All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lit...All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.展开更多
Nanofluidic hydrogel membranes have shown great potential for osmotic energy harvesting(OEH)due to their unique properties.These membranes are made of hydrogels that contain embedded nanofluidic channels,which provide...Nanofluidic hydrogel membranes have shown great potential for osmotic energy harvesting(OEH)due to their unique properties.These membranes are made of hydrogels that contain embedded nanofluidic channels,which provide high selectivity for ions and molecules,making them ideal for osmotic processes.This review explores how to harness the osmotic pressure difference between two solutions separated by the membrane to generate sustainable energy.The review compares the materials membranes and the key advantages of nanofluidic hydrogel membranes:flexibility and ion-transport properties for high power density for OEH,It highlights the size and distribution of the nanofluidic channels within the hydrogel matrix that can be adjusted to optimize ion transport and energy generation efficiency.This flexibility enables customization based on specific requirements for osmotic energy harvesting.This review discusses advancing the transition to sustainable energy sources,challenges,and prospectus for developing and using nanofluidic hydrogel membranes,which hold significant potential for enhancing energy and environmental sustainability.展开更多
Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cath...Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cathode materials influence the cost and energy output of SIBs.Therefore,the development of advanced cathode materials is crucial for the practical application of SIBs.Among various cathode materials,layered transition metal oxides(LTMOs)have received widespread attention owing to their straightforward preparation,abundant availability,and cost-competitiveness.Notably,layered Fe-based oxide cathodes are deemed to be one of the most promising candidates for the lowest price and easy-to-improve performance.Nevertheless,the challenges such as severe phase transitions,sluggish diffusion kinetics and interfacial degradation pose significant hurdles in achieving high-performance cathodes for SIBs.This review first briefly outlines the classification of layered structures and the working principle of layered oxides.Then,recent advances in modification strategies employed to address current issues with layered iron-based oxide cathodes are systematically reviewed,including ion doping,biphasic engineering and surface modification.Furthermore,the review not only outlines the prospects and development directions for layered Fe-based oxide cathodes but also provides novel insights and directions for future research endeavors for SIBs.展开更多
动脉粥样硬化作为心脑血管疾病的核心病理基础,在我国的发病率呈持续攀升态势,构成了巨大的公共卫生负担。中医学理论认为,“脾气散精”是调控水谷精微化生、转运与输布的关键环节。脾不散精,则膏脂转运障碍,内生痰浊,积聚血脉,化为斑块...动脉粥样硬化作为心脑血管疾病的核心病理基础,在我国的发病率呈持续攀升态势,构成了巨大的公共卫生负担。中医学理论认为,“脾气散精”是调控水谷精微化生、转运与输布的关键环节。脾不散精,则膏脂转运障碍,内生痰浊,积聚血脉,化为斑块,此乃动脉粥样硬化发生与发展的重要中医病机。本研究立足于“脾气散精”理论,以脾虚痰浊这一动脉粥样硬化关键病因为切入点,旨在将动脉粥样硬化防治研究重心前移。课题组前期研究发现,健脾祛痰方能有效减少主动脉管腔粥样斑块面积,延缓脂肪异常沉积,抑制血管周围脂肪组织细胞内脂滴形成,并显著促进白色脂肪向棕色脂肪转化(即白色脂肪棕色化)。分子机制研究表明,该方能上调解偶联蛋白1(Uncoupling Protein 1,UCP1)、线粒体动力相关蛋白1(Dynamin-related Protein 1,DRP1)及线粒体三磷酸腺苷(Adenosine Triphosphate,ATP)依赖的LON蛋白酶1(Lon Protease 1,LONP1)的表达水平。线粒体动力学通过裂变与融合维持网络稳态,直接调控UCP1转录,驱动脂肪细胞产热代谢。LONP1是线粒体基质核心蛋白酶。最新研究发现,LONP1可调控心肌细胞线粒体裂变-融合动态变化。另有研究表明,LONP1在白色脂肪棕色化中起重要作用。因此,本研究从LONP1介导线粒体动力学角度探讨其调控白色脂肪棕色化治疗动脉粥样硬化的作用机制,丰富“脾气散精”理论的科学内涵,为中医药防治动脉粥样硬化的治疗策略提供科学依据。展开更多
