Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state el...Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state electrolytes(PSEs)are competitive candidates for replacing commercial liquid electrolytes due to their flexibility,shape versatility and easy machinability.Despite the rapid development of PSEs,their practical application still faces obstacles including poor ionic conductivity,narrow electrochemical stable window and inferior mechanical strength.Polymer/inorganic composite electrolytes(PIEs)formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes(ISEs),exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics.Some PIEs are highly compatible with high-voltage cathode and lithium metal anode,which offer desirable access to obtaining lithium metal batteries with high energy density.This review elucidates the current issues and recent advances in PIEs.The performance of PIEs was remarkably influenced by the characteristics of the fillers including type,content,morphology,arrangement and surface groups.We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs.Finally,the obstacles and opportunities for creating high-performance PIEs are outlined.This review aims to provide some theoretical guidance and direction for the development of PIEs.展开更多
Lithium metal is one of the most promising anodes for next-generation batteries due to its high capacity and low reduction potential.However,the notorious Li dendrites can cause the short life span and safety issues,h...Lithium metal is one of the most promising anodes for next-generation batteries due to its high capacity and low reduction potential.However,the notorious Li dendrites can cause the short life span and safety issues,hindering the extensive application of lithium batteries.Herein,Li_(7)La_(3)Zr_(2)O_(12)(LLZO)ceramics are integrated into polyethylene oxide(PEO)to construct a facile polymer/inorganic composite solid-state electrolyte(CSSE)to inhibit the growth of Li dendrites and widen the electrochemical stability window.Given the feasibility of our strategy,the designed PEO-LLZO-LiTFSI composite solid-state electrolyte(PLLCSSE)exhibits an outstanding cycling property of 134.2 mAh g^(-1) after 500 cycles and the Coulombic efficiency of 99.1%after 1000 cycles at 1 C in LiFePO_(4)-Li cell.When cooperated with LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)cathode,the PLL-CSSE renders a capacity retention of 82.4%after 200 cycles at 0.2 C.More importantly,the uniform dispersion of LLZO in PEO matrix is tentative tested via Raman and FT-IR spectra and should be responsible for the improved electrochemical performance.The same conclusion can be drawn from the interface investigation after cycling.This work presents an intriguing solid-state electrolyte with high electrochemical performance,which will boost the development of all-solid-state lithium batteries with high energy density.展开更多
Narrow spectral response,low charge separation efficiency and slow water oxidation kinetics of TiO_(2)limit its application in photoelectrochemical and photocatalytic water splitting.Herein,a promising organic/inorgan...Narrow spectral response,low charge separation efficiency and slow water oxidation kinetics of TiO_(2)limit its application in photoelectrochemical and photocatalytic water splitting.Herein,a promising organic/inorganic composite catalyst Ag/PANI/3DOMM‐TiO_(2–x)with a three‐dimensional ordered macro‐and meso‐porous(3DO MM)structure,oxygen vacancy and Ti^(3+)defects,heterojunction formation and noble metal Ag was designed based on the Z‐scheme mechanism and successfully prepared.The Ag/PANI/3DOMM‐TiO_(2–x)ternary catalyst exhibited enhanced hydrogen production activity in both photocatalytic and photoelectrochemical water splitting.The photocatalytic hydrogen production rate is 420.90μmol g^(–1)h^(–1),which are 19.80 times and 2.06 times higher than the commercial P25 and 3DOMM‐TiO_(2),respectively.In the photoelectrochemical tests,the Ag/PANI/3DOMM‐TiO_(2–x)photoelectrode shows enhanced separation and transfer of carriers with a high current density of 1.55 mA cm^(–2)at equilibrium potential of 1.23 V under simulated AM 1.5 G illumination,which is approximately 5 times greater than the 3DOMM‐TiO_(2).The present work has demonstrated the promising potential of organic/inorganic Z‐scheme photocatalyst in driving water splitting for hydrogen production.展开更多
To assess the effects of river damming on dissolved inorganic carbon in the Jialing River, a total of 40 water samples, including inflow, outflow, and stratified water in four cascade reservoirs(Tingzikou, Xinzheng,Do...To assess the effects of river damming on dissolved inorganic carbon in the Jialing River, a total of 40 water samples, including inflow, outflow, and stratified water in four cascade reservoirs(Tingzikou, Xinzheng,Dongxiguan, Caojie) were collected in January and July,2016. The major cations, anions, and δ^(13)C_(DIC) values were analyzed. It was found that the dissolved compositions are dominated by carbonate weathering, while sulfuric acids may play a relatively important role during carbonate weathering and increasing DIC concentration. Different reservoirs had