In order to obtain high power density,energy density and safe energy storage lithium ion batteries(LIB)to meet growing demand for electronic products,oxide cathodes have been widely explored in all-solidstate lithium ...In order to obtain high power density,energy density and safe energy storage lithium ion batteries(LIB)to meet growing demand for electronic products,oxide cathodes have been widely explored in all-solidstate lithium batteries(ASSLB)using sulfide solid electrolyte.However,the electrochemical performances are still not satisfactory,due to the high interfacial resistance caused by severe interfacial instability between sulfide solid electrolyte and oxide cathode,especially Ni-rich oxide cathodes,in charge-discharge process.Ni-rich LiNi0.8Co0.1Mn0.1O2(NCM811)material at present is one of the most key cathode candidates to achieve the high energy density up to 300 Wh kg^-1 in liquid LIB,but rarely investigated in ASSLB using sulfide electrolyte.To design the stable interface between NCM811 and sulfide electrolyte should be extremely necessary.In this work,in view of our previous work,LiNbO3 coating with about 1 wt% content is adopted to improve the interfacial stability and the electrochemical performances of NCM811 cathode in ASSLB using Li10GeP2S12 solid electrolyte.Consequently,LiNbO3-coated NCM811 cathode displays the higher discharge capacity and rate performance than the reported oxide electrodes in ASSLB using sulfide solid electrolyte to our knowledge.展开更多
Ground granulated blast furnace slag (GGBFS) and steelmaking slag have been used as a raw material for cement production or as an aggregate to make concrete, which contribute aluminum, calcium, iron, and silicon oxide...Ground granulated blast furnace slag (GGBFS) and steelmaking slag have been used as a raw material for cement production or as an aggregate to make concrete, which contribute aluminum, calcium, iron, and silicon oxides. The suitability of the slag for a particular application depends on its reactivity, cost, availability, and its influence on the properties of the resulting concrete. For the interest of durability studying of concrete in the presence of slag, the accelerated carbonation products and leaching behavior of the slag and Portland cement (PC) were studied. The experimental results confirmed that the slag was more resistant to carbonation compared to PC. The carbonation degree of GGBFS reduced by 17.74/; and the carbonation degrees of steelmaking slags reduced by 9.51/-11.94/. Carbonation neutralized the alkaline nature of the hydrated pastes and gave rise to the redox potential of the leachate slightly (30-77 mV). The carbonation also increased the release of most of the elements presented, except for calcium, to the aqueous environment. It is concluded that blend cements (PC plus slag) have economical advantages and better durability compared to PC.展开更多
China initiated a national carbon trading market in December 2017.Commitments and actions to reduce greenhouse gas(GHG)emissions require consistent,reliable and timely information on GHG emissions.GHG monitoring and m...China initiated a national carbon trading market in December 2017.Commitments and actions to reduce greenhouse gas(GHG)emissions require consistent,reliable and timely information on GHG emissions.GHG monitoring and modeling studies provide GHG emission estimates to evaluate and guide progress towards emission reductions.GHG monitoring has mainly focused on global-scale background networks over the last few decades,while recent efforts have been made on regional and urban scales,such as projects in the Beijing-Tianjin-Hebei city cluster,in Paris,Washington-Baltimore.展开更多
有机太阳能电池(organic solar cells,OSCs)是光伏发电和能源功能材料的重要组成部分,因其制作简单、材料来源广泛、轻量化、柔性好等突出优势成为电池材料领域研究的热点.然而,与无机/钙钛矿太阳能电池相比,有机太阳能电池存在较大的...有机太阳能电池(organic solar cells,OSCs)是光伏发电和能源功能材料的重要组成部分,因其制作简单、材料来源广泛、轻量化、柔性好等突出优势成为电池材料领域研究的热点.然而,与无机/钙钛矿太阳能电池相比,有机太阳能电池存在较大的电压损失(即能量损失),限制了效率的进一步提升.目前实验室报道最高效率远低于肖克利-奎伊瑟(Shockley-Queisser)理论所定义的极限效率.因此,最大化降低有机太阳能电池的电压损失,是进一步提升电池器件效率的关键.针对上述问题,国家纳米科学中心的相关科研人员做出了很多努力,在高开路电压、低能量损失的有机太阳能电池分子设计、理论计算以及新型器件结构等方面做了非常出色的工作.本文综述了近年来的相关研究进展,希望为有机太阳能电池相关领域的研究者提供借鉴并对有机太阳能电池的发展起到促进作用.展开更多
