The development of highly safe and low-cost aqueous batteries is of great significance in the background of carbon neutrality.However,the practical deployment of aqueous batteries has been plagued due to their relativ...The development of highly safe and low-cost aqueous batteries is of great significance in the background of carbon neutrality.However,the practical deployment of aqueous batteries has been plagued due to their relatively low capacity and poor cycling stability.Herein,we propose unique conversion electrochemistry of copper selenides for robust and energetic aqueous charge storage.In situ X-ray diffraction and operando Raman techniques reveal a reversible transformation from CuSe to Cu_(2)Se through the intermediates of Cu_(3)Se_(2) and Cu_(1.8)Se.Such a conversion process activates the redox carrier of Cu^(2+)ion and delivers a remarkable rate capability of 285 mAh g^(-1) at 20 A g^(-1) and electrochemical durability up to 30,000 cycles.Furthermore,Cu^(2+)and H+coinsertion chemistry is proposed to facilitate the conversion process.As a proof-of-concept,a hybrid aqueous pouch cell coupling CuSe//Zn is capable of affording maximum energy and power densities of 190 Wh kg^(-1) and 1366W kg^(-1),respectively.展开更多
LiMn_(6) hexatomic-rings act as functional units in Li-rich layered oxides(LLOs),which determine the capacity,voltage,and structural stability of LLOs.However,the symmetry of the LiMn_(6) hexatomic-ring is always brok...LiMn_(6) hexatomic-rings act as functional units in Li-rich layered oxides(LLOs),which determine the capacity,voltage,and structural stability of LLOs.However,the symmetry of the LiMn_(6) hexatomic-ring is always broken,especially in the grain surface of LLOs,which will greatly affect its electrochemical performance.Herein,the symmetry-breaking of LiMn_(6) hexatomic-ring in the grain surface of Li_(2)MnO_(3) was studied,and their effect on charge compensation mechanism and structure evolution behavior was thoroughly investigated.The results show that the electrochemical activity of the symmetry-broken LiMn_(6) hexatomic-ring is higher than that of the unbroken LiMn_(6),and the former is more favorable for spinelization on the grain surface.Furthermore,the exposure proportion of crystallographic planes with different symmetry-broken LiMn_(6) hexatomic-ring has also been discussed,which can be adjusted by changing the partial pressure of oxygen.The in-depth understanding of the symmetry-breaking of LiMn_(6) hexatomic-ring will provide more targeted strategies for designing high-performance LLOs cathodes for lithium-ion batteries.展开更多
Despite the significant progress in the fabrication of advanced electrode materials,complex control strategies and tedious processing are often involved for most targeted materials to tailor their compositions,morphol...Despite the significant progress in the fabrication of advanced electrode materials,complex control strategies and tedious processing are often involved for most targeted materials to tailor their compositions,morphologies,and chemistries.Inspired by the unique geometric structures of natural biomacromolecules together with their high affinities for metal species,we propose the use of skin collagen fibers for the template crafting of a novel multicore-shell Fe2N-carbon framework anode configuration,composed of hierarchical N-doped carbon nanofiber bundles firmly embedded with Fe2N nanoparticles(Fe2N@N-CFBs).In the resultant heterostructure,the Fe2N nanoparticles firmly confined inside the carbon shells are spatially isolated but electronically well connected by the long-range carbon nanofiber framework.This not only provides direct and continuous conductive pathways to facilitate electron/ion transport,but also helps cushion the volume expansion of the encapsulated Fe2N to preserve the electrode microstructure.Considering its unique structural characteristics,Fe2N@N-CFBs as an advanced anode material exhibits remarkable electrochemical performances for lithium-and potassium-ion batteries.Moreover,this bio-derived structural strategy can pave the way for novel low-cost and high-efficiency syntheses of metal-nitride/carbon nanofiber heterostructures for potential applications in energy-related fields and beyond.展开更多
Boosting the utilization efficiency of sulfur electrodes and suppressing the“shuttle effect”of intermediate polysulfides remain the critical challenge for high-performance lithium-sulfur batteries(LSBs).However,most...Boosting the utilization efficiency of sulfur electrodes and suppressing the“shuttle effect”of intermediate polysulfides remain the critical challenge for high-performance lithium-sulfur batteries(LSBs).However,most of reported sulfur electrodes are not competent to realize the fast conversion of polysulfides into insoluble lithium sulfides when applied with high sulfur loading,as well as to mitigate the more serious shuttle effect of polysulfides,especially when worked at an elevated temperature.Herein,we reported a unique structural engineering strategy of crafting a unique hierarchical multifunctional electrode architecture constructed by rooting MOF-derived CoS2/carbon nanoleaf arrays(CoS2-CNA)into a nitrogen-rich 3D conductive scaffold(CTNF@CoS2-CNA)for LSBs.An accelerated electrocatalytic effect and improved polysulfide redox kinetics arising from CoS2-CNA were investigated.Besides,the strong capillarity effect and chemisorption of CTNF@CoS2-CNA to polysulfides enable high loading and efficient utilization of sulfur,thus leading to high-performance LIBs performed not only at room temperature but also up to an elevated temperature(55°C).Even with the ultrahigh sulfur loading of 7.19 mg cm?2,the CTNF@CoS2-CNA/S cathode still exhibits high rate capacity at 55°C.展开更多
