lonic liquids with stimuli-responsive characteristics are an essential branch in the comprehensive ionic liquids'family,which can meet the controllable and reversible needs in practical applications with different...lonic liquids with stimuli-responsive characteristics are an essential branch in the comprehensive ionic liquids'family,which can meet the controllable and reversible needs in practical applications with different stimulation means.In this review,we summarize the recent research progress of these stimuli-responsive ionic liquids,mainly focusing on their chemical structures,properties,responsive mechanism,aggregation structures,and phase behaviors,which were driven by external stimuli,such as CO2,magnetism,light,temperature,redox,and pH.Then,the particular or potential applications of stimuli-responsive ionic liquids are expounded in various fields of science,including catalytic reaction,extraction,separation,nano-material preparation,and gas absorption.In the end,the challenges and strategies of the subject are briefly presented.It is expected that this review will contribute to the rational design and applications of stimu-liresponsive ionic liquids in the future.展开更多
The study introduces eco-friendly leaching agents as alternatives to traditional rare earth element(REE)extraction solvents,addressing environmental concerns associated with ammonium sulfate.Bio-based ionic liquids(IL...The study introduces eco-friendly leaching agents as alternatives to traditional rare earth element(REE)extraction solvents,addressing environmental concerns associated with ammonium sulfate.Bio-based ionic liquids(ILs),known for their non-toxic and biodegradable properties,were screened using the COSMO-RS software.Initially,105 ILs involving 7 cations and 15 anions were computationally screened to find the best ILs for REE extraction.The chosen criteria were based on hydrogen bond formation,affinity screening,hydrophobicity,viscosity,and eco-toxicity test.Based on the COSMO-RS screening,choline oleate,choline decanoate,and choline hexanoate exhibit high solubility for REEs,with a chemical potential of 17.60,17.01,and 18.37 kcal/mol at REE oxidation state+2.Choline glycinate,choline oleate,choline decanoate,choline hexanoate,choline lysinate,and choline leucinate were selected for their strong affinity to extract REE dissociate ions.Experimental results show slightly higher REE extraction from ammonium sulfate(3.17 ppm)compared to choline glycinate(3.15 ppm).For long-term applications,choline glycinate offers a promising eco-friendly and cost-effective alternative to traditional leaching agents,promoting economic feasibility and environmental friendliness.展开更多
Rare earth elements(REEs) were extracted from phosphogypsum(PG) using an indirect leaching method that produces CaCO_(3).The carbonation process transforms PG into CaCO_(3),and a potential source of value is the(NH_(4...Rare earth elements(REEs) were extracted from phosphogypsum(PG) using an indirect leaching method that produces CaCO_(3).The carbonation process transforms PG into CaCO_(3),and a potential source of value is the(NH_(4))_(2)SO_(4) fertilizer.The calcium carbonate byproduct is rich in REEs that are originally present in PG.Calcium carbonate,a byproduct of PG carbonation and a rich source of REEs,could dissolve in nitric acid to produce a calcium nitrate leach solution that contains RE nitrate.Subsequently,the most widely used solvent extraction technique can make use of an environmentally benign nitrate ionic liquid.Cyphos IL 101(trihexyl(tetradecyl)phosphonium chloride) is transformed into trihexyl(tetradecyl)phosphonium nitrate([P_(66614)][NO_(3)]) ionic liquid by adding 2.5 mol/L potassium nitrate.The extraction examinations were tested by equilibration of 2 mL of [P_(66614)][NO_(3)] with 2 mL of a synthetic solution of 1000 mg/L of individual La,Ce,and Nd to gain the optimal extraction conditions.The high extraction efficiency of La,Ce,and Nd was gained by stirring a 1/1 aqueous/organic phase ratio and 3 mol/L NH_(4)NO_(3)(as salting out) at 800 r/min for 40 min at 50℃ to decrease the viscosity of [P_(66614)][NO_(3)].The La(Ⅲ),Ce(Ⅲ),and Nd(Ⅲ) stripping efficiencies were examined from their loaded [P_(66614)][NO_(3)] ionic liquid by 1/1 A/O ratio of acidified water,800 r/min stirring speed,and 25℃.After nine cycles,the extraction and stirring efficiency for the La,Ce,and Nd drop to about 80%.The extraction and stripping parameters are applied to the RE leachate from PG to gain the RE oxide with an assay of 92.67%.展开更多
