted from convection.Our results indicate that even above the local regions with lower sea level altitudes compared with the Andes and Tibetan Plateau,the GWPE also exhibits fine structures in geographic distributions.We found that dissipation layers above the tropopause jet provide the body force to generate secondary waves in the upper stratosphere,especially during the winter months of each hemisphere and at latitudes of greater than 20°N/S.
基金supported by the National Natural Science Foundation of China (22169002)the Chongzuo Key Research and Development Program of China (20220603)the Counterpart Aid Project for Discipline Construction from Guangxi University(2023M02)
文摘P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.
基金financial support from the Shanghai Key Laboratory of MFree,China(Grant No.22dz2260800)the Shanghai Science and Technology Committee,China(Grant No.22JC1410300)。
文摘New results presented in the 2023 MRE HP Special Volume clearly demonstrate the cross-disciplinary synergistic progress in high-pressure physics and chemistry.The prevalence of pressure-induced crystal chemistry of clathrate-like host-guest cages in borides,^(1,2)nitrides,^(3)and hydrides^(4)has led to exotic compositions and physical properties.
基金supported by the National Natural Science Foundation of China (Grant Nos. 41975048, 42030605, and 42175069)the Natural Science Foundation of Jiangsu Province (Grant No.BK20191404)
文摘The representation of the Arctic stratospheric circulation and the quasi-biennial oscillation(QBO)during the period 1981–2019 in a 40-yr Chinese global reanalysis dataset(CRA-40)is evaluated by comparing two widely used reanalysis datasets,ERA-5 and MERRA-2.CRA-40 demonstrates a comparable performance with ERA-5 and MERRA-2 in characterizing the winter and spring circulation in the lower and middle Arctic stratosphere.Specifically,differences in the climatological polar-mean temperature and polar night jet among the three reanalyses are within±0.5 K and±0.5 m s^(–1),respectively.The onset dates of the stratospheric sudden warming and stratospheric final warming events at 10 hPa in CRA-40,together with the dynamics and circulation anomalies during the onset process of warming events,are nearly identical to the other two reanalyses with slight differences.By contrast,the CRA-40 dataset demonstrates a deteriorated performance in describing the QBO below 10 hPa compared to the other two reanalysis products,manifested by the larger easterly biases of the QBO index,the remarkably weaker amplitude of the QBO,and the weaker wavelet power of the QBO period.Such pronounced biases are mainly concentrated in the period 1981–98 and largely reduced by at least 39%in 1999–2019.Thus,particular caution is needed in studying the QBO based on CRA-40.All three reanalyses exhibit greater disagreement in the upper stratosphere compared to the lower and middle stratosphere for both the polar region and the tropics.
基金supported by the National Key RandD Program of China(2022YFF0503703)the National Natural Science Foundation of China(through grant42127805)。
文摘Utilizing the European Centre for Medium-Range Weather Forecast(ECMWF)Reanalysis v5(ERA5),for the first time,we have confirmed close links among Sudden Stratospheric Warmings(SSWs)in the Northern Hemisphere(NH),the polar vortices,and stratospheric Planetary Waves(PWs)by analyzing and comparing their trends.Interestingly,within overall increasing trends,the duration and strength of SSWs exhibit increasing and decreasing trends before and after the winter of 2002,respectively.To reveal possible physical mechanisms driving these trends,we analyzed the long-term trends of the winter(from December to February)polar vortices and of stratospheric PWs with zonal wave number 1.Notably,our results show that in all three time periods(the entire period of 41winters,1980 to 2020,and the two subperiods—1980-2002 and 2002-2020)enhancing SSWs were always accompanied by weakening winter polar vortices and strengthening polar PWs like Stationary Planetary Waves(SPWs)and 16-day waves,and vice versa.This is the first proof,based on ERA5 long-term trend data,that weakening polar vortices and enhancing stratospheric PWs(especially SPWs)could cause an increase in SSWs.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2020R1A6A1A03043435 and 2020R1A2C1099862)supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(P0012451,The Competency Development Program for Industry Specialist)。
文摘MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical strength,etc.This review begins by presenting MXenes,providing insights into their structural characteristics,synthesis methods,and surface functional groups.The review covers a thorough analysis of MXene surface properties,including surface chemistry and termination group impacts.The properties of MXenes are influenced by their synthesis,which can be fluorine-based or fluorinedependent.Fluorine-based synthesis techniques involve etching with fluorine-based reagents,mainly including HF or LiF/HCl,while fluorine-free methods include electrochemical etching,chemical vapor deposition(CVD),alkaline etching,Lewis acid-based etching,etc.These techniques result in the emergence of functional groups such as-F,-O,-OH,-Cl,etc.on the MXenes surface,depending on the synthesis method used.Properties of MXenes,such as electrical conductivity,electronic properties,catalytic activity,magnetic properties,mechanical strength,and chemical and thermal stability,are examined,and the role of functional groups in determining these properties is explored.The review delves into the diverse applications of MXenes,encompassing supercapacitors,battery materials,hydrogen storage,fuel cells,electromagnetic interference(EMI) shielding,pollutant removal,water purification,flexible electronics,sensors,additive manufacturing,catalysis,biomedical and healthcare fields,etc.Finally,this article outlines the challenges and opportunities in the current and future development of MXenes research,addressing various aspects such as synthesis scalability,etching challenges,and multifunctionality,and exploring novel applications.The review concludes with future prospects and conclusions envisioning the impact of MXenes on future technologies and innovation.