A decomposition experiment of Populus purdomii litter,a commonly used afforestation species in the Qinling Mountains,China,was conducted.Water extracts of five conifer litters were used to treat P.purdomii litter and ...A decomposition experiment of Populus purdomii litter,a commonly used afforestation species in the Qinling Mountains,China,was conducted.Water extracts of five conifer litters were used to treat P.purdomii litter and its soil.The P.purdomii litter was incubated at room temperature(20–25℃)and constant soil moisture for 6 months.During the decomposition period,the dynamics of litter mass and nutrient contents were detected to investigate the impacts of plant secondary metabolites.The results indicate that litter extracts of Pinus tabuliformis,Platycladus orientalis,Pinus armandii and Larix principisrupprechtii significantly inhibited the overall nutrient release of P.purdomii litter,while the last three types of litter extracts simultaneously inhibited its decomposition.Conversely,the litter extracts of Picea asperata significantly accelerated the overall nutrient release of P.purdomii.Generally,most of the conifer species,whose litter released terpenoids,phenolics,steroids,and aliphatic acids,will inhibit the decomposition and/or nutrient release from P.purdomii litter.Their negative effects on the decomposers and soil enzymatic activities indicates that planting diversity should be lower when mixed planted with P.purdomii.展开更多
With the rapid rise of China’s economy and the deployment of the Belt and Road Initiative,traditional Chinese medicine(TCM),one of the main components of Chinese culture,has become an important aspect of foreign exch...With the rapid rise of China’s economy and the deployment of the Belt and Road Initiative,traditional Chinese medicine(TCM),one of the main components of Chinese culture,has become an important aspect of foreign exchange.Therefore,recent research has focused on how to effectively spread TCM culture internationally and improve TCM acceptance.Australia is currently a representative region with decent TCM development.Taking TCM development in Australia as a starting point,this article analyzes the challenges in TCM development,discusses countermeasures to address these issues,and provides recommendations for improving the international development and dissemination of TCM.展开更多
SeS_(2) has become a promising cathode material owing to its enhanced electrical conductivity over sulfur and higher theoretical specific capacity than selenium;however,the working Li-SeS_(2) batteries have to face th...SeS_(2) has become a promising cathode material owing to its enhanced electrical conductivity over sulfur and higher theoretical specific capacity than selenium;however,the working Li-SeS_(2) batteries have to face the practical challenges from the severe shuttling of soluble dual intermediates of polysulfide and polyselenide,especially in high-SeS_(2)-loading cathodes.Herein,a natural organic polymer,Nicandra physaloides pectin(NPP),is proposed to serve as an effective polysulfide/polyselenide captor to address the shuttling issues.Informed by theoretical calculations,NPP is competent to provide a Lewis base-based strong binding interaction with polysulfides/polyselenides via forming lithium bonds,and it can be homogeneously deposited onto a three-dimensional double-carbon conductive scaffold to finally constitute a polysulfide/polyselenide-immobilizing interlayer.Operando spectroscopy analysis validates the enhanced polysulfide/polyselenide trapping and high conversion efficiency on the constructed interlayer,hence bestowing the Li-SeS_(2) cells with ultrahigh rate capability(448 mAh g^(−1)at 10 A g^(−1)),durable cycling lifespan(≈0.037%capacity attenuation rate per cycle),and high areal capacity(>6.5 mAh cm^(−2))at high SeS_(2) loading of 15.4 mg cm^(−2).Importantly,pouch cells assembled with this interlayer exhibit excellent flexibility,decent rate capability with relatively low electrolyte-to-capacity ratio,and stable cycling life even under a low electrolyte condition,promising a low-cost,viable design protocol toward practical Li-SeS_(2) batteries.展开更多
