Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium batteries.However,the poor chemical stability and compatibilit...Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium batteries.However,the poor chemical stability and compatibility with lithium metal limit their application.Herein,Li_(5.4)PS_(4.4)Cl1.4I0.2solid electrolyte with high ionic conductivity of 11.49 m S ccm^(-1)and improved chemical stability is synthesized by iodine doping.An ultra-thin Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane with thickness of 10μm can be obtained by wet coating process,exhibiting a high ionic conductivity of 2.09 mS ccm^(-1)and low areal resistance of 1.17Ωcm^(-2).Moreover,iodine doping could in-situ form LiI at the lithium/electrolyte interface and improve the critical current density of Li_(5.4)PS_(4.4)Cl_(1.6)from 0.8 to 1.35 mA cm^(-2).The resultant LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)/Li battery shows excellent cycling stability at 1 C,with a reversible specific capacity of 110.1 mA h g^(-1)and a retention of 80.5% after 1000 cycles.In addition,the assembled LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane/Li pouch cell delivers an initial discharge capacity of 110.4 mA h g^(-1)and 80.5% capacity retention after 100 cycles.展开更多
C/SiO_(x)anode with higher capacity and lower lithiation potential has been recognized as a nextgeneration alternative to graphite for high-energy-density lithium-ion batteries.However,C/SiO_(x)suffers from low initia...C/SiO_(x)anode with higher capacity and lower lithiation potential has been recognized as a nextgeneration alternative to graphite for high-energy-density lithium-ion batteries.However,C/SiO_(x)suffers from low initial Coulombic efficiency(ICE),which significantly hinders its practical application.Herein,we reported a straightforward iodine redox chemistry strategy to realize highly reversible Li storage behavior and remarkably enhanced ICE of high-capacity C/SiO_(x)anode toward long-life lithium-ion batteries.Specifically,I2is introduced into porous C/SiO_(x)via simple fumigation to synthesize their composite(C/SiO_(x)@I),in which I_(2)can effectively inhibit the irreversible lithiation reactions of SiO_(x)through redox reaction.Further,redox reaction intermediates of LiI_(3)and LiIO_(3)can inhibit the decomposition of electrolyte and LiPF6,thereby reducing the thickness of the solid-electrolyte interphase film.Consequently,the obtained C/SiO_(x)@I exhibits a considerable capacity of 1241 mAh g^(-1)with an improved ICE of 88.5%at 0.1 A g^(-1)and impressive cyclability,showing capacity retention of 95%after 700 cycles at5.0 A g^(-1).Besides,the C/SiO_(x)@I with a 12%addition ratio can greatly enhance the capacity of graphite from 352 to 454 mAh g^(-1),with negligible impact on its ICE.When the addition ratio is 9%,the energy density of the 18,650 cylindrical battery composed of graphite and Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2)can be enhanced by approximately 25 Wh kg^(-1).This study opens a new avenue for developing high ICE in SiO_(x)-based anodes for high-energy-density lithium-ion batteries.展开更多
A simple and efficient method for the selective iodination of various aromatic compounds by using potassium iodide in the presence of benzyltnphenylphosphonium perchlorate,is reported.This method provides several adva...A simple and efficient method for the selective iodination of various aromatic compounds by using potassium iodide in the presence of benzyltnphenylphosphonium perchlorate,is reported.This method provides several advantages such as good selectivity between ortho and para positions of aromatic compounds and high yields of the products.展开更多