The rapid growth in global energy demand has necessitated the development of efficient energy storage and conversion devices,with the aim of enhancing grid stability,promoting the adoption of electric vehicles,and pow...The rapid growth in global energy demand has necessitated the development of efficient energy storage and conversion devices,with the aim of enhancing grid stability,promoting the adoption of electric vehicles,and powering portable electronics.However,the performance of these devices is constrained by the limitations of traditional electrode materials and catalysts.Bimetallic tellurides have emerged as a promising solution due to their exceptional synergistic effects,high electronic conductivity,abundant redox-active sites,and outstanding electrochemical stability.Nevertheless,achieving cost-effective synthesis and stable applications remains a significant challenge.Hence,the most recent advances of bimetallic tellurides electrodes from synthesis to application are systematically reviewed.Several synthetic strategies for exquisite bimetallic tellurides nanostructures,including tellurization,ball-milling,solvo/hydrothermal,electrodeposition,wet chemical,and template method,are discussed.Moreover,the applications of bimetallic tellurides are extensively summarized in energy storage and conversion devices,which include alkali metal-ion batteries(Li-ion,Na-ion,and K-ion),supercapacitor,hydrogen evolution reaction(HER),and oxygen evolution reaction(OER).Besides,the challenges and potential solutions of bimetallic telluride for energy applications are also suggested.This work provides fundamental insight and guidelines for the future design of bimetallic tellurides in energy storage and conversion technologies.展开更多
A novel method for scandium recovery is proposed through high-surface area silanol-rich silica sorbents which were prepared with calcium silicate hydrate(C-S-H) as raw material.Two types of silanol-rich silica particl...A novel method for scandium recovery is proposed through high-surface area silanol-rich silica sorbents which were prepared with calcium silicate hydrate(C-S-H) as raw material.Two types of silanol-rich silica particles,i.e.,LAC-S(silica derived from acid leaching of amorphous C-S-H) and LLC-S(silica derived from acid leaching of low-crystallinity C-S-H) are obtained after calcium ions are removed from both amorphous and low-crystallinity forms of C-S-H through a facile acid leaching process(3 mol/L,25℃,24 h).(29)^Si NMR spectroscopy reveals that the proportion of silicon atoms carrying silanol groups increases from less than 43% to over 80% when silica particles are transferred from a dry state to an aqueous solution.Batch adsorption experiments were conducted to evaluate the sorption performance and selectivity of these silica sorbents toward Sc(Ⅲ).The scandium sorption capacities of LAC-S and LLC-S at an equilibrium pH of 4.2 are 174.45 and 129.57 mg/g,respectively.The separation factors(SFSc/Ln) of both silica particles exceed 1000 in the initial pH range of 3.5-5.The loaded scandium ions are recovered with 3 mol/L hydrochloric acid and the sorbents exhibit good reusability.This strategy provides an efficient and green method for recovering scandium from aqueous solutions.展开更多
Poor Li plating reversibility and high thermal runaway risks are key challenges for fast charging lithiumion batteries with graphite anodes.Herein,a dielectric and fire-resistant separator based on hybrid nanofibers o...Poor Li plating reversibility and high thermal runaway risks are key challenges for fast charging lithiumion batteries with graphite anodes.Herein,a dielectric and fire-resistant separator based on hybrid nanofibers of barium sulfate(BS)and bacterial cellulose(BC)is developed to synchronously enhance the battery's fast charging and thermal-safety performances.The regulation mechanism of the dielectric BS/BC separator in enhancing the Li^(+)ion transport and Li plating reversibility is revealed.(1)The Max-Wagner polarization electric field of the dielectric BS/BC separator can accelerate the desolvation of solvated Li^(+)ions,enhancing their transport kinetics.(2)Moreover,due to the charge balancing effect,the dielectric BS/BC separator homogenizes the electric field/Li^(+)ion flux at the graphite anode-separator interface,facilitating uniform Li plating and suppressing Li dendrite growth.Consequently,the fast-charge graphite anode with the BS/BC separator shows higher Coulombic efficiency(99.0%vs.96.9%)and longer cycling lifespan(100 cycles vs.59 cycles)than that with the polypropylene(PP)separator in the constantlithiation cycling test at 2 mA cm^(-2).The high-loading LiFePO4(15.5 mg cm^(-2))//graphite(7.5 mg cm^(-2))full cell with the BS/BC separator exhibits excellent fast charging performance,retaining 70%of its capacity after 500 cycles at a high rate of 2C,which is significantly better than that of the cell with the PP separator(retaining only 27%of its capacity after 500 cycles).More importantly,the thermally stable BS/BC separator effectively elevates the critical temperature and reduces the heat release rate during thermal runaway,thereby significantly enhancing the battery's safety.展开更多