The rapid expansion of renewable energies asks for great progress of energy-storage technologies for sustainable energy supplies,which raises the compelling demand of high-performance rechargeable batteries.To satisfy...The rapid expansion of renewable energies asks for great progress of energy-storage technologies for sustainable energy supplies,which raises the compelling demand of high-performance rechargeable batteries.To satisfy the huge demand from the coming energy-storage market,the resource and cost-effectiveness of rechargeable batteries become more and more important.Manganese(Mn)as a key transition element with advantages including high abundance,low cost,and low toxicity derives various kinds(spinels,layered oxides,polyanions,Prussian blue analogs,etc.)of high-performance Mn-based electrode materials,especially cathodes,for rechargeable batteries ranging from Li-ion batteries,Na-ion batteries,aqueous batteries,to multivalent metal-ion batteries.It is anticipated that Mn-based materials with Mn as the major transition-metal element will constitute a flourishing family of Mn-based rechargeable batteries(Mn RBs)for large-scale and differentiated energy-storage applications.On the other hand,several critical issues including Jahn-Teller effect,Mn dissolution,and O release greatly hinder the pace of Mn RBs,which require extensive material optimizations and battery/system improvements.This review aims to provide an investigation about Mn-based materials and batteries for the coming energy-storage demands,with compelling issues and challenges that must be overcome.展开更多
Pyrochlore-structured polyantimonic acid(PAA)is a potential high-capacity electrode material,but its innately poor electroconductivity(~10^(-10)S/cm)seriously impairs its electrochemical reversibility for lithium-ion ...Pyrochlore-structured polyantimonic acid(PAA)is a potential high-capacity electrode material,but its innately poor electroconductivity(~10^(-10)S/cm)seriously impairs its electrochemical reversibility for lithium-ion storage.Herein,we report design and synthesis of a novel V-substituted PAA(PAA-V),where V^(5+)are introduced to partially replace Sb^(5+).Owing to identical valence and close ionic radius relative to Sb^(5+),the V^(5+)cation can constitute the covalent VO_6octahedra framework without changing the pyrochlore crystal structure of PAA.As a result,the V^(5+)-substitution is capable to modulate the electronic structure of PAA with significantly improved electrical conductivity(~10^(-6)S/cm for PAA-V)and meanwhile decreases the size of crystals with reduced diffusion length for Li^(+)-ions.With varying the ratio of V^(5+)-substitution,the PAA-V with optimized substitution molar ratio(18%)exhibits the best lithium-ion storage performance,delivering a long cycling life with high reversible capacity(731 m Ah/g after 1200cycles at 1 A/g)and outstanding rate capability(279 mAh/g at 15 A/g).More importantly,by pairing the PAA-V as anode and commercial LiFePO_(4)as cathode,the full cell with a limited negative/positive capacity ratio of 1.2 exhibits decent cycling stability at 1 C after 150 cycles with 85.5%capacity retention.展开更多
Gastric cancer(GC)is the fifth most common cancer and the third leading cause of cancer-related death worldwide[1],Metastasis is the leading cause of GC mortality.The complex dynamic interactions between tumor cells a...Gastric cancer(GC)is the fifth most common cancer and the third leading cause of cancer-related death worldwide[1],Metastasis is the leading cause of GC mortality.The complex dynamic interactions between tumor cells and stromal cells in the tumor microenvironment are crucial for tumor metastasis.Many secreted cytokines have been well documented to mediate the crosstalk between tumor cells and stromal cells in a paracrine manner[2].However,how the juxtacrine signals transduced by adjacent cellcell adhesion modulate cancer metastasis has yet to be elucidated[3].As one of the most important cell-cell adhesion molecules,the classical cadherin superfamily also initiates different intracellular signaling cascades and regulates cytoskeletal dynamics,permeability,cell polarity,and tumor progression[4,5].展开更多
The voltage decay of lithium-rich layered oxides(LLOs)is still one of the key challenges for their application in commercial battery although these materials possess the advantages of high specific capacity and low co...The voltage decay of lithium-rich layered oxides(LLOs)is still one of the key challenges for their application in commercial battery although these materials possess the advantages of high specific capacity and low cost.In this work,the relationship between voltage decay and tap density of LLOs has been focused.The voltage decay can be significantly suppressed with the increasing tap density as well as the homogenization of the primary or secondary particle size of agglomerated spherical LLOs.Experimental results have shown that an extreme small voltage decay of 0.98 m V cycle^(-1)can be obtained through adjusting the tap density of agglomerated spherical LLOs to 1.99 g cm^(-3),in which the size of primary and secondary particles are uniform.Our work offers a new insight towards the voltage decay and capacity fading of LLOs through precursor preparation process,promoting their application in the real battery in the future.展开更多
Al_(4)B_(2)O_(9) whiskers on the surface of porous SiC substrates were fabricated by chemical reactions between Al(NO_(3))_(3) and H_(3)BO_(3),which is a facile method to prepare cilia-like microstructure for gas-soli...Al_(4)B_(2)O_(9) whiskers on the surface of porous SiC substrates were fabricated by chemical reactions between Al(NO_(3))_(3) and H_(3)BO_(3),which is a facile method to prepare cilia-like microstructure for gas-solid separation.Scanning electron microscopy(SEM),X-ray diffraction(XRD),and Fourier transform infrared(FTIR)spectroscopy were employed to investigate the structural morphology and phase compositions.Al_(4)B_(2)O_(9) whiskers with nanometer-sized diameters and micrometer-sized lengths grew on the surface of SiC substrates,and a self-catalytic mechanism was used to explain Al_(4)B_(2)O_(9) whisker growth.展开更多