基金financially supported by the National Natural Science Foundation of China(51972064 and 52222315)
文摘Rechargeable lithium-sulfur(Li-S)batteries,featuring high energy density,low cost,and environmental friendliness,have been dubbed as one of the most promising candidates to replace current commercial rechargeable Li-ion batteries.However,their practical deployment has long been plagued by the infamous“shuttle effect”of soluble Li polysulfides(LiPSs)and the rampant growth of Li dendrites.Therefore,it is important to specifically elucidate the solvation structure in the Li-S system and systematically summarize the feasibility strategies that can simultaneously suppress the shuttle effect and the growth of Li dendrites for practical applications.This review attempts to achieve this goal.In this review,we first introduce the importance of developing Li-S batteries and highlight the key challenges.Then,we revisit the working principles of Li-S batteries and underscore the fundamental understanding of LiPSs.Next,we summarize some representative characterization techniques and theoretical calculations applied to characterize the solvation structure of LiPSs.Afterward,we overview feasible designing strategies that can simultaneously suppress the shuttle effect of soluble LiPSs and the growth of Li dendrites.Finally,we conclude and propose personal insights and perspectives on the future development of Li-S batteries.We envisage that this timely review can provide some inspiration to build better Li-S batteries for promoting practical applications.
基金National Natural Science Foundation of China General Project(52377160)National Natural Science Foundation of China National Young Talents Project(GYKP010)+1 种基金Shaanxi Provincial Natural Science Program(2023-JC-YB-425)Xi′an Jiaotong University Young Top Talents Program.
文摘Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehensive overview of recent advancements in the plasma-enabled synthesis of life’s building blocks, charting the complex environmental parameters believed to have surrounded life’s inception. This discussion elaborates on the fundamental mechanisms of discharge plasmas and their likely role in fostering conditions necessary for the origin of life on early Earth. We consider a variety of chemical reactions facilitated by plasma, specifically the synthesis of vital organic molecules - amino acids, nucleobases, sugars, and lipids. Further, we delve into the impact of plasmas on prebiotic chemical evolution. We expect this review to open new horizons for future investigations in plasma-related prebiotic chemistry that could offer valuable insights for unraveling the mysteries of life's origin.
文摘Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with the continuous development of material systems and modification strategies,researchers have gradually found that D-band center theory is usually effective for large metal particle systems,but for small metal particle systems or semiconductors,such as single atom systems,the opposite conclusion to the D-band center theory is often obtained.To solve the issue above,here we propose a bonding and anti-bonding orbitals stable electron intensity difference(BASED)theory for surface chemistry.The newly-proposed BASED theory can not only successfully explain the abnormal phenomena of D-band center theory,but also exhibits a higher accuracy for prediction of adsorption energy and bond length of intermediates on active sites.Importantly,a new phenomenon of the spin transition state in the adsorption process is observed based on the BASED theory,where the active center atom usually yields an unstable high spin transition state to enhance its adsorption capability in the adsorption process of intermediates when their distance is about 2.5Å.In short,the BASED theory can be considered as a general principle to understand catalytic mechanism of intermediates on surfaces.