Objective To recognize the spatial and temporal characteristics of iodine deficiency disorders(IDD),China national IDD surveillance data for the years of 1995–2018 were analyzed.Methods Time series analysis was used ...Objective To recognize the spatial and temporal characteristics of iodine deficiency disorders(IDD),China national IDD surveillance data for the years of 1995–2018 were analyzed.Methods Time series analysis was used to describe and predict the IDD related indicators,and spatial analysis was used to analyze the spatial distribution of salt iodine levels.Results In China,the median urinary iodine concentration increased in 1995–1997,then decreased to adequate levels,and are expected to remain appropriate in 2019–2022.The goiter rate continually decreased and is expected to be maintained at a low level.Since 2002,the coverage rates of iodized salt and the consumption rates of qualified iodized salt(the percentage of qualified iodized salt in all tested salt) increased and began to decline in 2012;they are expected to continue to decrease.Spatial epidemiological analysis indicated a positive spatial correlation in 2016–2018 and revealed feature regarding the spatial distribution of salt related indicators in coastal areas and areas near iodine-excess areas.Conclusions Iodine nutrition in China showed gradual improvements.However,a recent decline has been observed in some areas following changes in the iodized salt supply in China.In the future,more regulations regarding salt management should be issued to strengthen IDD control and prevention measures,and avoid the recurrence of IDD.展开更多
In order to ensure that the intake of iodine from iodized salt is adequate, the effects of cooking, storage and iedination on iodine content in iodized salt have been studied. For moni toring the analytical Performanc...In order to ensure that the intake of iodine from iodized salt is adequate, the effects of cooking, storage and iedination on iodine content in iodized salt have been studied. For moni toring the analytical Performance, a qoality control exawhnation was also undertaken. The loss of iodine was greater when salt was stored in plastic bag than in glass bottle. The loss was greater in fortified salt stored at 37℃ and under 76% humidity than in that at 20 ~ 25℃ and under lower humidity. The retention of iodine varied with the kind of has and also was influenced by the water content of cooked food. In general, the retention of iodine during cooking varied considerably (from 36. 6% to 86. 1 % ). The iodine concentration in salts varied greater from 3.0 to 100.3 mg/kg in salt for markets, and from 0 to 90.0 mg/kg in salts for households. 48. 3 % of samples from markets were found to be in compliance with national standards (30 ~ 50 mg/kg), and 72.0% of samples from households were in compliance with national standartl (20 ~ 50 mg/kg). Analytical data collected from 8 of the cooperative laheratories foran analytical reference material showed a 95% codridence interval of the population mean for both precision and accuracy, falling within X± 2SD and passing quality control exdrination展开更多
We fed adult mink diets containing supplemental iodine, from 0 to 320 ppm, for one or seven months prior to breeding. Blood samples collected from the adults and their offspring (kits) at 4 wk post-partum were assayed...We fed adult mink diets containing supplemental iodine, from 0 to 320 ppm, for one or seven months prior to breeding. Blood samples collected from the adults and their offspring (kits) at 4 wk post-partum were assayed for total thyroxine (T4), triiodothyronine (T3), reverse T3 (rT3), and T4-binding indices. As expected T4 concentrations of the adult and kit mink varied inversely with the level of supplemental iodine. In addition, T3 and rT3 concentrations decreased gradually in kits from the long-term experiment in response to the increased dietary iodine of the dams. T3 concentrations of kits from dams fed iodine short-term decreased markedly while rTy concentrations were elevated greatly in response to increased dietary iodine of the dam. These decreases in hormone levels are due to serum iodine blocking the thyroid uptake of iodine and subsequent decrease of hormone synthesis. Excess iodine may also block the effect of thyroid stimulating hormone. The T4-binding indices of the adults, in general, were depressed, while the T4-binding indices of the kits were more variable. These effects are probably due to fluctuations in thyroglobulin.展开更多