Single crystal Ni-rich cathode materials(SCNCM)are a good supplement in the market of nickel-based materials due to their safety and excellent electrochemical performance.However,the challenges of cation mixing,phase ...Single crystal Ni-rich cathode materials(SCNCM)are a good supplement in the market of nickel-based materials due to their safety and excellent electrochemical performance.However,the challenges of cation mixing,phase change during charge/discharge,and low thermal stability remain unresolved in single crystal particles.To address these issues,SCNCM are rationally modified by incorporating transition metal(TM)oxides,and the influence of metal ions with different valence states on the electrochemical properties of SCNCM is methodically explored through experimental results and theoretical calculations.Enhanced structural stability is demonstrated in SCNCM after the modifications,and the degree of improvement in the matrix materials varies depending on the valence state of doped TM ions.The highest structural stability is found in WO_(3)-modified SCNCM,due to the smaller effective ion radii,higher electro-negativity,stronger W-O bond,and efficient suppression of oxygen vacancy generation.As a result,WO_(3)-modified SCNCM have outstanding cycle performance,with a capacity retention rate of90.2%after 200 cycles.This study provides an insight into the design of advanced SCNCM with enhanced reversibility and cyclability.展开更多
Enantiomer identification is of paramount industrial value and physiological significance.Construction of sensitive chiral sensors with high enantiomeric discrimination ability is highly desirable.In this work,a chira...Enantiomer identification is of paramount industrial value and physiological significance.Construction of sensitive chiral sensors with high enantiomeric discrimination ability is highly desirable.In this work,a chiral covalent organic framework/anodic aluminum oxide(c-COF/AAO)membrane was prepared for electrochemical enantioselective recognition and sensing.Benefiting from the remarkable asymmetry,the asprepared nanofluidic c-COF/AAO presents a distinct ion current rectification(ICR)characteristic,enabling sensitive bioanalysis.In addition,owing to the large surface area,high chemical stability and perfect ion selectivity of chiral COF,the prepared c-COF/AAO membrane presents exceptionally selective mass transport and thereby enables excellent chiral discrimination for S-/R-Naproxen(S-/R-Npx)enantiomers.It is especially noteworthy that the detection limit is achieved as low as 3.88 pmol/L.These results raise the possibility for a facile,stable and low-cost method to carry out sensitive enantioselective recognition and detection.展开更多
In light of the burgeoning energy technology sector and the ever-growing demand for lithium across diverse industrial domains,conventional lithium extraction methods have been proven inadequate due to their limited pr...In light of the burgeoning energy technology sector and the ever-growing demand for lithium across diverse industrial domains,conventional lithium extraction methods have been proven inadequate due to their limited production capacity and high operational costs.This work introduces a novel approach to the manganese-titanium based composite HMTO(Mn:Ti=1:4)lithium ion-sieve(LIS)nanospheres,employing lithium acetate dihydrate,manganese carbonate and titanium dioxide P25 as the primary materials.These nanospheres exhibit relatively uniform spherical morphology,narrow size distribution,small average particle size(ca.55 nm),large specific surface area(43.58 m^(2)g^(-1))and high surface O_(2)-content(59.01%).When utilized as the adsorbents for Li^(+)ions,the HMTO(Mn:Ti=1:4)LIS demonstrates a fast adsorption rate,approaching