In the quest for the development of safer lithium-metal batteries(LMBs),the integration of inorganic fillers and ionic liquids into polymer matrices has emerged as a promising strategy to enhance safety,ionic conducti...In the quest for the development of safer lithium-metal batteries(LMBs),the integration of inorganic fillers and ionic liquids into polymer matrices has emerged as a promising strategy to enhance safety,ionic conductivity and battery performance.This study introduces a novel composite ionogel(IG)synthesized through a facile one-pot method,incorporating butyl methacrylate(BMA)and poly(ethylene glycol)diacrylate(PEGDA)with the ionic liquid 1-butyl-1-methylpyrrolidinium bis(fluorosulfonyl)imide(PYR_(14)FSI)and garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)nanoparticles.A distinctive feature of the approach is the use of an organosilane functionalization of the LLZTO nanoparticles,which ensures their full integration into the polymer matrix during free-radical polymerization.Moreover,this method effectively eliminates the Li_(2)CO_(3)passivation layer that typically forms on the surface of the LLZTO nanoparticles,thus,further contributing to an enhanced performance.As a result,a LMB with the functionalized LLZTO IG electrolyte delivered more than 160 mA h g^(−1)with a very good capacity retention of 97.7%after 400 cycles in Li|IG|LFP cells.展开更多
Solid-state batteries(SSBs) are highly attractive on account of their high energy density and good safety.In high-voltage and high-current conditions,however,the interface reactions,structural changes,and decompositio...Solid-state batteries(SSBs) are highly attractive on account of their high energy density and good safety.In high-voltage and high-current conditions,however,the interface reactions,structural changes,and decomposition of the electrolyte impede the transmission of lithium ions in all-solid-state lithium batteries(ASSLBs),significantly reducing the charging and discharging capacity and cycling stability of the battery and therefore restricting its practical applications.The main content of review is to conduct an in-depth analysis of the existing problems of solid-state batteries from the aspects of interface reactions,material failure,ion migration,and dendrite growth,and points out the main factors influencing the electrochemical performance of ASSLBs.Additionally,the compatibility and ion conduction mechanisms between polymer electrolytes,inorganic solid electrolytes,and composite electrolytes and the electrode materials are discussed.Furthermore,the perspectives of electrode materials,electrolyte properties,and interface modification are summarized and prospected,providing new optimization directions for the future commercialization of high-voltage solid-state electrolytes.展开更多
The rising need for efficient and sustainable energy storage systems has led to increased interest in the use of advanced electrolytes consisting of deep eutectic solvents(DESs) and ionic liquids(ILs).These electrolyt...The rising need for efficient and sustainable energy storage systems has led to increased interest in the use of advanced electrolytes consisting of deep eutectic solvents(DESs) and ionic liquids(ILs).These electrolytes are appealing candidates for supercapacitors,next-generation lithium-ion batteries,and different energy storage systems because of their special features including non-flammability,low volatility,lowtoxicity,good electrochemical stability,and good thermal and chemical stability.This review explores the advantages of the proposed electrolytes by examining their potential to address the critical challenges in lithium battery technology,including safety concerns,energy density limitations,and operational stability.To achieve this,a comprehensive overview of the lithium salts commonly employed in rechargeable lithium battery electrolytes is presented.Moreover,key physicochemical and functional attributes of ILs and DESs,such as electrochemical stability,ionic conductivity,nonflammability,and viscosity are also discussed with a focus on how these features impact battery performance.The integration of lithium salts with ILs and DESs in modern lithium battery technologies,including lithium-ion(Li-ion) batteries,lithium-oxygen(Li-O_(2)) batteries,and lithium-sulfur(Li-S) batteries,are further examined in the study.Various electrochemical performance metrics including cycling stability,charge/discharge profiles,retention capacity and battery's couiombic efficiency(CE) are also analyzed for the above-mentioned systems.By summarizing recent advances and challenges,this review also highlights the potential of electrolytes consisting of DESs and ILs to enhance energy density,durability,and safety in future energy storage applications.Additionally future research directions,including the molecular optimization of ILs and DESs,optimizing lithium salt compositions,and developing scalable synthesis methods to accelerate their practical implementation in next-generation energy storage applications are also explored.展开更多