The design and synthesis of photoactive macrocyclic molecules continue to attract attention because such species play important roles in supramolecular chemistry as well as photoelectronic applications.Donoracceptor(D...The design and synthesis of photoactive macrocyclic molecules continue to attract attention because such species play important roles in supramolecular chemistry as well as photoelectronic applications.Donoracceptor(D-A)conjugated macrocycles are an emerging class of photoactive molecules due to their D-A conjugated structural characteristics and tunable optical properties.In addition,the well-defined cavities in such D-A macrocycles endow them with versatile host-guest properties.In this review,we provide a comprehensive summary of D-A conjugated macrocycle chemistry,detailing recent progress in the area of synthetic methods,optical properties,host-guest chemistry and applications of the underlying chemistry to chemical sensors,bioimaging and photoelectronic devices.Our objective is to provide not only a review of the fundamental findings,but also to outline future research directions where D-A conjugated macrocycles and their constructs may have a role to play.展开更多
Sulfide electrolyte-based all-solid-state batteries(ASSBs)are potential next generation energy storage technology due to the high ionic conductivity of sulfide electrolytes and potentially improved energy density and ...Sulfide electrolyte-based all-solid-state batteries(ASSBs)are potential next generation energy storage technology due to the high ionic conductivity of sulfide electrolytes and potentially improved energy density and safety.However,the performance of ASSBs at/below subzero temperatures has not been explored systematically.Herein,low temperature(LT)performance of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)|Li_(9.54)Si_(1.74)P_(1.44)S11.7Cl_(0.3)(LiSPSCl)|Li_(4)Ti_(5)O_(12)(LTO)ASSBs was investigated.By charging the ASSB to 6 V at−40℃,a capacity of 100.7 mAh∙g^(−1)at 20 mA∙g^(−1)was achieved,which is much higher than that charged to 4.3 V(4.6 mAh∙g^(−1))at−40℃.Moreover,atomic resolution microscopy revealed that the NCM811 remained almost intact even after being charged to 6 V.In contrast,NCM811 was entirely destructed when charged to 6 V at room temperature.The sharp difference arises from the large internal charge transfer resistance at LT which requires high voltage to overcome.Nevertheless,such high voltage is not harmful to the active material but beneficial to extracting most energy out of the ASSBs at LT.We also demonstrated that thinner electrolyte is favorable for LT operation of ASSBs due to the reduced ion transfer distance.This work provides new strategies to boost the capacity and energy density of sulfide-based ASSBs at LT for dedicated LT applications.展开更多
Lithium–indium(Li-In)alloys are important anode materials for sulfide-based all-solid-state batteries(ASSBs),but how different Li concentrations in the alloy anodes impact the electrochemical performance of ASSBs rem...Lithium–indium(Li-In)alloys are important anode materials for sulfide-based all-solid-state batteries(ASSBs),but how different Li concentrations in the alloy anodes impact the electrochemical performance of ASSBs remains unexplored.This paper systematically investigates the impact that different Li concentrations in Li-In anodes have on the performance of ASSBs.We show that In with 1 wt%Li(LiIn-1)exhibits the best performance for ASSBs among all the tested Li-In anodes.In essence,LiIn-1 not only provides sufficient Li to compensate for first-cycle capacity loss in the anode but also facilitates the formation of a LiIn alloy phase that has the best charge transfer kinetics among all the Li_(x) In alloy phases.The ASSB with a LiIn-1 anode and a LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) cathode reached 3400 cycles at an initial capacity of 125 mAh/g.Remarkably,ASSBs with a high cathode active material(CAM)loading of 36 mg/cm 2 delivered a high areal capacity of 4.05 mAh/cm^(2) at high current density(4.8 mA/cm^(2)),with a capacity retention of 92% after 740 cycles.At an ultra-high CAM loading of 55.3 mg/cm^(2),the ASSB achieved a stable areal capacity of 8.4 mAh/cm^(2) at current density of 1.7 mA/cm 2.These results bring us one step closer to the practical application of ASSBs.展开更多
CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate ...CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.展开更多