equilibrium within 6.0 h with an equilibrium adsorption capacity(qe)of 79.5 mg g^(-1)and a maximum adsorption capacity(qm)of 87.26 mg g^(-1)(initial concentration CO:1.8 g L^(-1)).In addition,the HMTO(Mn:Ti=1:4)also delivers a high lithium extraction from the simulated high magnesium-lithium molar ratio salt lake brine(Mg:Li=103),achieving a qeof 33.85 mg g^(-1)along with a remarkable selectivity(α_(Mg)^(Li)=2192.76).Particularly,the HMTO(Mn:Ti=1:4)LIS showcases a satisfactory recycling adsorption performance.The adsorption capacity remains at a high level,even that determined after the 5th cycle(55.45 mg g^(-1))surpasses that of the most recently reported adsorbents.Ultimately,the fantastic synergistic lithium adsorption mechanism is deliberately uncovered by leveraging the ion exchange principles and molecular dynamics(MD)simulations.展开更多
Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been d...Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn^(2+)diffusion kinetics.By employing electrodeposition to coat MoS_(2)on the surface of BaV_(6)O_(16)·3H_(2)O nanowires,the directional builtin electric field generated at the heterointerface acts as a cation accelerator,continuously accelerating Zn^(2+)diffusion into the active material.The optimized Zn^(2+)diffusion coefficient in CC@BaV-V_(6)O_(16)·3H_(2)@MoS_(2)(7.5×10^(8)cm^(2)s^(-1)) surpasses that of most reported V-based cathodes.Simultaneously,MoS_(2)serving as a cathodic armor extends the cycling life of the Zn-CC@BaV_(6)O_(16)·3H_(2)@MoS_(2)full batteries to over 10000 cycles.This work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.展开更多
Dual atomic catalysts(DAC),particularly copper(Cu_(2))-based nitrogen(N)doped graphene,show great potential to effectively convert CO_(2)and nitrate(NO_(3)-)into important industrial chemicals such as ethylene,glycol,...Dual atomic catalysts(DAC),particularly copper(Cu_(2))-based nitrogen(N)doped graphene,show great potential to effectively convert CO_(2)and nitrate(NO_(3)-)into important industrial chemicals such as ethylene,glycol,acetamide,and urea through an efficient catalytical process that involves C–C and C–N coupling.However,the origin of the coupling activity remained unclear,which substantially hinders the rational design of Cu-based catalysts for the N-integrated CO_(2)reduction reaction(CO_(2)RR).To address this challenge,this work performed advanced density functional theory calculations incorporating explicit solvation based on a Cu_(2)-based N-doped carbon(Cu_(2)N_(6)C_(10))catalyst for CO_(2)RR.These calculations are aimed to gain insight into the reaction mechanisms for the synthesis of ethylene,acetamide,and urea via coupling in the interfacial reaction micro-environment.Due to the sluggishness of CO_(2),the formation of a solvation electric layer by anions(F^(-),Cl^(-),Br^(-),and I^(-))and cations(Na+,Mg^(2+),K+,and Ca^(2+))leads to electron transfer towards the Cu surface.This process significantly accelerates the reduction of CO_(2).These results reveal that*CO intermediates play a pivotal role in N-integrated CO_(2)RR.Remarkably,the Cu_(2)-based N-doped carbon catalyst examined in this study has demonstrated the most potential for C–N coupling to date.Our findings reveal that through the process of a condensation reaction between*CO and NH_(2)OH for urea synthesis,*NO_(3)-is reduced to*NH_(3),and*CO_(2)to*CCO at dual Cu atom sites.This dual-site reduction facilitates the synthesis of acetamide through a nucleophilic reaction between NH_(3)and the ketene intermediate.Furthermore,we found that the I-and Mg^(2+)ions,influenced by pH,were highly effective for acetamide and ammonia synthesis,except when F-and Ca^(2+)were present.Furthermore,the mechanisms of C–N bond formation were investigated via ab-initio molecular dynamics simulations,and we found that adjusting the micro-environment can change the dominant side reaction,shifting from hydrogen production in acidic conditions to water reduction in alkaline ones.This study introduces a novel approach using ion-H_(2)O cages to significantly enhance the efficiency of C–N coupling reactions.展开更多
文摘All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.