variable characteristics of water physiochemical stratification. The DIC concentrations of reservoir water were lower in summer than those in winter due to the dilute effects and intensive aquatic photosynthesis, as well as imported tributaries. The δ^(13)C_(DIC) values in Tingzikou Reservoir were higher during summer than those in winter,which indicated that intensive photosynthesis increased the δ^(13)C_(DIC) values in residual water, but a similar trend was not obvious in other reservoirs. Except for in Xinzheng Reservoir, the δ^(13)C_(DIC) values in inflow and outflow reservoir water were lower than those in the surface water of stratified sampling in summer. For stratified sampling, it could be found that, in summer, the Tingzikou Reservoir δ^(13)C_(DIC) values significantly decreased with water depthdue to the anaerobic breakdown of organic matter. The significant correlation(p<0.01 or 0.05) between the DIC concentrations, the δ^(13)C_(DIC) values and anthropogenic species(Na^++K^+, Cl~–, SO_4^(2-) and NO_3^-) showed that the isotope composition of DIC can be a useful tracer of contaminants. In total, Tingzikou Reservoir showed lacustrine features, Xinzheng Reservoir and Dongxiguan Reservoir had "transitional'' features, and Caojie Reservoir had a total of "fluvial'' features. Generally, cascade reservoirs in the Jialing River exhibited natural river features rather than typical lake features due to characteristics of reservoir water in physiochemical stratification, spatiotemporal variations of DIC concentrations and isotopic compositions. It is evident that the dissolved inorganic carbon dynamics of natural rivers had been partly remolded by dam building.展开更多
Lithium sulfur batteries are regarded as a promising candidate for high-energy-density energy storage devices.However,the lithium metal anode in lithium-sulfur batteries encounters the problem of lithium dendrites and...Lithium sulfur batteries are regarded as a promising candidate for high-energy-density energy storage devices.However,the lithium metal anode in lithium-sulfur batteries encounters the problem of lithium dendrites and lithium metal consumption caused by polysulfide corrosion.Herein we design a dualfunction PMMA/PPC/LiNO3composite as an artificial solid electrolyte interphase(PMCN-SEI)to protect Li metal anode.This SEI offers multiple sites of C=O for polysulfide anchoring to constrain corrosion of Li metal anode.The lithiated polymer group and Li3N in PMCN-SEI can homogenize lithium-ion deposition behavior to achieve a dendrite-free anode.As a result,the PMCN-SEI protected Li metal anode enables the Li||Li symmetric batteries to maintain over 300 cycles(1300 h)at a capacity of 5 m Ah cm^(-2),corresponding to a cumulative capacity of 3.25 Ah cm^(-2).Moreover,Li-S batteries assembled with 20μm of Li metal anode(N/P=1.67)still deliver an initial capacity of 1166 m A h g-1at 0.5C.Hence,introducing polycarbonate polymer/inorganic composite SEI on Li provides a new solution for achieving the high energy density of Li-S batteries.展开更多
Halide perovskite light-emitting electrochemical cells are a novel type of the perovskite optoelectronic devices that differs from the perovskite light-emitting diodes by a simple monolayered architecture.Here,we deve...Halide perovskite light-emitting electrochemical cells are a novel type of the perovskite optoelectronic devices that differs from the perovskite light-emitting diodes by a simple monolayered architecture.Here,we develop a perovskite electrochemical cell both for light emission and detection,where the active layer consists of a composite material made of halide perovskite microcrystals,polymer support matrix,and added mobile ions.The perovskite electrochemical cell of CsPbBr3:PEO:LiTFSI composition,emitting light at the wavelength of 523 nm,yields the luminance more than 7000 cd/m2 and electroluminescence efficiency of 4.3 lm/W.The device fabricated on a silicon substrate with transparent single-walled carbon nanotube film as a top contact exhibits 40%lower Joule heating compared to the perovskite optoelectronic devices fabricated on conventional ITO/glass substrates.Moreover,the device operates as a photodetector with a sensitivity up to 0.75 A/W,specific detectivity of 8.56×1011 Jones,and linear dynamic range of 48 dB.The technological potential of such a device is proven by demonstration of 24-pixel indicator display as well as by successful device miniaturization by creation of electroluminescent images with the smallest features less than 50μm.展开更多