Reticular chemistry enables the precise design and synthesis of crystalline extended materials,however,its application in hierarchical self-assembly of superstructures remains challenging due to the limited control ov...Reticular chemistry enables the precise design and synthesis of crystalline extended materials,however,its application in hierarchical self-assembly of superstructures remains challenging due to the limited control over weak interactions between synthons,in contrast to the stronger coordination or covalent bonds typically involved.Herein,we introduce an anion-competitive strategy to control the topology and structural diversity of superstructures.Cationic tetrahedral Zr-based metal–organic polyhedra were used as cage-like synthons,which were charge-balanced by Cl^(-)ions and interconnected via hydrogen bonds to form hierarchical superstructures.Introducing trigonal planar NO_(3)^(-)ions to compete with spherical Cl^(-)ions produced three new superstructures featuring different hydrogen bond-based linkages and distinct topologies(dia,bnn,and xhy),diverging from the previously reported flu topology.Furthermore,the superstructures with dia and bnn topologies exhibit high porosities and record iodine adsorption capacities in solution(4.31 and 4.19 g·g^(-1),respectively).This work demonstrates the potential of reticular chemistry for the versatile design and construction of diversified hierarchical superstructures.展开更多
Main observation and conclusion An anodic oxidation enabled synthesis of hypervalent iodinel(Ⅲ)reagents from aryl iodides is demonstrated.Under mild electrochem-ical conditions,a range of arylidine(Ⅲ)reagents includ...Main observation and conclusion An anodic oxidation enabled synthesis of hypervalent iodinel(Ⅲ)reagents from aryl iodides is demonstrated.Under mild electrochem-ical conditions,a range of arylidine(Ⅲ)reagents including iodosylarenes,(difunctionaliodo)arenes,benziodoxoles and diaryliodoni-um salts can be efficiently synthesized and derivatized in good to excellent yields with high selectivity.As only electrons serve as the oxidation reagents,this method offers a more straightforward and sustainable manner avoiding the use of expensive or hazardous chemical oxidants.展开更多
Exploring the physiochemical properties and expanding the applications of actinide-containing materials is paramount to address the escalating challenge of radioactive waste accumulation.However,unlocking the full pot...Exploring the physiochemical properties and expanding the applications of actinide-containing materials is paramount to address the escalating challenge of radioactive waste accumulation.However,unlocking the full potential of these materials is largely crippled by the radiotoxicity of the actinides.We report here two porous and luminescent thorium-based metal-organic frameworks(Th-BITD-1 and Th-BITD-2)that serve as a bifunctional platform for sequencing and sensing of radioiodine,a much more radioactive fission product discharged during the nuclear fuel reprocessing.In particular,Th-BITD-1 displays better iodine uptake performance than Th-BITD-2 via the solution-based process and vapor diffusion with the maximum adsorption capacities of 831 and 1099 mg/g,respectively.Fur thermore,Th-BITD-1 can function as a highly sensitive luminescence sensor for iodate with a quenching constant(Ksv)of 6.6(5)×10^(3) M^(-1)and a detection limit of 2.02μM,respectively,outperforming 2.96(6)×10^(3)M^(-1)and 10.5μM of Th-BITD-2.Moreover,a positive correlation between the sensing efficacy and the iodate adsorption capacity has been revealed.This work highlights the opportunity in designing novel actinide-based MOFs for their potential applications in radiological fields,e.g.,radionuclide separation and detection.展开更多
Comprehensive Summary,A convenient approach for the construction of 2-aminobenzothiazoles via I2-catalyzed tandem cyclization reaction of amines and carbon disulfide has been developed.The present approach starts from...Comprehensive Summary,A convenient approach for the construction of 2-aminobenzothiazoles via I2-catalyzed tandem cyclization reaction of amines and carbon disulfide has been developed.The present approach starts from simple and readily available starting materials,affording a series of 2-aminobenzothiazoles in up to 89%yields under metal-free conditions.In this work,C—H/N—H functionalization was achieved and multiple C-hetero bonds were successfully constructed in one pot.展开更多