基金supported by the Shenzhen Science and Technology Innovation Commission(JCYJ20241202123500002)the Foundation for Special Projects in Key Fields of Guangdong Province Universities(2024ZDZX3031,2023ZDZX3005)+1 种基金the National Natural Science Foundation of China(21702038)the Fundacao para a Ciencia e a Tecnologia(FCT),Portugal,through projects UIDB/00100/2020(DOI:10.54499/UIDB/00100/2020),UIDP/00100/2020(DOI:10.54499/UIDP/00100/2020),and LA/P/0056/2020(DOI:10.54499/LA/P/0056/2020)of Centro de Química Estrutural。
文摘Nanofluidic hydrogel membranes have shown great potential for osmotic energy harvesting(OEH)due to their unique properties.These membranes are made of hydrogels that contain embedded nanofluidic channels,which provide high selectivity for ions and molecules,making them ideal for osmotic processes.This review explores how to harness the osmotic pressure difference between two solutions separated by the membrane to generate sustainable energy.The review compares the materials membranes and the key advantages of nanofluidic hydrogel membranes:flexibility and ion-transport properties for high power density for OEH,It highlights the size and distribution of the nanofluidic channels within the hydrogel matrix that can be adjusted to optimize ion transport and energy generation efficiency.This flexibility enables customization based on specific requirements for osmotic energy harvesting.This review discusses advancing the transition to sustainable energy sources,challenges,and prospectus for developing and using nanofluidic hydrogel membranes,which hold significant potential for enhancing energy and environmental sustainability.
基金supported by the National Natural Science Foundation of China(no.52374301)the Open Project of Guangxi Key Laboratory of Electrochemical Energy Materials(no.GXUEEM2024001)+2 种基金the Hebei Provincial Natural Science Foundation(no.E2024501010)the Shijiazhuang Basic Research Project(no.241790667A)the Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(no.22567627H)。
文摘Sodium-ion batteries(SIBs)have the advantages of environmental friendliness,cost-effectiveness,and high energy density,which are considered one of the most promising candidates for lithium-ion batteries(LIBs).The cathode materials influence the cost and energy output of SIBs.Therefore,the development of advanced cathode materials is crucial for the practical application of SIBs.Among various cathode materials,layered transition metal oxides(LTMOs)have received widespread attention owing to their straightforward preparation,abundant availability,and cost-competitiveness.Notably,layered Fe-based oxide cathodes are deemed to be one of the most promising candidates for the lowest price and easy-to-improve performance.Nevertheless,the challenges such as severe phase transitions,sluggish diffusion kinetics and interfacial degradation pose significant hurdles in achieving high-performance cathodes for SIBs.This review first briefly outlines the classification of layered structures and the working principle of layered oxides.Then,recent advances in modification strategies employed to address current issues with layered iron-based oxide cathodes are systematically reviewed,including ion doping,biphasic engineering and surface modification.Furthermore,the review not only outlines the prospects and development directions for layered Fe-based oxide cathodes but also provides novel insights and directions for future research endeavors for SIBs.
文摘动脉粥样硬化作为心脑血管疾病的核心病理基础,在我国的发病率呈持续攀升态势,构成了巨大的公共卫生负担。中医学理论认为,“脾气散精”是调控水谷精微化生、转运与输布的关键环节。脾不散精,则膏脂转运障碍,内生痰浊,积聚血脉,化为斑块,此乃动脉粥样硬化发生与发展的重要中医病机。本研究立足于“脾气散精”理论,以脾虚痰浊这一动脉粥样硬化关键病因为切入点,旨在将动脉粥样硬化防治研究重心前移。课题组前期研究发现,健脾祛痰方能有效减少主动脉管腔粥样斑块面积,延缓脂肪异常沉积,抑制血管周围脂肪组织细胞内脂滴形成,并显著促进白色脂肪向棕色脂肪转化(即白色脂肪棕色化)。分子机制研究表明,该方能上调解偶联蛋白1(Uncoupling Protein 1,UCP1)、线粒体动力相关蛋白1(Dynamin-related Protein 1,DRP1)及线粒体三磷酸腺苷(Adenosine Triphosphate,ATP)依赖的LON蛋白酶1(Lon Protease 1,LONP1)的表达水平。线粒体动力学通过裂变与融合维持网络稳态,直接调控UCP1转录,驱动脂肪细胞产热代谢。LONP1是线粒体基质核心蛋白酶。最新研究发现,LONP1可调控心肌细胞线粒体裂变-融合动态变化。另有研究表明,LONP1在白色脂肪棕色化中起重要作用。因此,本研究从LONP1介导线粒体动力学角度探讨其调控白色脂肪棕色化治疗动脉粥样硬化的作用机制,丰富“脾气散精”理论的科学内涵,为中医药防治动脉粥样硬化的治疗策略提供科学依据。
基金supported by the Young Elite Scientists Sponsorship Program by CAST(grant No.2022QNRC001)the National Natural Science Foundation of China(No.52474318)+1 种基金the Beijing Nova Program(Z211100002121082)the Interdisciplinary Research Project for Young Teachers of USTB(Fundamental Research Funds for the Central Universities,FRF-IDRY-GD23-005)。