The modeling system RAMS-CMAQ is applied in this paper to East Asia to simulate the temporo-spatial concentration distributions of atmo- spheric aerosols. For evaluating its performances, modeled concentrations of aer...The modeling system RAMS-CMAQ is applied in this paper to East Asia to simulate the temporo-spatial concentration distributions of atmo- spheric aerosols. For evaluating its performances, modeled concentrations of aerosols such as sulfate, nitrate, ammonium, black carbon and organic carbon were compared with observations obtained in East Asia on board of two aircrafts in the springtime of 2001. The comparison showed gener- ally good agreement, and, in particular, that the modeling system captured most of the important observed features, including vertical gradients of the aerosols of the Asian outflow over the western Pacific. The evaluation results provide us with much confidence for further use of the modeling system to investigate the transport and transformation processes of atmospheric aerosols over East Asia and to assess their impacts on the Earth's radiation budget.展开更多
Modulating the helicity of self-assemblies of conjugated molecules is important for their application in chiral electronics.In this communication,solvent effect has been investigated on how to modulate the helicity of...Modulating the helicity of self-assemblies of conjugated molecules is important for their application in chiral electronics.In this communication,solvent effect has been investigated on how to modulate the helicity of supramolecular assemblies of sugar-substituted perylenediimide(PTCDI-BAG)by using UV-Vis,circular dichroism spectroscopy and transmission electron microscopy.Left-handed helical nanowires are obtained in the mixed solvent system of both N,N-dimethylformamide/ethanol(DMF/ethanol)and N,N-dimethylacetamide/ethanol(DMAC/ethanol).As changing the solvents into dimethyl sulfoxide/ethanol(DMSO/ethanol),ethylene glycol/ethanol(EG/ethanol),or N-methyl-2-pyrrolidone/ethanol(NMP/ethanol),only right-handed heical nanowires are observed.The chirality of supramolecular structures can be tuned by the controlling of the polarity of the solvents.A theoretical calculation is carried out to explain the chiral optical inversion phenomena of PTCDI-BAG aggregates in different solvents,which reveals that reversed CD spectra is due to the difference of clockwise and anticlockwise rotation of the dimer.展开更多
The synthesis,structure,and properties of pyrene-based conformationally adaptive macrocycles are described.This new type of conformationally adaptive macrocycle was constructed through Perkin reaction,followed by imid...The synthesis,structure,and properties of pyrene-based conformationally adaptive macrocycles are described.This new type of conformationally adaptive macrocycle was constructed through Perkin reaction,followed by imidization.By changing the condensation partner as the linking unit,a family of conjugated macrocycles with different sizes of the cavity was synthesized,which provide a simple and modular synthetic strategy towards the conformationally adaptive macrocycles.Furthermore,the macrocycles provide two well-defined conformations through flipping pyrene subunit,which were unambiguously determined by single-crystal X-ray diffraction analysis.The conformational interconversion barrier was determined by density functional theory(DFT)calculations.This new macrocycle also demonstrated unique properties,such as vapochromic behavior and aggregation emission enhancement effect.Furthermore,we have also investigated the effect of the linker on the shape and photophysical properties of the resulting macrocyclic products.展开更多
基金financially supported partly by the National Key Research and Development Program of China (2018YFB0104302)NSFC (21503148)Major Programs of the Innovation Driven Plan of Guilin (No. 20160203)
文摘In order to obtain high power density,energy density and safe energy storage lithium ion batteries(LIB)to meet growing demand for electronic products,oxide cathodes have been widely explored in all-solidstate lithium batteries(ASSLB)using sulfide solid electrolyte.However,the electrochemical performances are still not satisfactory,due to the high interfacial resistance caused by severe interfacial instability between sulfide solid electrolyte and oxide cathode,especially Ni-rich oxide cathodes,in charge-discharge process.Ni-rich LiNi0.8Co0.1Mn0.1O2(NCM811)material at present is one of the most key cathode candidates to achieve the high energy density up to 300 Wh kg^-1 in liquid LIB,but rarely investigated in ASSLB using sulfide electrolyte.To design the stable interface between NCM811 and sulfide electrolyte should be extremely necessary.In this work,in view of our previous work,LiNbO3 coating with about 1 wt% content is adopted to improve the interfacial stability and the electrochemical performances of NCM811 cathode in ASSLB using Li10GeP2S12 solid electrolyte.Consequently,LiNbO3-coated NCM811 cathode displays the higher discharge capacity and rate performance than the reported oxide electrodes in ASSLB using sulfide solid electrolyte to our knowledge.