Conjugated microporous polymer(CMP)is an emerging organic semiconductor withπ-conjugated skeletons,and the bandgap of CMP can be flexibly modulated to harvest visible light.Based on the diversity and adjustability of...Conjugated microporous polymer(CMP)is an emerging organic semiconductor withπ-conjugated skeletons,and the bandgap of CMP can be flexibly modulated to harvest visible light.Based on the diversity and adjustability of monomers in CMP,we designed and synthesized donor-accepter(D-A)type BTNCMP through Sonogashira-Hagihara cross-coupling polymerization,further in-situ constructing series of inorganic/organic Z-scheme BW/BTN-n composite in the presence of Bi_(2)WO_(6).After optimization,the tetracycline hydrochloride(C0=10 mg·L^(-1))degradation efficiency reached 84%with BW/BTN-2 as catalyst in 90 min under visible light irradiation,the apparent rate constant k1 is 0.017 min^(-1),which is 1.7 and 5.7 times higher than bare Bi_(2)WO_(6) and BTN-CMP.X-ray photoelectron spectra and UV-Vis diffuse spectra showed that the enhanced photocatalytic activity originated from the tight heterojunction between Bi_(2)WO_(6) and BTN-CMP,which can extend the light absorption range and facilitate the separation and transport of photogenerated charges in the interface of heterojunction.The active species trapping experiments and electron spin resonance technique revealed that h+was the dominant active species during the photodegradation process of tetracycline hydrochloride(TCH).The present study demonstrated the feasibility to construct inorganic/organic composite for the photocatalytic degradation of environmental pollutants.展开更多
Particulate matter with diameters≤2.5μm(PM_(2.5))has been identified as a significant air pollutant contributing to premature mortality.Nevertheless,the specific compositions within PM_(2.5) that play the most cruci...Particulate matter with diameters≤2.5μm(PM_(2.5))has been identified as a significant air pollutant contributing to premature mortality.Nevertheless,the specific compositions within PM_(2.5) that play the most crucial role remain unclear,especially in areas with high pollution concentrations.This study aims to investigate the individual and joint mortality risks associated with PM_(2.5) inorganic chemical compositions and identify primary contributors.In 1998,we conducted a prospective cohort study in four northern Chinese cities(Tianjin,Shenyang,Taiyuan,and Rizhao).Satellite-based machine learning models calculated PM_(2.5) inorganic chemical compositions,including sulfate(SO_(4)^(2–)),nitrate(NO_(3)^(–)),ammonium(NH_(4)^(+)),and chloride(Cl^(-)).A time-varying Cox proportional hazards model was applied to analyze associations between these compositions and cardiorespiratory mortality,encompassing nonaccidental causes,cardiovascular diseases(CVDs),nonmalignant respiratory diseases(RDs),and lung cancer.The quantile-based g-computation model evaluated joint exposure effects and relative contributions of the compositions.Stratified analysis was used to identify vulnerable subpopulations.During 785,807 person-years of follow-up,5812(15.5%)deaths occurred from nonaccidental causes,including 2932(7.8%)from all CVDs,479(1.3%)from nonmalignant RDs,and 552(1.4%)from lung cancer.Every interquartile range(IQR)increase in SO_(4)^(2–)was associated with mortality from nonaccidental causes(hazard ratio:1.860;95%confidence interval:1.809,1.911),CVDs(1.909;1.836,1.985),nonmalignant RDs(2.178;1.975,2.403),and lung cancer(1.773;1.624,1.937).In the joint exposure model,a simultaneous rise of one IQR in all four compositions increased the risk of cardiorespiratory mortality by at least 36.3%,with long-term exposure to SO_(4)^(2–)contributing the most to nonaccidental and cardiopulmonary deaths.Individuals with higher incomes and lower education levels were found to be more vulnerable.Long-term exposure to higher levels of PM_(2.5) inorganic compositions was associated with significantly increased cardiopulmonary mortality,with SO_(4)^(2–)potentially being the primary contributor.These findings offer insights into how PM_(2.5) sources impact health,aiding the development of more effective governance measures.展开更多
A detailed computational investigation,based on density functional theory,of the interaction of polyani-line(PANI)and graphene nanoribbons(GNRs)with SrTiO_(3) is presented.The adsorption of PANI in var-ious oxidation ...A detailed computational investigation,based on density functional theory,of the interaction of polyani-line(PANI)and graphene nanoribbons(GNRs)with SrTiO_(3) is presented.The adsorption of PANI in var-ious oxidation states and co-adsorption with GNRs is found to be thermodynamically favourable.Ad-sorbed PANI introduces N and C 2p states into the SrTiO_(3) bandgap,while co-adsorption of PANI and GNRs leads to a bridging of the gap and semi-metallic behaviour,thus rendering the electrical properties highly sensitive to the loading of the GNRs/PANI in the composites.Modelling the lattice dynamics of the composites predicts a 68-88%reduction in the lattice thermal conductivity due to reduced phonon group velocities.Taken together,these findings provide insight into the growing number of experimental studies highlighting the enhanced thermoelectric performance of oxide-polymer composites and indicate co-adsorption with graphene as a facile direction for future research.展开更多