Redox mediators(RMs),serving as intermediate electron carriers or reservoirs,play vital roles in developing new charge transfer energy storage systems with high voltage or capacity in aqueous batteries.However,the und...Redox mediators(RMs),serving as intermediate electron carriers or reservoirs,play vital roles in developing new charge transfer energy storage systems with high voltage or capacity in aqueous batteries.However,the underlying mechanism and selection criteria of RMs remain unclear in aqueous batteries,which hinders the further exploitation of new RMs and aqueous battery chemistries.展开更多
Lithium-ion batteries(LIBs)are considered to be indispensable in modern society.Major advances in LIBs depend on the development of new high-performance electrode materials,which requires a fundamental understanding o...Lithium-ion batteries(LIBs)are considered to be indispensable in modern society.Major advances in LIBs depend on the development of new high-performance electrode materials,which requires a fundamental understanding of their properties.First-principles calculations have become a powerful technique in developing new electrode materials for high-energy–den-sity LIBs in terms of predicting and interpreting the characteristics and behaviors of electrode materials,understanding the charge/discharge mechanisms at the atomic scale,delivering rational design strategies for electrode materials,etc.In this review,we present an overview of first-principles calculation methods and highlight their valuable role in contemporary research on LIB cathode materials.This overview focuses on three LIB cathode scenarios,which are divided by their cati-onic/anionic redox mechanisms.Then,representative examples of rational cathode design based on theoretical predictions are presented.Finally,we present a personal perspective on the current challenges and future directions of first-principles calculations in LIBs.展开更多
The conventional method for determining growth kinetics of microbial consortia relies on the total biomass concentration.This may be inaccurate for substrates that are uncommon in nature and can only be degraded by a ...The conventional method for determining growth kinetics of microbial consortia relies on the total biomass concentration.This may be inaccurate for substrates that are uncommon in nature and can only be degraded by a small portion of the microbial community.1,4-dioxane,an emerging contaminant,is an example of such substrates.In this work,we evaluated an improved method for determining the growth kinetics of a 1,4-dioxane-degrading microbial consortium.In the improved method,we considered only bacterial taxa whose concentration increase correlated to 1,4-dioxane concentration decrease in duplicate microcosm tests.Using PEST(Parameter Estimation),a modelindependent parameter estimator,the kinetic constants were estimated by fitting the Monod kineticsbased simulation results to the experimental data that consisted of the concentrations of 1,4-dioxane and the considered bacterial taxa.The estimated kinetic constants were evaluated by comparing the simulation results with experimental results from another set of microcosm tests.The evaluation was quantified by the sum of squared relative residual,which was four orders of magnitude lower for the improved method than the conventional method.By further dividing the considered bacterial taxa into oligotrophs and copiotrophs,the sum of squared relative residual further decreased.展开更多
基金Natural Science Foundation of Shanghai,Grant/Award Number:22ZR1403600Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20180002+1 种基金National Natural Science Foundation of China,Grant/Award Numbers:22109029,51772197,51872192,52025028,52172219Natural Science Foundation of the Jiangsu Higher Education Institutions of China,Grant/Award Number:19KJA170001。
文摘The development of highly safe and low-cost aqueous batteries is of great significance in the background of carbon neutrality.However,the practical deployment of aqueous batteries has been plagued due to their relatively low capacity and poor cycling stability.Herein,we propose unique conversion electrochemistry of copper selenides for robust and energetic aqueous charge storage.In situ X-ray diffraction and operando Raman techniques reveal a reversible transformation from CuSe to Cu_(2)Se through the intermediates of Cu_(3)Se_(2) and Cu_(1.8)Se.Such a conversion process activates the redox carrier of Cu^(2+)ion and delivers a remarkable rate capability of 285 mAh g^(-1) at 20 A g^(-1) and electrochemical durability up to 30,000 cycles.Furthermore,Cu^(2+)and H+coinsertion chemistry is proposed to facilitate the conversion process.As a proof-of-concept,a hybrid aqueous pouch cell coupling CuSe//Zn is capable of affording maximum energy and power densities of 190 Wh kg^(-1) and 1366W kg^(-1),respectively.