文摘The rapid growth in global energy demand has necessitated the development of efficient energy storage and conversion devices,with the aim of enhancing grid stability,promoting the adoption of electric vehicles,and powering portable electronics.However,the performance of these devices is constrained by the limitations of traditional electrode materials and catalysts.Bimetallic tellurides have emerged as a promising solution due to their exceptional synergistic effects,high electronic conductivity,abundant redox-active sites,and outstanding electrochemical stability.Nevertheless,achieving cost-effective synthesis and stable applications remains a significant challenge.Hence,the most recent advances of bimetallic tellurides electrodes from synthesis to application are systematically reviewed.Several synthetic strategies for exquisite bimetallic tellurides nanostructures,including tellurization,ball-milling,solvo/hydrothermal,electrodeposition,wet chemical,and template method,are discussed.Moreover,the applications of bimetallic tellurides are extensively summarized in energy storage and conversion devices,which include alkali metal-ion batteries(Li-ion,Na-ion,and K-ion),supercapacitor,hydrogen evolution reaction(HER),and oxygen evolution reaction(OER).Besides,the challenges and potential solutions of bimetallic telluride for energy applications are also suggested.This work provides fundamental insight and guidelines for the future design of bimetallic tellurides in energy storage and conversion technologies.
基金Project supported by the National Natural Science Foundation of China (52064002)Guangxi Science and Technology Major Project(AA23073018)。
文摘A novel method for scandium recovery is proposed through high-surface area silanol-rich silica sorbents which were prepared with calcium silicate hydrate(C-S-H) as raw material.Two types of silanol-rich silica particles,i.e.,LAC-S(silica derived from acid leaching of amorphous C-S-H) and LLC-S(silica derived from acid leaching of low-crystallinity C-S-H) are obtained after calcium ions are removed from both amorphous and low-crystallinity forms of C-S-H through a facile acid leaching process(3 mol/L,25℃,24 h).(29)^Si NMR spectroscopy reveals that the proportion of silicon atoms carrying silanol groups increases from less than 43% to over 80% when silica particles are transferred from a dry state to an aqueous solution.Batch adsorption experiments were conducted to evaluate the sorption performance and selectivity of these silica sorbents toward Sc(Ⅲ).The scandium sorption capacities of LAC-S and LLC-S at an equilibrium pH of 4.2 are 174.45 and 129.57 mg/g,respectively.The separation factors(SFSc/Ln) of both silica particles exceed 1000 in the initial pH range of 3.5-5.The loaded scandium ions are recovered with 3 mol/L hydrochloric acid and the sorbents exhibit good reusability.This strategy provides an efficient and green method for recovering scandium from aqueous solutions.
基金financially supported by the National Natural Science Foundation of China(Grant No.52202328,52372099)the Shanghai Sailing Program(22YF1455500).
文摘Poor Li plating reversibility and high thermal runaway risks are key challenges for fast charging lithiumion batteries with graphite anodes.Herein,a dielectric and fire-resistant separator based on hybrid nanofibers of barium sulfate(BS)and bacterial cellulose(BC)is developed to synchronously enhance the battery's fast charging and thermal-safety performances.The regulation mechanism of the dielectric BS/BC separator in enhancing the Li^(+)ion transport and Li plating reversibility is revealed.(1)The Max-Wagner polarization electric field of the dielectric BS/BC separator can accelerate the desolvation of solvated Li^(+)ions,enhancing their transport kinetics.(2)Moreover,due to the charge balancing effect,the dielectric BS/BC separator homogenizes the electric field/Li^(+)ion flux at the graphite anode-separator interface,facilitating uniform Li plating and suppressing Li dendrite growth.Consequently,the fast-charge graphite anode with the BS/BC separator shows higher Coulombic efficiency(99.0%vs.96.9%)and longer cycling lifespan(100 cycles vs.59 cycles)than that with the polypropylene(PP)separator in the constantlithiation cycling test at 2 mA cm^(-2).The high-loading LiFePO4(15.5 mg cm^(-2))//graphite(7.5 mg cm^(-2))full cell with the BS/BC separator exhibits excellent fast charging performance,retaining 70%of its capacity after 500 cycles at a high rate of 2C,which is significantly better than that of the cell with the PP separator(retaining only 27%of its capacity after 500 cycles).More importantly,the thermally stable BS/BC separator effectively elevates the critical temperature and reduces the heat release rate during thermal runaway,thereby significantly enhancing the battery's safety.