Research and development of the ideal artificial bone-substitute materials to replace autologous and allogeneic bones for repairing bone defects is still a challenge in clinical orthopedics.Recently,poly(lactic-co-gly...Research and development of the ideal artificial bone-substitute materials to replace autologous and allogeneic bones for repairing bone defects is still a challenge in clinical orthopedics.Recently,poly(lactic-co-glycolic acid)(PLGA)-based artificial bone-substitute materials are attracting increasing attention as the benefit of their suitable biocompatibility,degradability,mechanical properties,and capabilities to promote bone regeneration.In this article,we comprehensively review the artificial bone-substitute materials made from PLGA or the composites of PLGA and other organic and inorganic substances,elaborate on their applications for bone regeneration with or without bioactive factors,and prospect the challenges and opportunities in clinical bone regeneration.展开更多
To compare the inorganic chemical compositions of TSP(total suspended paniculate),PM10(particulate matter with an aerodynamic diameter less than 10 μm) and PM2.5(particulate matter with an aerodynamic diameter l...To compare the inorganic chemical compositions of TSP(total suspended paniculate),PM10(particulate matter with an aerodynamic diameter less than 10 μm) and PM2.5(particulate matter with an aerodynamic diameter less than 2.5 μm) in southern and northern cities in China,atmospheric particles were synchronously collected in Dalian(the northern city)and Xiamen(the southern city) in spring and autumn of 2004.The mass concentrations,twenty-three elements and nine soluble ions were assessed.The results show that in Dalian,the mass concentrations of Mg,Al,Ca,Mn and Fe in spring were 4.0-10.1,2.6-8.0,4.1-12,1.2-3.6 and 2.9-7.9 times higher,respectively,than those in Xiamen.The dust storm influence is more obvious in Dalian in spring.However,in Xiamen,heavy metals accounted for 13.9%-17.9%of TSP,while heavy metals contributed to 5.5%-9.3%of TSP in Dalian.These concentrations suggest that heavy metal pollution in Xiamen was more serious.In addition,the concentrations of Na+,Cl-,Ca2+ and Mg2+ were higher in Dalian due to the influence of marine aerosol,construction activities and soil dust.The NO3-/SO42- ratios in Dalian(0.25-0.49) were lower than those in Xiamen(0.51-0.62),indicating that the contributions of vehicle emission to particles in Xiamen were higher.Coefficient of divergence values was higher than 0.40,implying that the inorganic chemical composition profiles for the particles of Dalian and Xiamen were quite different from each other.展开更多
Haze episodes have become a major concern in Malaysia over the past few decades and have an increasingly important impact on the country each and every year. During haze episodes from biomass burning in Southeast Asia...Haze episodes have become a major concern in Malaysia over the past few decades and have an increasingly important impact on the country each and every year. During haze episodes from biomass burning in Southeast Asia, particularly from Sumatra, Indonesia, particulate matter PM2.5 is found to be one of the dangerous sources of airborne pollution and is known to seriously affect human health. This study determines the composition of carbohydrates (as levoglucosan), surfactants, major elements, and anions in PM2.5 during a 2013 haze episode. PM2.5 samples were collected from Universiti Kebangsaan Malaysia, Bangi, using a high volume sampler during a seven-day monitoring campaign during the peak of that year's haze episode. PM2.5 concentrations ranged between 14.52 and 160.93 μg/m3, exceeding the 2005 WHO air quality guidelines for PM2.5 (25 μg/m3 for 24-h mean). The patterns for levoglucosan, surfactants, major elements, and anionic compositions were proportional to the PM2.5 concentrations. Changes in PM2.5 observed on days 3 and 4 were influenced by a combination of meteorological factors, which substantiate the theory that such factors play a pivotal role in haze episodes.展开更多
基金the National Natural Science Foundation of China(Nos.22279070,U21A20170 and 22175106)the Ministry of Science and Technology of China(Nos.2019YFA0705703,2021YFB2501900 and 2019YFE0100200)+1 种基金the Tsinghua University Initiative Scientific Research Program(20223080001)the Tsinghua-Foshan Innovation Special Fund(2021THFS0216)。
文摘Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state electrolytes(PSEs)are competitive candidates for replacing commercial liquid electrolytes due to their flexibility,shape versatility and easy machinability.Despite the rapid development of PSEs,their practical application still faces obstacles including poor ionic conductivity,narrow electrochemical stable window and inferior mechanical strength.Polymer/inorganic composite electrolytes(PIEs)formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes(ISEs),exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics.Some PIEs are highly compatible with high-voltage cathode and lithium metal anode,which offer desirable access to obtaining lithium metal batteries with high energy density.This review elucidates the current issues and recent advances in PIEs.The performance of PIEs was remarkably influenced by the characteristics of the fillers including type,content,morphology,arrangement and surface groups.We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs.Finally,the obstacles and opportunities for creating high-performance PIEs are outlined.This review aims to provide some theoretical guidance and direction for the development of PIEs.