文摘Ground granulated blast furnace slag (GGBFS) and steelmaking slag have been used as a raw material for cement production or as an aggregate to make concrete, which contribute aluminum, calcium, iron, and silicon oxides. The suitability of the slag for a particular application depends on its reactivity, cost, availability, and its influence on the properties of the resulting concrete. For the interest of durability studying of concrete in the presence of slag, the accelerated carbonation products and leaching behavior of the slag and Portland cement (PC) were studied. The experimental results confirmed that the slag was more resistant to carbonation compared to PC. The carbonation degree of GGBFS reduced by 17.74/; and the carbonation degrees of steelmaking slags reduced by 9.51/-11.94/. Carbonation neutralized the alkaline nature of the hydrated pastes and gave rise to the redox potential of the leachate slightly (30-77 mV). The carbonation also increased the release of most of the elements presented, except for calcium, to the aqueous environment. It is concluded that blend cements (PC plus slag) have economical advantages and better durability compared to PC.
基金supported by the National Key R&D Program of Chinagrant number 2018YFC1507701the Key Research and Development(R&D)Projects of Shanxi Province grant number 201803D31220the EDF programthe Belt and Road national greenhouse gas and pollutant co-control study grant number 2019-434。
文摘China initiated a national carbon trading market in December 2017.Commitments and actions to reduce greenhouse gas(GHG)emissions require consistent,reliable and timely information on GHG emissions.GHG monitoring and modeling studies provide GHG emission estimates to evaluate and guide progress towards emission reductions.GHG monitoring has mainly focused on global-scale background networks over the last few decades,while recent efforts have been made on regional and urban scales,such as projects in the Beijing-Tianjin-Hebei city cluster,in Paris,Washington-Baltimore.
文摘有机太阳能电池(organic solar cells,OSCs)是光伏发电和能源功能材料的重要组成部分,因其制作简单、材料来源广泛、轻量化、柔性好等突出优势成为电池材料领域研究的热点.然而,与无机/钙钛矿太阳能电池相比,有机太阳能电池存在较大的电压损失(即能量损失),限制了效率的进一步提升.目前实验室报道最高效率远低于肖克利-奎伊瑟(Shockley-Queisser)理论所定义的极限效率.因此,最大化降低有机太阳能电池的电压损失,是进一步提升电池器件效率的关键.针对上述问题,国家纳米科学中心的相关科研人员做出了很多努力,在高开路电压、低能量损失的有机太阳能电池分子设计、理论计算以及新型器件结构等方面做了非常出色的工作.本文综述了近年来的相关研究进展,希望为有机太阳能电池相关领域的研究者提供借鉴并对有机太阳能电池的发展起到促进作用.
基金supported by the National Natural Science Foundation of China(Nos.21971041 and 22001039)Natural Science Foundation of Fujian Province(No.2020J01447).