基金National Key R&D Program of China (grant no. 2022YFB3807700)National Natural Science Foundation of China (Grant No. U1964205, U21A2075, 52172253,52102326, 52250610214, 22309194, 52372244)+4 种基金Ningbo S&T Innovation 2025 Major Special Programme (Grant No.2019B10044, 2021Z122, 2023Z106)Zhejiang Provincial Key R&D Program of China (Grant No. 2022C01072, 2024C01095)Jiangsu Provincial S&T Innovation Special Programme for carbon peak and carbon neutrality (Grant No. BE2022007)Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation of China (LBMHD24E020001)Youth Innovation Promotion Association CAS (Y2021080)。
文摘Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium batteries.However,the poor chemical stability and compatibility with lithium metal limit their application.Herein,Li_(5.4)PS_(4.4)Cl1.4I0.2solid electrolyte with high ionic conductivity of 11.49 m S ccm^(-1)and improved chemical stability is synthesized by iodine doping.An ultra-thin Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane with thickness of 10μm can be obtained by wet coating process,exhibiting a high ionic conductivity of 2.09 mS ccm^(-1)and low areal resistance of 1.17Ωcm^(-2).Moreover,iodine doping could in-situ form LiI at the lithium/electrolyte interface and improve the critical current density of Li_(5.4)PS_(4.4)Cl_(1.6)from 0.8 to 1.35 mA cm^(-2).The resultant LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)/Li battery shows excellent cycling stability at 1 C,with a reversible specific capacity of 110.1 mA h g^(-1)and a retention of 80.5% after 1000 cycles.In addition,the assembled LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane/Li pouch cell delivers an initial discharge capacity of 110.4 mA h g^(-1)and 80.5% capacity retention after 100 cycles.
基金financially supported by the National Natural Science Foundation of China(No.51962027,and 52262039)the Major Science and Technology Project of Inner Mongolia Autonomous Region(2021ZD0016)+3 种基金the National Key R&D Program of China(2020YFC1909105)the Fundamental Research Funds for Inner Mongolia University of Science&Technology(NO.2024QNJS071,2023QNJS052 and 2024QNJS064)the Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(No.NJYT24002)the Central Guidance Fund for Local Scientific and Technological Development(2024ZY0012)。
文摘C/SiO_(x)anode with higher capacity and lower lithiation potential has been recognized as a nextgeneration alternative to graphite for high-energy-density lithium-ion batteries.However,C/SiO_(x)suffers from low initial Coulombic efficiency(ICE),which significantly hinders its practical application.Herein,we reported a straightforward iodine redox chemistry strategy to realize highly reversible Li storage behavior and remarkably enhanced ICE of high-capacity C/SiO_(x)anode toward long-life lithium-ion batteries.Specifically,I2is introduced into porous C/SiO_(x)via simple fumigation to synthesize their composite(C/SiO_(x)@I),in which I_(2)can effectively inhibit the irreversible lithiation reactions of SiO_(x)through redox reaction.Further,redox reaction intermediates of LiI_(3)and LiIO_(3)can inhibit the decomposition of electrolyte and LiPF6,thereby reducing the thickness of the solid-electrolyte interphase film.Consequently,the obtained C/SiO_(x)@I exhibits a considerable capacity of 1241 mAh g^(-1)with an improved ICE of 88.5%at 0.1 A g^(-1)and impressive cyclability,showing capacity retention of 95%after 700 cycles at5.0 A g^(-1).Besides,the C/SiO_(x)@I with a 12%addition ratio can greatly enhance the capacity of graphite from 352 to 454 mAh g^(-1),with negligible impact on its ICE.When the addition ratio is 9%,the energy density of the 18,650 cylindrical battery composed of graphite and Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2)can be enhanced by approximately 25 Wh kg^(-1).This study opens a new avenue for developing high ICE in SiO_(x)-based anodes for high-energy-density lithium-ion batteries.
基金the Gachsaran branch,Islamic Azad University,for the partial support
文摘A simple and efficient method for the selective iodination of various aromatic compounds by using potassium iodide in the presence of benzyltnphenylphosphonium perchlorate,is reported.This method provides several advantages such as good selectivity between ortho and para positions of aromatic compounds and high yields of the products.