基金financially supported partly by the National Key Research and Development Program of China(2018YFE0111600)the Tianjin Sci.&Tech.Program(17YFZCGX00560)the Young Elite Scientists Sponsorship Program by Tianjin(TJSQNTJ-2017-05)。
文摘Lithium metal is one of the most promising anodes for next-generation batteries due to its high capacity and low reduction potential.However,the notorious Li dendrites can cause the short life span and safety issues,hindering the extensive application of lithium batteries.Herein,Li_(7)La_(3)Zr_(2)O_(12)(LLZO)ceramics are integrated into polyethylene oxide(PEO)to construct a facile polymer/inorganic composite solid-state electrolyte(CSSE)to inhibit the growth of Li dendrites and widen the electrochemical stability window.Given the feasibility of our strategy,the designed PEO-LLZO-LiTFSI composite solid-state electrolyte(PLLCSSE)exhibits an outstanding cycling property of 134.2 mAh g^(-1) after 500 cycles and the Coulombic efficiency of 99.1%after 1000 cycles at 1 C in LiFePO_(4)-Li cell.When cooperated with LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)cathode,the PLL-CSSE renders a capacity retention of 82.4%after 200 cycles at 0.2 C.More importantly,the uniform dispersion of LLZO in PEO matrix is tentative tested via Raman and FT-IR spectra and should be responsible for the improved electrochemical performance.The same conclusion can be drawn from the interface investigation after cycling.This work presents an intriguing solid-state electrolyte with high electrochemical performance,which will boost the development of all-solid-state lithium batteries with high energy density.
文摘Narrow spectral response,low charge separation efficiency and slow water oxidation kinetics of TiO_(2)limit its application in photoelectrochemical and photocatalytic water splitting.Herein,a promising organic/inorganic composite catalyst Ag/PANI/3DOMM‐TiO_(2–x)with a three‐dimensional ordered macro‐and meso‐porous(3DO MM)structure,oxygen vacancy and Ti^(3+)defects,heterojunction formation and noble metal Ag was designed based on the Z‐scheme mechanism and successfully prepared.The Ag/PANI/3DOMM‐TiO_(2–x)ternary catalyst exhibited enhanced hydrogen production activity in both photocatalytic and photoelectrochemical water splitting.The photocatalytic hydrogen production rate is 420.90μmol g^(–1)h^(–1),which are 19.80 times and 2.06 times higher than the commercial P25 and 3DOMM‐TiO_(2),respectively.In the photoelectrochemical tests,the Ag/PANI/3DOMM‐TiO_(2–x)photoelectrode shows enhanced separation and transfer of carriers with a high current density of 1.55 mA cm^(–2)at equilibrium potential of 1.23 V under simulated AM 1.5 G illumination,which is approximately 5 times greater than the 3DOMM‐TiO_(2).The present work has demonstrated the promising potential of organic/inorganic Z‐scheme photocatalyst in driving water splitting for hydrogen production.