基金financially supported by the National Natural Science Foundation of China,China(52004103,51974137,52274229,22350410378 and 52304328)the China Postdoctoral Science Foundation,China(2020M671361 and 2023M733189)+4 种基金the Natural Science Foundation of Jiangsu Province,China(BK20220534)the Jiangsu Postdoctoral Science Foundation,China(2020Z090)the Senior Talents Fund of Jiangsu University,China(5501220014)the Key Research and Development Project of Ningxia Province,China(2024BEE02001)the Open Project of Key Laboratory of Advanced Battery Materials of Yunnan Province,China(KLABM-2024092403).
文摘Single crystal Ni-rich cathode materials(SCNCM)are a good supplement in the market of nickel-based materials due to their safety and excellent electrochemical performance.However,the challenges of cation mixing,phase change during charge/discharge,and low thermal stability remain unresolved in single crystal particles.To address these issues,SCNCM are rationally modified by incorporating transition metal(TM)oxides,and the influence of metal ions with different valence states on the electrochemical properties of SCNCM is methodically explored through experimental results and theoretical calculations.Enhanced structural stability is demonstrated in SCNCM after the modifications,and the degree of improvement in the matrix materials varies depending on the valence state of doped TM ions.The highest structural stability is found in WO_(3)-modified SCNCM,due to the smaller effective ion radii,higher electro-negativity,stronger W-O bond,and efficient suppression of oxygen vacancy generation.As a result,WO_(3)-modified SCNCM have outstanding cycle performance,with a capacity retention rate of90.2%after 200 cycles.This study provides an insight into the design of advanced SCNCM with enhanced reversibility and cyclability.
基金supported by grants from the National Natural Science Foundation of China(Nos.22274076,22304084)the Primary Research&Development Plan of Jiangsu Province(No.BE2022793)+1 种基金the Natural Science Foundation of Jiangsu Province of China(No.BK20230377)Jiangsu Provincial Department of Education(No.211090B52303)。
文摘Enantiomer identification is of paramount industrial value and physiological significance.Construction of sensitive chiral sensors with high enantiomeric discrimination ability is highly desirable.In this work,a chiral covalent organic framework/anodic aluminum oxide(c-COF/AAO)membrane was prepared for electrochemical enantioselective recognition and sensing.Benefiting from the remarkable asymmetry,the asprepared nanofluidic c-COF/AAO presents a distinct ion current rectification(ICR)characteristic,enabling sensitive bioanalysis.In addition,owing to the large surface area,high chemical stability and perfect ion selectivity of chiral COF,the prepared c-COF/AAO membrane presents exceptionally selective mass transport and thereby enables excellent chiral discrimination for S-/R-Naproxen(S-/R-Npx)enantiomers.It is especially noteworthy that the detection limit is achieved as low as 3.88 pmol/L.These results raise the possibility for a facile,stable and low-cost method to carry out sensitive enantioselective recognition and detection.
基金supported by the National Natural Science Foundation of China(22075304,22378390)Natural Science Foundation of Shandong Province,China(ZR2022MB075)+2 种基金State Key Laboratory of Organic-Inorganic Composites(oic-202401016)State Key Laboratory of Chemical Engineering(SKL-ChE-24A02)Beijing Natural Science Foundation,China(3222050).