基金financially supported by the National Key R&D Program of China (2022YFB2404400)the National Natural Science Foundation of China (92263206,and 22002004)“The Youth Beijing Scholars program” (PXM2021_014204_000023)。
文摘LiMn_(6) hexatomic-rings act as functional units in Li-rich layered oxides(LLOs),which determine the capacity,voltage,and structural stability of LLOs.However,the symmetry of the LiMn_(6) hexatomic-ring is always broken,especially in the grain surface of LLOs,which will greatly affect its electrochemical performance.Herein,the symmetry-breaking of LiMn_(6) hexatomic-ring in the grain surface of Li_(2)MnO_(3) was studied,and their effect on charge compensation mechanism and structure evolution behavior was thoroughly investigated.The results show that the electrochemical activity of the symmetry-broken LiMn_(6) hexatomic-ring is higher than that of the unbroken LiMn_(6),and the former is more favorable for spinelization on the grain surface.Furthermore,the exposure proportion of crystallographic planes with different symmetry-broken LiMn_(6) hexatomic-ring has also been discussed,which can be adjusted by changing the partial pressure of oxygen.The in-depth understanding of the symmetry-breaking of LiMn_(6) hexatomic-ring will provide more targeted strategies for designing high-performance LLOs cathodes for lithium-ion batteries.
基金financial support from the National Natural Science Foundation of China(21878192,51502180)the Fundamental Research Funds for the Central Universities(2016SCU04A18)+1 种基金the 1000 Talents Program of Sichuan Province,the Sichuan Province Science and Technology Support Program(2014GZ0093)the Australian Research Council(DP160102627).
文摘Despite the significant progress in the fabrication of advanced electrode materials,complex control strategies and tedious processing are often involved for most targeted materials to tailor their compositions,morphologies,and chemistries.Inspired by the unique geometric structures of natural biomacromolecules together with their high affinities for metal species,we propose the use of skin collagen fibers for the template crafting of a novel multicore-shell Fe2N-carbon framework anode configuration,composed of hierarchical N-doped carbon nanofiber bundles firmly embedded with Fe2N nanoparticles(Fe2N@N-CFBs).In the resultant heterostructure,the Fe2N nanoparticles firmly confined inside the carbon shells are spatially isolated but electronically well connected by the long-range carbon nanofiber framework.This not only provides direct and continuous conductive pathways to facilitate electron/ion transport,but also helps cushion the volume expansion of the encapsulated Fe2N to preserve the electrode microstructure.Considering its unique structural characteristics,Fe2N@N-CFBs as an advanced anode material exhibits remarkable electrochemical performances for lithium-and potassium-ion batteries.Moreover,this bio-derived structural strategy can pave the way for novel low-cost and high-efficiency syntheses of metal-nitride/carbon nanofiber heterostructures for potential applications in energy-related fields and beyond.
基金financial support from the National Key Research and Development Program of China(2018YFB0104201).