文摘The design and synthesis of photoactive macrocyclic molecules continue to attract attention because such species play important roles in supramolecular chemistry as well as photoelectronic applications.Donoracceptor(D-A)conjugated macrocycles are an emerging class of photoactive molecules due to their D-A conjugated structural characteristics and tunable optical properties.In addition,the well-defined cavities in such D-A macrocycles endow them with versatile host-guest properties.In this review,we provide a comprehensive summary of D-A conjugated macrocycle chemistry,detailing recent progress in the area of synthetic methods,optical properties,host-guest chemistry and applications of the underlying chemistry to chemical sensors,bioimaging and photoelectronic devices.Our objective is to provide not only a review of the fundamental findings,but also to outline future research directions where D-A conjugated macrocycles and their constructs may have a role to play.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.22279112,51772262,5197010923,11575154,51971245,52022088,U20A20336,and 52002346)the Fok Ying-Tong Education Foundation of China(No.171064)+5 种基金the Natural Science Foundation of Hebei Province(Nos.B2022203018,B2018203297,B2020203037,and F2021203097)the Hebei One Hundred Talent Program(No.4570028)the High-Level Talents Research Program of the Yanshan University(Nos.00500021502 and 005000201)the Hebei Key Laboratory of Applied Chemistry after Operation Performance(No.22567616H)the Science and Technology Innovation Program of Hunan Province(No.2021RC3109)the Postgraduate Scientific Research Innovation Project of Xiangtan University(No.XDCX2022Y076).
文摘Sulfide electrolyte-based all-solid-state batteries(ASSBs)are potential next generation energy storage technology due to the high ionic conductivity of sulfide electrolytes and potentially improved energy density and safety.However,the performance of ASSBs at/below subzero temperatures has not been explored systematically.Herein,low temperature(LT)performance of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)|Li_(9.54)Si_(1.74)P_(1.44)S11.7Cl_(0.3)(LiSPSCl)|Li_(4)Ti_(5)O_(12)(LTO)ASSBs was investigated.By charging the ASSB to 6 V at−40℃,a capacity of 100.7 mAh∙g^(−1)at 20 mA∙g^(−1)was achieved,which is much higher than that charged to 4.3 V(4.6 mAh∙g^(−1))at−40℃.Moreover,atomic resolution microscopy revealed that the NCM811 remained almost intact even after being charged to 6 V.In contrast,NCM811 was entirely destructed when charged to 6 V at room temperature.The sharp difference arises from the large internal charge transfer resistance at LT which requires high voltage to overcome.Nevertheless,such high voltage is not harmful to the active material but beneficial to extracting most energy out of the ASSBs at LT.We also demonstrated that thinner electrolyte is favorable for LT operation of ASSBs due to the reduced ion transfer distance.This work provides new strategies to boost the capacity and energy density of sulfide-based ASSBs at LT for dedicated LT applications.
基金This work was financially supported by the National Natural Science Foundation of China(22279112,52022088,51971245,51772262,21406191,U20A20336,21935009)Beijing Natural Science Foundation(2202046)+2 种基金Fok Ying-Tong Education Foundation of China(171064)333 Talent Program of Hebei Province(C20221018)Natural Science Foundation of Hebei Province(B2022203018,B2020203037,B2018203297).
文摘Lithium–indium(Li-In)alloys are important anode materials for sulfide-based all-solid-state batteries(ASSBs),but how different Li concentrations in the alloy anodes impact the electrochemical performance of ASSBs remains unexplored.This paper systematically investigates the impact that different Li concentrations in Li-In anodes have on the performance of ASSBs.We show that In with 1 wt%Li(LiIn-1)exhibits the best performance for ASSBs among all the tested Li-In anodes.In essence,LiIn-1 not only provides sufficient Li to compensate for first-cycle capacity loss in the anode but also facilitates the formation of a LiIn alloy phase that has the best charge transfer kinetics among all the Li_(x) In alloy phases.The ASSB with a LiIn-1 anode and a LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) cathode reached 3400 cycles at an initial capacity of 125 mAh/g.Remarkably,ASSBs with a high cathode active material(CAM)loading of 36 mg/cm 2 delivered a high areal capacity of 4.05 mAh/cm^(2) at high current density(4.8 mA/cm^(2)),with a capacity retention of 92% after 740 cycles.At an ultra-high CAM loading of 55.3 mg/cm^(2),the ASSB achieved a stable areal capacity of 8.4 mAh/cm^(2) at current density of 1.7 mA/cm 2.These results bring us one step closer to the practical application of ASSBs.