基金financially supported by the second Tibetan Plateau Scientific Expedition and Research Program (STEP) (No.2019QZKK0605)the National Natural Science Foundation of China (42371151)+3 种基金the State Key Laboratory of Cryospheric Science (SKLCS-ZZ-2023)the research grant of State Key Laboratory of Isotope Geochemistry (SKLaBIG-KF-22-05)the Natural Science Foundation of Gansu Province (23JRRA648)China Postdoctoral Science Foundation (2022M723358)。
文摘Downward transport of stratospheric air into the troposphere(identified as stratospheric intrusions)could potentially modify the radiation budget and chemical of the Earth's surface atmosphere.As the highest and largest plateau on earth,the Tibetan Plateau including the Himalayas couples to global climate,and has attracted widespread attention due to rapid warming and cryospheric shrinking.Previous studies recognized strong stratospheric intrusions in the Himalayas but are poorly understood due to limited direct evidences and the complexity of the meteorological dynamics of the third pole.Cosmogenic^(35)S is a radioactive isotope predominately produced in the lower stratosphere and has been demonstrated as a sensitive chemical tracer to detect stratospherically sourced air mass in the planetary boundary layer.Here,we report 6-month(April–September 2018)observation of^(35)S in atmospheric sulfate aerosols(^(35)SO_(4)^(2-))collected from a remote site in the Himalayas to reveal the stratospheric intrusion phenomenon as well as its potential impacts in this region.Throughout the sampling campaign,the^(35)SO_(4)^(2-)concentrations show an average of 1,070±980 atoms/m^(3).In springtime,the average is 1,620±730 atoms/m^(3),significantly higher than the global existing data measured so far.The significant enrichments of^(35)SO_(4)^(2-)measured in this study verified the hypothesis that the Himalayas is a global hot spot of stratospheric intrusions,especially during the springtime as a consequence of its unique geology and atmospheric couplings.In combined with the ancillary evidences,e.g.,oxygen-17 anomaly in sulfate and modeling results,we found that the stratospheric intrusions have a profound impact on the surface ozone concentrations over the study region,and potentially have the ability to constrain how the mechanisms of sulfate oxidation are affected by a change in plateau atmospheric properties and conditions.This study provides new observational constraints on stratospheric intrusions in the Himalayas,which would further provide additional information for a deeper understanding on the environment and climatic changes over the Tibetan Plateau.
基金financially supported by the National Natural Science Foundation of China(Grant No.52272253)“Lingyan”Research and Development Plan of Zhejiang Province(Grant No.2022C01071)+2 种基金Low Cost Cathode Material(Grant No.TC220H06P)the Natural Science Foundation of Ningbo(Grant No.202003N4030)the Youth Innovation Promotion Association of Chinese Academy of Sciences(Grant No.2022299)
文摘The undesirable capacity loss after first cycle is universal among layered cathode materials,which results in the capacity and energy decay.The key to resolving this obstacle lies in understanding the effect and origin of specific active Li sites during discharge process.In this study,focusing on Ah-level pouch cells for reliability,an ultrahigh initial Coulombic efficiency(96.1%)is achieved in an archetypical Li-rich layered oxide material.Combining the structure and electrochemistry analysis,we demonstrate that the achievement of high-capacity reversibility is a kinetic effect,primarily related to the sluggish Li mobility during oxygen reduction.Activating oxygen reduction through small density would induce the oxygen framework contraction,which,according to Pauli repulsion,imposes a great repulsive force to hinder the transport of tetrahedral Li.The tetrahedral Li storage upon deep oxygen reduction is experimentally visualized and,more importantly,contributes to 6%Coulombic efficiency enhancement as well as 10%energy density improvement for pouch cells,which shows great potentials breaking through the capacity and energy limitation imposed by intercalation chemistry.
文摘Physical chemistry experiments are an important branch of chemical experiments.In view of problems and shortcomings in physical chemistry experiment teaching of food quality and safety major in Chengdu University,the teaching methods of physical chemistry experiment course of food quality and safety major were explored and practiced,aiming to arouse students enthusiasm for experiments and cultivate their ability of independent learning,comprehensive thinking and independent problem solving.
基金supported by the National Key R&D Program of China(No.2023YFB3809500)the National Natural Science Foundation of China(No.U23A20555,52202211)+3 种基金the Ninth Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)the Chongqing Technology Innovation and Application Development Project(No.CSTB2022TIAD-KPX0028)the Fundamental Research Funds for the Central Universities(2023CDJXY-018)the Venture&Innovation Support Program for Chongqing Overseas Returnees(cx2022119,cx2023087).