基金financially supported by the National Key Research and Development Program of China(2016YFA0601000)the National Natural Science Foundation of China(Grant No.41373136)
文摘To assess the effects of river damming on dissolved inorganic carbon in the Jialing River, a total of 40 water samples, including inflow, outflow, and stratified water in four cascade reservoirs(Tingzikou, Xinzheng,Dongxiguan, Caojie) were collected in January and July,2016. The major cations, anions, and δ^(13)C_(DIC) values were analyzed. It was found that the dissolved compositions are dominated by carbonate weathering, while sulfuric acids may play a relatively important role during carbonate weathering and increasing DIC concentration. Different reservoirs had variable characteristics of water physiochemical stratification. The DIC concentrations of reservoir water were lower in summer than those in winter due to the dilute effects and intensive aquatic photosynthesis, as well as imported tributaries. The δ^(13)C_(DIC) values in Tingzikou Reservoir were higher during summer than those in winter,which indicated that intensive photosynthesis increased the δ^(13)C_(DIC) values in residual water, but a similar trend was not obvious in other reservoirs. Except for in Xinzheng Reservoir, the δ^(13)C_(DIC) values in inflow and outflow reservoir water were lower than those in the surface water of stratified sampling in summer. For stratified sampling, it could be found that, in summer, the Tingzikou Reservoir δ^(13)C_(DIC) values significantly decreased with water depthdue to the anaerobic breakdown of organic matter. The significant correlation(p<0.01 or 0.05) between the DIC concentrations, the δ^(13)C_(DIC) values and anthropogenic species(Na^++K^+, Cl~–, SO_4^(2-) and NO_3^-) showed that the isotope composition of DIC can be a useful tracer of contaminants. In total, Tingzikou Reservoir showed lacustrine features, Xinzheng Reservoir and Dongxiguan Reservoir had "transitional'' features, and Caojie Reservoir had a total of "fluvial'' features. Generally, cascade reservoirs in the Jialing River exhibited natural river features rather than typical lake features due to characteristics of reservoir water in physiochemical stratification, spatiotemporal variations of DIC concentrations and isotopic compositions. It is evident that the dissolved inorganic carbon dynamics of natural rivers had been partly remolded by dam building.
基金supported by the Jilin Province Science and Technology Department Program(YDZJ202201ZYTS304)the Science and Technology Project of Jilin Provincial Education Department(JJKH20220428KJ)+3 种基金the Jilin Province Science and Technology Department Program(YDZJ202101ZYTS047)the National Natural Science Foundation of China(21905110,21905041,22279045,22102020)the Special foundation of Jilin Province Industrial Technology Research and Development(2019C042)the Fundamental Research Funds for the Central Universities(2412020FZ008)。
文摘Lithium sulfur batteries are regarded as a promising candidate for high-energy-density energy storage devices.However,the lithium metal anode in lithium-sulfur batteries encounters the problem of lithium dendrites and lithium metal consumption caused by polysulfide corrosion.Herein we design a dualfunction PMMA/PPC/LiNO3composite as an artificial solid electrolyte interphase(PMCN-SEI)to protect Li metal anode.This SEI offers multiple sites of C=O for polysulfide anchoring to constrain corrosion of Li metal anode.The lithiated polymer group and Li3N in PMCN-SEI can homogenize lithium-ion deposition behavior to achieve a dendrite-free anode.As a result,the PMCN-SEI protected Li metal anode enables the Li||Li symmetric batteries to maintain over 300 cycles(1300 h)at a capacity of 5 m Ah cm^(-2),corresponding to a cumulative capacity of 3.25 Ah cm^(-2).Moreover,Li-S batteries assembled with 20μm of Li metal anode(N/P=1.67)still deliver an initial capacity of 1166 m A h g-1at 0.5C.Hence,introducing polycarbonate polymer/inorganic composite SEI on Li provides a new solution for achieving the high energy density of Li-S batteries.
基金M.Baeva,A.Vorobyov,V.Neplokh acknowledge the Russian Science Foundation No.22-79-10286(https://rscf.ru/project/22-79-10286/)for supporting silicon substrate processing.D.Gets,APolushkin and S.Makarov acknowledge the Ministry of Science and Higher Education of the Russian Federation(Project 075-15-2021-589)for supporting perovskite synthesisA.G.Nasibulin and D.V.Krasnikov acknowledge the Russian Science Foundation(grant No.20-73-10256)for supporting synthesis of SWCNTs.
文摘Halide perovskite light-emitting electrochemical cells are a novel type of the perovskite optoelectronic devices that differs from the perovskite light-emitting diodes by a simple monolayered architecture.Here,we develop a perovskite electrochemical cell both for light emission and detection,where the active layer consists of a composite material made of halide perovskite microcrystals,polymer support matrix,and added mobile ions.The perovskite electrochemical cell of CsPbBr3:PEO:LiTFSI composition,emitting light at the wavelength of 523 nm,yields the luminance more than 7000 cd/m2 and electroluminescence efficiency of 4.3 lm/W.The device fabricated on a silicon substrate with transparent single-walled carbon nanotube film as a top contact exhibits 40%lower Joule heating compared to the perovskite optoelectronic devices fabricated on conventional ITO/glass substrates.Moreover,the device operates as a photodetector with a sensitivity up to 0.75 A/W,specific detectivity of 8.56×1011 Jones,and linear dynamic range of 48 dB.The technological potential of such a device is proven by demonstration of 24-pixel indicator display as well as by successful device miniaturization by creation of electroluminescent images with the smallest features less than 50μm.