基金partly supported by the National Natural Science Foundation of China [81773370 and 82173638]the Natural Science Foundation of Heilongjiang Province [TD2019H001]
文摘Objective To recognize the spatial and temporal characteristics of iodine deficiency disorders(IDD),China national IDD surveillance data for the years of 1995–2018 were analyzed.Methods Time series analysis was used to describe and predict the IDD related indicators,and spatial analysis was used to analyze the spatial distribution of salt iodine levels.Results In China,the median urinary iodine concentration increased in 1995–1997,then decreased to adequate levels,and are expected to remain appropriate in 2019–2022.The goiter rate continually decreased and is expected to be maintained at a low level.Since 2002,the coverage rates of iodized salt and the consumption rates of qualified iodized salt(the percentage of qualified iodized salt in all tested salt) increased and began to decline in 2012;they are expected to continue to decrease.Spatial epidemiological analysis indicated a positive spatial correlation in 2016–2018 and revealed feature regarding the spatial distribution of salt related indicators in coastal areas and areas near iodine-excess areas.Conclusions Iodine nutrition in China showed gradual improvements.However,a recent decline has been observed in some areas following changes in the iodized salt supply in China.In the future,more regulations regarding salt management should be issued to strengthen IDD control and prevention measures,and avoid the recurrence of IDD.
文摘In order to ensure that the intake of iodine from iodized salt is adequate, the effects of cooking, storage and iedination on iodine content in iodized salt have been studied. For moni toring the analytical Performance, a qoality control exawhnation was also undertaken. The loss of iodine was greater when salt was stored in plastic bag than in glass bottle. The loss was greater in fortified salt stored at 37℃ and under 76% humidity than in that at 20 ~ 25℃ and under lower humidity. The retention of iodine varied with the kind of has and also was influenced by the water content of cooked food. In general, the retention of iodine during cooking varied considerably (from 36. 6% to 86. 1 % ). The iodine concentration in salts varied greater from 3.0 to 100.3 mg/kg in salt for markets, and from 0 to 90.0 mg/kg in salts for households. 48. 3 % of samples from markets were found to be in compliance with national standards (30 ~ 50 mg/kg), and 72.0% of samples from households were in compliance with national standartl (20 ~ 50 mg/kg). Analytical data collected from 8 of the cooperative laheratories foran analytical reference material showed a 95% codridence interval of the population mean for both precision and accuracy, falling within X± 2SD and passing quality control exdrination
基金Supported in part by the Mink Farmers Research Foundation,Thiensville,WI and The Heger Company,North St.Paul,MN.
文摘We fed adult mink diets containing supplemental iodine, from 0 to 320 ppm, for one or seven months prior to breeding. Blood samples collected from the adults and their offspring (kits) at 4 wk post-partum were assayed for total thyroxine (T4), triiodothyronine (T3), reverse T3 (rT3), and T4-binding indices. As expected T4 concentrations of the adult and kit mink varied inversely with the level of supplemental iodine. In addition, T3 and rT3 concentrations decreased gradually in kits from the long-term experiment in response to the increased dietary iodine of the dams. T3 concentrations of kits from dams fed iodine short-term decreased markedly while rTy concentrations were elevated greatly in response to increased dietary iodine of the dam. These decreases in hormone levels are due to serum iodine blocking the thyroid uptake of iodine and subsequent decrease of hormone synthesis. Excess iodine may also block the effect of thyroid stimulating hormone. The T4-binding indices of the adults, in general, were depressed, while the T4-binding indices of the kits were more variable. These effects are probably due to fluctuations in thyroglobulin.
基金supported by National Natural Science Foundation of China(grant no.22101093)Natural Science Foundation of Hubei Province,China(grant no.2022CFB163)Knowledge Innovation Program of Wuhan-Shuguang Project,and Fundamental Research Funds for the Central Universities(grant no.CCNU22QN008,CCNU24JCPT017).