文摘Rechargeable magnesium batteries(RMBs),as a low-cost,high-safety and high-energy storage technology,have attracted tremendous attention in large-scale energy storage applications.However,the key anode/electrolyte interfacial issues,including surface passivation,uneven Mg plating/stripping,and pulverization after cycling still result in a large overpotential,short cycling life,poor power density,and possible safety hazards of cells,severely impeding the commercial development of RMBs.In this review,a concise overview of recently advanced strategies to address these anode/electroyte interfacial issues is systematically classified and summarized.The design of magnesiophilic substrates,construction of artificial SEI layers,and modification of electrolyte are important and effective strategies to improve the uniformity/kinetics of Mg plating/stripping and achieve the stable anode/electrolyte interface.The key opportunities and challenges in this field are advisedly put forward,and the insights into future directions for stabilizing Mg metal anodes and the anode/electrolyte interface are highlighted.This review provides important references fordeveloping the high-performance and high-safety RMBs.
文摘An engineering system approach of 2-D cylindrical model of transient mass balance calculations of ozone and other concerned chemicals along with fourteen photolysis, ozone-generating and ozone-depleting chemical reaction equations was developed, validated, and used for studying the ozone concentrations, distribution and peak of the layer, ozone depletion and total ozone abundance in the stratosphere. The calculated ozone concentrations and profile at both the Equator and a 60˚N location were found to follow closely with the measured data. The calculated average ozone concentration was within 1% of the measured average, and the deviation of ozone profiles was within 14%. The monthly evolution of stratospheric ozone concentrations and distribution above the Equator was studied with results discussed in details. The influences of slow air movement in both altitudinal and radial directions on ozone concentrations and profile in the stratosphere were explored and discussed. Parametric studies of the influences of gas diffusivities of ozone D<sub>O3</sub> and active atomic oxygen D<sub>O</sub> on ozone concentrations and distributions were also studied and delineated. Having both influences through physical diffusion and chemical reactions, the diffusivity (and diffusion) of atomic oxygen D<sub>O</sub> was found to be more sensitive and important than that of ozone D<sub>O3</sub> on ozone concentrations and distribution. The 2-D ozone model present in this paper for stratospheric ozone and its layer and depletion is shown to be robust, convenient, efficient, and executable for analyzing the complex ozone phenomena in the stratosphere. .
基金Supported by 2020 Teaching Reform Research Project of Pingdingshan University(2020-JY05)School-level Ideological and Political Demonstration Course of Pingdingshan University in 2023-Ecological Engineering+1 种基金Science and Technology Research Project of Henan Provincial Department of Science and Technology(212102110189)High-level Talent Start-up Fund Project of Pingdingshan University(PXY-BSQD-202001).
文摘Integrating ideological and political theories teaching into the whole process of classroom teaching construction is a new requirement for implementing the fundamental task of cultivating people by virtue and playing the role of collaborative education.In order to realize the seamless integration of inorganic and analytical chemistry courses and ideological and political education,this paper summarizes the current situation of ideological and political research on inorganic and analytical chemistry courses in three major databases in China(VIP,CNKI and Wanfang),and sorts out the knowledge points,ideological and political elements and educational goals according to the content of the course chapters,to provide a basic guarantee for the ideological and political education construction of the course.
基金supported by the National Natural Science Foundation of China(Grant Nos.:81603182 and 81703607)the Fundamental Research Funds for the Central Universities,China(Grant Nos.:DUT24MS018,DUT23YG228,DUT21RC(3)057)+1 种基金the Open funding of Cancer Hospital of Dalian University of Technology,China(Grant No.:2024-ZLKF-33)the Natural Science Foundation of Liaoning Province,China(Grant No.:2023-MSBA-018).
文摘Green analytical chemistry(GAC)focuses on mitigating the adverse effects of analytical activities on human safety,human health,and environment.In addition to the 12 principles of GAC,proper GAC tools should be developed and employed to assess the greenness of different analytical assays.The 15 widely used GAC metrics,i.e.,national environmental methods index(NEMI),advanced NEMI,assessment of green profile(AGP),chloroform-oriented toxicity estimation scale(ChlorTox Scale),Analytical Eco-Scale,Green Certificate Modified Eco-Scale,analytical method greenness score(AMGS),green analytical procedure index(GAPI),ComplexGAPI,red-green-blue(RGB)additive color model,RGB 12 algorithm,analytical greenness calculator(AGREE),AGREE preparation(AGREEprep),HEXAGON,and blue applicability grade index(BAGI),are selected as the typical tools.This article comprehensively presents and elucidates the principles,characteristics,merits,and demerits of 15 widely used GAC tools.This review is helpful for researchers to use the current GAC metrics to assess the environmental sustainability of analytical assays.