文摘In light of the burgeoning energy technology sector and the ever-growing demand for lithium across diverse industrial domains,conventional lithium extraction methods have been proven inadequate due to their limited production capacity and high operational costs.This work introduces a novel approach to the manganese-titanium based composite HMTO(Mn:Ti=1:4)lithium ion-sieve(LIS)nanospheres,employing lithium acetate dihydrate,manganese carbonate and titanium dioxide P25 as the primary materials.These nanospheres exhibit relatively uniform spherical morphology,narrow size distribution,small average particle size(ca.55 nm),large specific surface area(43.58 m^(2)g^(-1))and high surface O_(2)-content(59.01%).When utilized as the adsorbents for Li^(+)ions,the HMTO(Mn:Ti=1:4)LIS demonstrates a fast adsorption rate,approaching equilibrium within 6.0 h with an equilibrium adsorption capacity(qe)of 79.5 mg g^(-1)and a maximum adsorption capacity(qm)of 87.26 mg g^(-1)(initial concentration CO:1.8 g L^(-1)).In addition,the HMTO(Mn:Ti=1:4)also delivers a high lithium extraction from the simulated high magnesium-lithium molar ratio salt lake brine(Mg:Li=103),achieving a qeof 33.85 mg g^(-1)along with a remarkable selectivity(α_(Mg)^(Li)=2192.76).Particularly,the HMTO(Mn:Ti=1:4)LIS showcases a satisfactory recycling adsorption performance.The adsorption capacity remains at a high level,even that determined after the 5th cycle(55.45 mg g^(-1))surpasses that of the most recently reported adsorbents.Ultimately,the fantastic synergistic lithium adsorption mechanism is deliberately uncovered by leveraging the ion exchange principles and molecular dynamics(MD)simulations.
基金National Natural Science Foundation of China (61761047 and 41876055)Program for Innovative Research Team (in Science and Technology) in University of Yunnan Province。
文摘Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn^(2+)diffusion kinetics.By employing electrodeposition to coat MoS_(2)on the surface of BaV_(6)O_(16)·3H_(2)O nanowires,the directional builtin electric field generated at the heterointerface acts as a cation accelerator,continuously accelerating Zn^(2+)diffusion into the active material.The optimized Zn^(2+)diffusion coefficient in CC@BaV-V_(6)O_(16)·3H_(2)@MoS_(2)(7.5×10^(8)cm^(2)s^(-1)) surpasses that of most reported V-based cathodes.Simultaneously,MoS_(2)serving as a cathodic armor extends the cycling life of the Zn-CC@BaV_(6)O_(16)·3H_(2)@MoS_(2)full batteries to over 10000 cycles.This work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.
基金National Natural Science Foundation of China(U22B20149,22308376)Outstanding Young Scholars Foundation of China University of Petroleum(Beijing)(2462023BJRC015)Foundation of United Institute for Carbon Neutrality(CNIF20230209)。
文摘Dual atomic catalysts(DAC),particularly copper(Cu_(2))-based nitrogen(N)doped graphene,show great potential to effectively convert CO_(2)and nitrate(NO_(3)-)into important industrial chemicals such as ethylene,glycol,acetamide,and urea through an efficient catalytical process that involves C–C and C–N coupling.However,the origin of the coupling activity remained unclear,which substantially hinders the rational design of Cu-based catalysts for the N-integrated CO_(2)reduction reaction(CO_(2)RR).To address this challenge,this work performed advanced density functional theory calculations incorporating explicit solvation based on a Cu_(2)-based N-doped carbon(Cu_(2)N_(6)C_(10))catalyst for CO_(2)RR.These calculations are aimed to gain insight into the reaction mechanisms for the synthesis of ethylene,acetamide,and urea via coupling in the interfacial reaction micro-environment.Due to the sluggishness of CO_(2),the formation of a solvation electric layer by anions(F^(-),Cl^(-),Br^(-),and I^(-))and cations(Na+,Mg^(2+),K+,and Ca^(2+))leads to electron transfer towards the Cu surface.This process significantly accelerates the reduction of CO_(2).These results reveal that*CO intermediates play a pivotal role in N-integrated CO_(2)RR.Remarkably,the Cu_(2)-based N-doped carbon catalyst examined in this study has demonstrated the most potential for C–N coupling to date.Our findings reveal that through the process of a condensation reaction between*CO and NH_(2)OH for urea synthesis,*NO_(3)-is reduced to*NH_(3),and*CO_(2)to*CCO at dual Cu atom sites.This dual-site reduction facilitates the synthesis of acetamide through a nucleophilic reaction between NH_(3)and the ketene intermediate.Furthermore,we found that the I-and Mg^(2+)ions,influenced by pH,were highly effective for acetamide and ammonia synthesis,except when F-and Ca^(2+)were present.Furthermore,the mechanisms of C–N bond formation were investigated via ab-initio molecular dynamics simulations,and we found that adjusting the micro-environment can change the dominant side reaction,shifting from hydrogen production in acidic conditions to water reduction in alkaline ones.This study introduces a novel approach using ion-H_(2)O cages to significantly enhance the efficiency of C–N coupling reactions.