基金supported by the National Natural Science Foundation of China(91834301 and 21878076)the Science and Technology Commission of Shanghai Municipality(19160712100)。
文摘Conjugated microporous polymer(CMP)is an emerging organic semiconductor withπ-conjugated skeletons,and the bandgap of CMP can be flexibly modulated to harvest visible light.Based on the diversity and adjustability of monomers in CMP,we designed and synthesized donor-accepter(D-A)type BTNCMP through Sonogashira-Hagihara cross-coupling polymerization,further in-situ constructing series of inorganic/organic Z-scheme BW/BTN-n composite in the presence of Bi_(2)WO_(6).After optimization,the tetracycline hydrochloride(C0=10 mg·L^(-1))degradation efficiency reached 84%with BW/BTN-2 as catalyst in 90 min under visible light irradiation,the apparent rate constant k1 is 0.017 min^(-1),which is 1.7 and 5.7 times higher than bare Bi_(2)WO_(6) and BTN-CMP.X-ray photoelectron spectra and UV-Vis diffuse spectra showed that the enhanced photocatalytic activity originated from the tight heterojunction between Bi_(2)WO_(6) and BTN-CMP,which can extend the light absorption range and facilitate the separation and transport of photogenerated charges in the interface of heterojunction.The active species trapping experiments and electron spin resonance technique revealed that h+was the dominant active species during the photodegradation process of tetracycline hydrochloride(TCH).The present study demonstrated the feasibility to construct inorganic/organic composite for the photocatalytic degradation of environmental pollutants.
基金National Key Research and Development Program of China(Grants 2017YFC0211605 and 2017YFC0211704).
文摘Particulate matter with diameters≤2.5μm(PM_(2.5))has been identified as a significant air pollutant contributing to premature mortality.Nevertheless,the specific compositions within PM_(2.5) that play the most crucial role remain unclear,especially in areas with high pollution concentrations.This study aims to investigate the individual and joint mortality risks associated with PM_(2.5) inorganic chemical compositions and identify primary contributors.In 1998,we conducted a prospective cohort study in four northern Chinese cities(Tianjin,Shenyang,Taiyuan,and Rizhao).Satellite-based machine learning models calculated PM_(2.5) inorganic chemical compositions,including sulfate(SO_(4)^(2–)),nitrate(NO_(3)^(–)),ammonium(NH_(4)^(+)),and chloride(Cl^(-)).A time-varying Cox proportional hazards model was applied to analyze associations between these compositions and cardiorespiratory mortality,encompassing nonaccidental causes,cardiovascular diseases(CVDs),nonmalignant respiratory diseases(RDs),and lung cancer.The quantile-based g-computation model evaluated joint exposure effects and relative contributions of the compositions.Stratified analysis was used to identify vulnerable subpopulations.During 785,807 person-years of follow-up,5812(15.5%)deaths occurred from nonaccidental causes,including 2932(7.8%)from all CVDs,479(1.3%)from nonmalignant RDs,and 552(1.4%)from lung cancer.Every interquartile range(IQR)increase in SO_(4)^(2–)was associated with mortality from nonaccidental causes(hazard ratio:1.860;95%confidence interval:1.809,1.911),CVDs(1.909;1.836,1.985),nonmalignant RDs(2.178;1.975,2.403),and lung cancer(1.773;1.624,1.937).In the joint exposure model,a simultaneous rise of one IQR in all four compositions increased the risk of cardiorespiratory mortality by at least 36.3%,with long-term exposure to SO_(4)^(2–)contributing the most to nonaccidental and cardiopulmonary deaths.Individuals with higher incomes and lower education levels were found to be more vulnerable.Long-term exposure to higher levels of PM_(2.5) inorganic compositions was associated with significantly increased cardiopulmonary mortality,with SO_(4)^(2–)potentially being the primary contributor.These findings offer insights into how PM_(2.5) sources impact health,aiding the development of more effective governance measures.
基金NDW thanks the EPSRC DTP competition 2018-19 at the University of Huddersfield for funding(EP/R513234/1)JMS is currently supported by a UKRI Future Leaders Fellowship(MR/T043121/1)+2 种基金previously held a University of Manchester Presidential Fellowship.Calculations were performed on the Orion computing fa-cility and the Violeta HPC at the University of Huddersfield,and the THOMAS and YOUNG facilities at the UK Materials and Molecular Modelling Hub(MMM Hub)which is partially funded by the EPSRC(EP/P020194/1 and EP/T022213/1)via our membership of the UK’s HEC Materials Chemistry Consortium(MCC),which is also funded by the EPSRC(EP/R029431/1 and EP/X035859/1).