基金supported by the General Project of Top-Design of Multi-Scale Nature-Social ModelsData Support and Decision Support System for NSFC Carbon Neutrality Major Project(42341202)the Basic Scientific Research Fund of the Chinese Academy of Meteorological Sciences(2021Z014)。
文摘CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.
基金grants from the Ministry of Science and Technology of China (Grant no. 2006CB403702) the National Natural Science Foundation of China (Grant no. 40333029).
文摘The modeling system RAMS-CMAQ is applied in this paper to East Asia to simulate the temporo-spatial concentration distributions of atmo- spheric aerosols. For evaluating its performances, modeled concentrations of aerosols such as sulfate, nitrate, ammonium, black carbon and organic carbon were compared with observations obtained in East Asia on board of two aircrafts in the springtime of 2001. The comparison showed gener- ally good agreement, and, in particular, that the modeling system captured most of the important observed features, including vertical gradients of the aerosols of the Asian outflow over the western Pacific. The evaluation results provide us with much confidence for further use of the modeling system to investigate the transport and transformation processes of atmospheric aerosols over East Asia and to assess their impacts on the Earth's radiation budget.
基金supported by the National Natural Science Foundation of China (Grant Nos.91027031 and 21125420)the Ministry of Science and Technology of China (Grant No.2011CB932300)the Chinese Academy of Sciences.
文摘Modulating the helicity of self-assemblies of conjugated molecules is important for their application in chiral electronics.In this communication,solvent effect has been investigated on how to modulate the helicity of supramolecular assemblies of sugar-substituted perylenediimide(PTCDI-BAG)by using UV-Vis,circular dichroism spectroscopy and transmission electron microscopy.Left-handed helical nanowires are obtained in the mixed solvent system of both N,N-dimethylformamide/ethanol(DMF/ethanol)and N,N-dimethylacetamide/ethanol(DMAC/ethanol).As changing the solvents into dimethyl sulfoxide/ethanol(DMSO/ethanol),ethylene glycol/ethanol(EG/ethanol),or N-methyl-2-pyrrolidone/ethanol(NMP/ethanol),only right-handed heical nanowires are observed.The chirality of supramolecular structures can be tuned by the controlling of the polarity of the solvents.A theoretical calculation is carried out to explain the chiral optical inversion phenomena of PTCDI-BAG aggregates in different solvents,which reveals that reversed CD spectra is due to the difference of clockwise and anticlockwise rotation of the dimer.
基金supported by the National Natural Science Foundation of China (51303185, 21021091, 51033006, 51222306, 51003107, 61201105, 3591027043, 91222203, 91233205, 21473222 and 21773040)the Ministry of Science and Technology of China (2011CB808400, 2011CB932300, 2013CB933403, 2013CB933500 and 2014CB643600)the Chinese Academy of Sciences (Y42D0A12D1 and Y42D0412D1)。
基金supported by the National Natural Science Foundation of China(Nos.21971041 and 22001039)Natural Science Foundation of Fujian Province(Nos.2018J01431,2018J01690 and 2020J01447)Research Foundation of Education Bureau of Fujian Province(No.JT180813)。
文摘The synthesis,structure,and properties of pyrene-based conformationally adaptive macrocycles are described.This new type of conformationally adaptive macrocycle was constructed through Perkin reaction,followed by imidization.By changing the condensation partner as the linking unit,a family of conjugated macrocycles with different sizes of the cavity was synthesized,which provide a simple and modular synthetic strategy towards the conformationally adaptive macrocycles.Furthermore,the macrocycles provide two well-defined conformations through flipping pyrene subunit,which were unambiguously determined by single-crystal X-ray diffraction analysis.The conformational interconversion barrier was determined by density functional theory(DFT)calculations.This new macrocycle also demonstrated unique properties,such as vapochromic behavior and aggregation emission enhancement effect.Furthermore,we have also investigated the effect of the linker on the shape and photophysical properties of the resulting macrocyclic products.