文摘Boosting the utilization efficiency of sulfur electrodes and suppressing the“shuttle effect”of intermediate polysulfides remain the critical challenge for high-performance lithium-sulfur batteries(LSBs).However,most of reported sulfur electrodes are not competent to realize the fast conversion of polysulfides into insoluble lithium sulfides when applied with high sulfur loading,as well as to mitigate the more serious shuttle effect of polysulfides,especially when worked at an elevated temperature.Herein,we reported a unique structural engineering strategy of crafting a unique hierarchical multifunctional electrode architecture constructed by rooting MOF-derived CoS2/carbon nanoleaf arrays(CoS2-CNA)into a nitrogen-rich 3D conductive scaffold(CTNF@CoS2-CNA)for LSBs.An accelerated electrocatalytic effect and improved polysulfide redox kinetics arising from CoS2-CNA were investigated.Besides,the strong capillarity effect and chemisorption of CTNF@CoS2-CNA to polysulfides enable high loading and efficient utilization of sulfur,thus leading to high-performance LIBs performed not only at room temperature but also up to an elevated temperature(55°C).Even with the ultrahigh sulfur loading of 7.19 mg cm?2,the CTNF@CoS2-CNA/S cathode still exhibits high rate capacity at 55°C.
基金supported by the Specialized Research Fund for the Doctoral Program of Yan’an University(YDBK2017-26)the Natural Science Basic Research Plan in Shaanxi Province of China(2018JQ4047)the Young Talent fund of University Association for Science and Technology in Shaanxi,China(20170704)
文摘A decomposition experiment of Populus purdomii litter,a commonly used afforestation species in the Qinling Mountains,China,was conducted.Water extracts of five conifer litters were used to treat P.purdomii litter and its soil.The P.purdomii litter was incubated at room temperature(20–25℃)and constant soil moisture for 6 months.During the decomposition period,the dynamics of litter mass and nutrient contents were detected to investigate the impacts of plant secondary metabolites.The results indicate that litter extracts of Pinus tabuliformis,Platycladus orientalis,Pinus armandii and Larix principisrupprechtii significantly inhibited the overall nutrient release of P.purdomii litter,while the last three types of litter extracts simultaneously inhibited its decomposition.Conversely,the litter extracts of Picea asperata significantly accelerated the overall nutrient release of P.purdomii.Generally,most of the conifer species,whose litter released terpenoids,phenolics,steroids,and aliphatic acids,will inhibit the decomposition and/or nutrient release from P.purdomii litter.Their negative effects on the decomposers and soil enzymatic activities indicates that planting diversity should be lower when mixed planted with P.purdomii.
文摘With the rapid rise of China’s economy and the deployment of the Belt and Road Initiative,traditional Chinese medicine(TCM),one of the main components of Chinese culture,has become an important aspect of foreign exchange.Therefore,recent research has focused on how to effectively spread TCM culture internationally and improve TCM acceptance.Australia is currently a representative region with decent TCM development.Taking TCM development in Australia as a starting point,this article analyzes the challenges in TCM development,discusses countermeasures to address these issues,and provides recommendations for improving the international development and dissemination of TCM.
基金by the National Key Research&Development Program of China(2018YFB0104200)the National Natural Science Foundation of China(201878192 and 51904193).
文摘SeS_(2) has become a promising cathode material owing to its enhanced electrical conductivity over sulfur and higher theoretical specific capacity than selenium;however,the working Li-SeS_(2) batteries have to face the practical challenges from the severe shuttling of soluble dual intermediates of polysulfide and polyselenide,especially in high-SeS_(2)-loading cathodes.Herein,a natural organic polymer,Nicandra physaloides pectin(NPP),is proposed to serve as an effective polysulfide/polyselenide captor to address the shuttling issues.Informed by theoretical calculations,NPP is competent to provide a Lewis base-based strong binding interaction with polysulfides/polyselenides via forming lithium bonds,and it can be homogeneously deposited onto a three-dimensional double-carbon conductive scaffold to finally constitute a polysulfide/polyselenide-immobilizing interlayer.Operando spectroscopy analysis validates the enhanced polysulfide/polyselenide trapping and high conversion efficiency on the constructed interlayer,hence bestowing the Li-SeS_(2) cells with ultrahigh rate capability(448 mAh g^(−1)at 10 A g^(−1)),durable cycling lifespan(≈0.037%capacity attenuation rate per cycle),and high areal capacity(>6.5 mAh cm^(−2))at high SeS_(2) loading of 15.4 mg cm^(−2).Importantly,pouch cells assembled with this interlayer exhibit excellent flexibility,decent rate capability with relatively low electrolyte-to-capacity ratio,and stable cycling life even under a low electrolyte condition,promising a low-cost,viable design protocol toward practical Li-SeS_(2) batteries.