文摘A detailed computational investigation,based on density functional theory,of the interaction of polyani-line(PANI)and graphene nanoribbons(GNRs)with SrTiO_(3) is presented.The adsorption of PANI in var-ious oxidation states and co-adsorption with GNRs is found to be thermodynamically favourable.Ad-sorbed PANI introduces N and C 2p states into the SrTiO_(3) bandgap,while co-adsorption of PANI and GNRs leads to a bridging of the gap and semi-metallic behaviour,thus rendering the electrical properties highly sensitive to the loading of the GNRs/PANI in the composites.Modelling the lattice dynamics of the composites predicts a 68-88%reduction in the lattice thermal conductivity due to reduced phonon group velocities.Taken together,these findings provide insight into the growing number of experimental studies highlighting the enhanced thermoelectric performance of oxide-polymer composites and indicate co-adsorption with graphene as a facile direction for future research.
基金This study was financially supported by the National Natural Science Foundation of China(Grant Nos.51973216,51873207,51803006,and 51833010)the Science and Technology Development Program of Jilin Province(Grant No.20200404182YY)+1 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Grant No.2019005)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology)(Grant No.2020-KF-5).
文摘Research and development of the ideal artificial bone-substitute materials to replace autologous and allogeneic bones for repairing bone defects is still a challenge in clinical orthopedics.Recently,poly(lactic-co-glycolic acid)(PLGA)-based artificial bone-substitute materials are attracting increasing attention as the benefit of their suitable biocompatibility,degradability,mechanical properties,and capabilities to promote bone regeneration.In this article,we comprehensively review the artificial bone-substitute materials made from PLGA or the composites of PLGA and other organic and inorganic substances,elaborate on their applications for bone regeneration with or without bioactive factors,and prospect the challenges and opportunities in clinical bone regeneration.
基金supported by the National Natural Science Foundation of China(No.41175111)
文摘To compare the inorganic chemical compositions of TSP(total suspended paniculate),PM10(particulate matter with an aerodynamic diameter less than 10 μm) and PM2.5(particulate matter with an aerodynamic diameter less than 2.5 μm) in southern and northern cities in China,atmospheric particles were synchronously collected in Dalian(the northern city)and Xiamen(the southern city) in spring and autumn of 2004.The mass concentrations,twenty-three elements and nine soluble ions were assessed.The results show that in Dalian,the mass concentrations of Mg,Al,Ca,Mn and Fe in spring were 4.0-10.1,2.6-8.0,4.1-12,1.2-3.6 and 2.9-7.9 times higher,respectively,than those in Xiamen.The dust storm influence is more obvious in Dalian in spring.However,in Xiamen,heavy metals accounted for 13.9%-17.9%of TSP,while heavy metals contributed to 5.5%-9.3%of TSP in Dalian.These concentrations suggest that heavy metal pollution in Xiamen was more serious.In addition,the concentrations of Na+,Cl-,Ca2+ and Mg2+ were higher in Dalian due to the influence of marine aerosol,construction activities and soil dust.The NO3-/SO42- ratios in Dalian(0.25-0.49) were lower than those in Xiamen(0.51-0.62),indicating that the contributions of vehicle emission to particles in Xiamen were higher.Coefficient of divergence values was higher than 0.40,implying that the inorganic chemical composition profiles for the particles of Dalian and Xiamen were quite different from each other.
文摘Haze episodes have become a major concern in Malaysia over the past few decades and have an increasingly important impact on the country each and every year. During haze episodes from biomass burning in Southeast Asia, particularly from Sumatra, Indonesia, particulate matter PM2.5 is found to be one of the dangerous sources of airborne pollution and is known to seriously affect human health. This study determines the composition of carbohydrates (as levoglucosan), surfactants, major elements, and anions in PM2.5 during a 2013 haze episode. PM2.5 samples were collected from Universiti Kebangsaan Malaysia, Bangi, using a high volume sampler during a seven-day monitoring campaign during the peak of that year's haze episode. PM2.5 concentrations ranged between 14.52 and 160.93 μg/m3, exceeding the 2005 WHO air quality guidelines for PM2.5 (25 μg/m3 for 24-h mean). The patterns for levoglucosan, surfactants, major elements, and anionic compositions were proportional to the PM2.5 concentrations. Changes in PM2.5 observed on days 3 and 4 were influenced by a combination of meteorological factors, which substantiate the theory that such factors play a pivotal role in haze episodes.