文摘Reticular chemistry enables the precise design and synthesis of crystalline extended materials,however,its application in hierarchical self-assembly of superstructures remains challenging due to the limited control over weak interactions between synthons,in contrast to the stronger coordination or covalent bonds typically involved.Herein,we introduce an anion-competitive strategy to control the topology and structural diversity of superstructures.Cationic tetrahedral Zr-based metal–organic polyhedra were used as cage-like synthons,which were charge-balanced by Cl^(-)ions and interconnected via hydrogen bonds to form hierarchical superstructures.Introducing trigonal planar NO_(3)^(-)ions to compete with spherical Cl^(-)ions produced three new superstructures featuring different hydrogen bond-based linkages and distinct topologies(dia,bnn,and xhy),diverging from the previously reported flu topology.Furthermore,the superstructures with dia and bnn topologies exhibit high porosities and record iodine adsorption capacities in solution(4.31 and 4.19 g·g^(-1),respectively).This work demonstrates the potential of reticular chemistry for the versatile design and construction of diversified hierarchical superstructures.
基金the Thousand Tal-ents Program for Young Scholars,the Shenzhen Science and Technology Innovation Committee(No.JCYJ20190809142809370)the Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002).
文摘Main observation and conclusion An anodic oxidation enabled synthesis of hypervalent iodinel(Ⅲ)reagents from aryl iodides is demonstrated.Under mild electrochem-ical conditions,a range of arylidine(Ⅲ)reagents including iodosylarenes,(difunctionaliodo)arenes,benziodoxoles and diaryliodoni-um salts can be efficiently synthesized and derivatized in good to excellent yields with high selectivity.As only electrons serve as the oxidation reagents,this method offers a more straightforward and sustainable manner avoiding the use of expensive or hazardous chemical oxidants.
基金supported by the National Natural Science Foundation of China(22076196,U22B20139,12175024,21906163,22276147,and 22076152).
文摘Exploring the physiochemical properties and expanding the applications of actinide-containing materials is paramount to address the escalating challenge of radioactive waste accumulation.However,unlocking the full potential of these materials is largely crippled by the radiotoxicity of the actinides.We report here two porous and luminescent thorium-based metal-organic frameworks(Th-BITD-1 and Th-BITD-2)that serve as a bifunctional platform for sequencing and sensing of radioiodine,a much more radioactive fission product discharged during the nuclear fuel reprocessing.In particular,Th-BITD-1 displays better iodine uptake performance than Th-BITD-2 via the solution-based process and vapor diffusion with the maximum adsorption capacities of 831 and 1099 mg/g,respectively.Fur thermore,Th-BITD-1 can function as a highly sensitive luminescence sensor for iodate with a quenching constant(Ksv)of 6.6(5)×10^(3) M^(-1)and a detection limit of 2.02μM,respectively,outperforming 2.96(6)×10^(3)M^(-1)and 10.5μM of Th-BITD-2.Moreover,a positive correlation between the sensing efficacy and the iodate adsorption capacity has been revealed.This work highlights the opportunity in designing novel actinide-based MOFs for their potential applications in radiological fields,e.g.,radionuclide separation and detection.
基金Financial support from the National Natural Science Foundation of China(Nos.22271244,22201240,and 21871226)the Hunan Provincial Natural Science Foundation of China(No.2020JJ5531)+1 种基金Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal University(2022C02)the Undergraduate Investigated Study and Innovated Experiment Plan from Ministry of Education of China and the Science and Technology Innovation Program of Hunan Province(2020RC1009)is gratefully acknowledged.
文摘Comprehensive Summary,A convenient approach for the construction of 2-aminobenzothiazoles via I2-catalyzed tandem cyclization reaction of amines and carbon disulfide has been developed.The present approach starts from simple and readily available starting materials,affording a series of 2-aminobenzothiazoles in up to 89%yields under metal-free conditions.In this work,C—H/N—H functionalization was achieved and multiple C-hetero bonds were successfully constructed in one pot.