基金financially supported by the National Key R&D Program of China(2022YFB2404400)the National Natural Science Foundation of China(92263206,21875007,21975006,21974007,and U19A2018)+1 种基金the Youth Beijing Scholars program(PXM2021_014204_000023)the Beijing Natural Science Foundation(2222001 and KZ202010005007)。
文摘The rapid expansion of renewable energies asks for great progress of energy-storage technologies for sustainable energy supplies,which raises the compelling demand of high-performance rechargeable batteries.To satisfy the huge demand from the coming energy-storage market,the resource and cost-effectiveness of rechargeable batteries become more and more important.Manganese(Mn)as a key transition element with advantages including high abundance,low cost,and low toxicity derives various kinds(spinels,layered oxides,polyanions,Prussian blue analogs,etc.)of high-performance Mn-based electrode materials,especially cathodes,for rechargeable batteries ranging from Li-ion batteries,Na-ion batteries,aqueous batteries,to multivalent metal-ion batteries.It is anticipated that Mn-based materials with Mn as the major transition-metal element will constitute a flourishing family of Mn-based rechargeable batteries(Mn RBs)for large-scale and differentiated energy-storage applications.On the other hand,several critical issues including Jahn-Teller effect,Mn dissolution,and O release greatly hinder the pace of Mn RBs,which require extensive material optimizations and battery/system improvements.This review aims to provide an investigation about Mn-based materials and batteries for the coming energy-storage demands,with compelling issues and challenges that must be overcome.
基金financial support from the National Natural Science Foundation of China(No.21878192)the Fundamental Research Funds for the Central Universities(No.2016SCU04A18)the 1000 Talents Program of Sichuan Province,and the Sichuan Province Science and Technology Support Program(No.2019YFG0221)。
文摘Pyrochlore-structured polyantimonic acid(PAA)is a potential high-capacity electrode material,but its innately poor electroconductivity(~10^(-10)S/cm)seriously impairs its electrochemical reversibility for lithium-ion storage.Herein,we report design and synthesis of a novel V-substituted PAA(PAA-V),where V^(5+)are introduced to partially replace Sb^(5+).Owing to identical valence and close ionic radius relative to Sb^(5+),the V^(5+)cation can constitute the covalent VO_6octahedra framework without changing the pyrochlore crystal structure of PAA.As a result,the V^(5+)-substitution is capable to modulate the electronic structure of PAA with significantly improved electrical conductivity(~10^(-6)S/cm for PAA-V)and meanwhile decreases the size of crystals with reduced diffusion length for Li^(+)-ions.With varying the ratio of V^(5+)-substitution,the PAA-V with optimized substitution molar ratio(18%)exhibits the best lithium-ion storage performance,delivering a long cycling life with high reversible capacity(731 m Ah/g after 1200cycles at 1 A/g)and outstanding rate capability(279 mAh/g at 15 A/g).More importantly,by pairing the PAA-V as anode and commercial LiFePO_(4)as cathode,the full cell with a limited negative/positive capacity ratio of 1.2 exhibits decent cycling stability at 1 C after 150 cycles with 85.5%capacity retention.
基金supported by the National Natural Science Foundation of China(81972276,31771540,82173040,91740205,and 31620103911)Natural Science Foundation of Zhejiang Province(LYY19H310011)Fundamental Research Funds for the Central Universities(2021QNA7004)。
文摘Gastric cancer(GC)is the fifth most common cancer and the third leading cause of cancer-related death worldwide[1],Metastasis is the leading cause of GC mortality.The complex dynamic interactions between tumor cells and stromal cells in the tumor microenvironment are crucial for tumor metastasis.Many secreted cytokines have been well documented to mediate the crosstalk between tumor cells and stromal cells in a paracrine manner[2].However,how the juxtacrine signals transduced by adjacent cellcell adhesion modulate cancer metastasis has yet to be elucidated[3].As one of the most important cell-cell adhesion molecules,the classical cadherin superfamily also initiates different intracellular signaling cascades and regulates cytoskeletal dynamics,permeability,cell polarity,and tumor progression[4,5].
基金financially supported by the Beijing Natural Science Foundation(JQ19003)National Key R&D Program of China(grant no.2018YFB0104300)+4 种基金National Natural Science Foundation of China(grant no 51622202,21603009,and 21875007)Beijing Natural Science Foundation(B)(KZ201910005002)Beijing Natural Science Foundation(L182009)Project of Youth Talent Plan of Beijing Municipal Education Commission(CIT&TCD201804013)High-grade discipline construction of Beijing(PXM2019-014204-500031)。
文摘The voltage decay of lithium-rich layered oxides(LLOs)is still one of the key challenges for their application in commercial battery although these materials possess the advantages of high specific capacity and low cost.In this work,the relationship between voltage decay and tap density of LLOs has been focused.The voltage decay can be significantly suppressed with the increasing tap density as well as the homogenization of the primary or secondary particle size of agglomerated spherical LLOs.Experimental results have shown that an extreme small voltage decay of 0.98 m V cycle^(-1)can be obtained through adjusting the tap density of agglomerated spherical LLOs to 1.99 g cm^(-3),in which the size of primary and secondary particles are uniform.Our work offers a new insight towards the voltage decay and capacity fading of LLOs through precursor preparation process,promoting their application in the real battery in the future.
基金financially supported by the Shaanxi Provincial Science and Technology Co-ordinating Innovation Projects(2012KTZB03-01-04)the Fundamental Research Funds for the Central Universities(2013G1291068).
文摘Al_(4)B_(2)O_(9) whiskers on the surface of porous SiC substrates were fabricated by chemical reactions between Al(NO_(3))_(3) and H_(3)BO_(3),which is a facile method to prepare cilia-like microstructure for gas-solid separation.Scanning electron microscopy(SEM),X-ray diffraction(XRD),and Fourier transform infrared(FTIR)spectroscopy were employed to investigate the structural morphology and phase compositions.Al_(4)B_(2)O_(9) whiskers with nanometer-sized diameters and micrometer-sized lengths grew on the surface of SiC substrates,and a self-catalytic mechanism was used to explain Al_(4)B_(2)O_(9) whisker growth.
基金supported by the National Key R&D Program of China(grant nos.2018YFA0209401 and 2018YFE0201701)National Natural Science Foundation of China(NSFC grant no.22109029)+1 种基金Natural Science Foundation of Shanghai(grant no.22ZR1403600)Fudan University(grant nos.JIH2203010 and IDH2203008/003).
文摘Redox mediators(RMs),serving as intermediate electron carriers or reservoirs,play vital roles in developing new charge transfer energy storage systems with high voltage or capacity in aqueous batteries.However,the underlying mechanism and selection criteria of RMs remain unclear in aqueous batteries,which hinders the further exploitation of new RMs and aqueous battery chemistries.
基金supported by the Beijing Natural Science Foundation(JQ19003,KZ202010005007 KZ201910005002)the National Natural Science Foundation of China(U19A2018,21875007,51802009 and 22075007).
文摘Lithium-ion batteries(LIBs)are considered to be indispensable in modern society.Major advances in LIBs depend on the development of new high-performance electrode materials,which requires a fundamental understanding of their properties.First-principles calculations have become a powerful technique in developing new electrode materials for high-energy–den-sity LIBs in terms of predicting and interpreting the characteristics and behaviors of electrode materials,understanding the charge/discharge mechanisms at the atomic scale,delivering rational design strategies for electrode materials,etc.In this review,we present an overview of first-principles calculation methods and highlight their valuable role in contemporary research on LIB cathode materials.This overview focuses on three LIB cathode scenarios,which are divided by their cati-onic/anionic redox mechanisms.Then,representative examples of rational cathode design based on theoretical predictions are presented.Finally,we present a personal perspective on the current challenges and future directions of first-principles calculations in LIBs.
基金supported by Geosyntec Consultants through contract RF02700.
文摘The conventional method for determining growth kinetics of microbial consortia relies on the total biomass concentration.This may be inaccurate for substrates that are uncommon in nature and can only be degraded by a small portion of the microbial community.1,4-dioxane,an emerging contaminant,is an example of such substrates.In this work,we evaluated an improved method for determining the growth kinetics of a 1,4-dioxane-degrading microbial consortium.In the improved method,we considered only bacterial taxa whose concentration increase correlated to 1,4-dioxane concentration decrease in duplicate microcosm tests.Using PEST(Parameter Estimation),a modelindependent parameter estimator,the kinetic constants were estimated by fitting the Monod kineticsbased simulation results to the experimental data that consisted of the concentrations of 1,4-dioxane and the considered bacterial taxa.The estimated kinetic constants were evaluated by comparing the simulation results with experimental results from another set of microcosm tests.The evaluation was quantified by the sum of squared relative residual,which was four orders of magnitude lower for the improved method than the conventional method.By further dividing the considered bacterial taxa into oligotrophs and copiotrophs,the sum of squared relative residual further decreased.