Battery safety is influenced by various factors,with thermal runaway being one of the most significant concerns.While most studies have concentrated on developing one-time,self-activating mechanism for thermal protect...Battery safety is influenced by various factors,with thermal runaway being one of the most significant concerns.While most studies have concentrated on developing one-time,self-activating mechanism for thermal protection,such as temperature-responsive electrodes,and thermal-shutdown separators,these methods only provide irreversible protection.Recently,reversible temperature-sensitive electrolytes have emerged as promising alternatives,offering both thermo-reversibility and self-protective properties.However,further research is crucial to fully understand these thermal-shutdown electrolytes.In this study,we propose lower critical solution temperature(LCST)phase behavior poly(benzyl methacrylate)/imidazolium-based ionic liquid mixtures to prepare temperature-sensitive electrolytes that provide reversible thermal shutdown protection of batteries.This electrolyte features an appropriate protection temperature(~105℃)and responds quickly within a 1 min at 105℃,causing cells to hardly discharge as the voltage suddenly drops to 3.38 V,and providing efficient thermal shutdown protection within 30 min.Upon cooling back to room temperature,the battery regains its original performance.Additionally,the electrolyte exhibits excellent cycling stability with the capacity retention of the battery is 91.6%after 500 cycles.This work provides a viable solution for preventing batteries from thermal runaway triggered by overheating.展开更多
Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium batteries.However,the poor chemical stability and compatibilit...Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium batteries.However,the poor chemical stability and compatibility with lithium metal limit their application.Herein,Li_(5.4)PS_(4.4)Cl1.4I0.2solid electrolyte with high ionic conductivity of 11.49 m S ccm^(-1)and improved chemical stability is synthesized by iodine doping.An ultra-thin Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane with thickness of 10μm can be obtained by wet coating process,exhibiting a high ionic conductivity of 2.09 mS ccm^(-1)and low areal resistance of 1.17Ωcm^(-2).Moreover,iodine doping could in-situ form LiI at the lithium/electrolyte interface and improve the critical current density of Li_(5.4)PS_(4.4)Cl_(1.6)from 0.8 to 1.35 mA cm^(-2).The resultant LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)/Li battery shows excellent cycling stability at 1 C,with a reversible specific capacity of 110.1 mA h g^(-1)and a retention of 80.5% after 1000 cycles.In addition,the assembled LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane/Li pouch cell delivers an initial discharge capacity of 110.4 mA h g^(-1)and 80.5% capacity retention after 100 cycles.展开更多
Moisture enabled electric generation(MEG)is an innovative green energy technology that converts the chemical potential energy of atmospheric water vapor into electricity.Here,we report a novel molecular-level zero-dim...Moisture enabled electric generation(MEG)is an innovative green energy technology that converts the chemical potential energy of atmospheric water vapor into electricity.Here,we report a novel molecular-level zero-dimensional(0D)perovskite-based MEG device that efficiently harvests ambient moisture to generate electric power,which makes perovskite a new kind of potential MEG.The 0D perovskite,DAP₂PbI₆,(where DAP is 1,3-bis(ammonium)-2-hydroxypropane diiodide.)features a unique hydrogen-bonding network formed between its ammonium(–NH_(3)^(+))and hydroxyl(–OH)groups,imparting water stability and remarkable hydrophilicity.Such robust interactions facilitate water adsorption and the subsequent release of hydrogen ions under humid conditions.These protonic species establish an ion gradient,driving a directional current via the ion-gradient diffusion–induced voltage.We demonstrated a maximum volumetric power density of 45 mW·cm^(–3)—substantially exceeding previously reported values for protein-or carbon-based MEG.Additionally,SEM and AFM analyses confirm DAP₂PbI₆is stable upon moisture exposure,while temperature-dependent impedance spectroscopy and theoretical calculations reveal that proton diffusion is the primary mechanism for the observed moisture-driven electricity.These findings underscore the promise of hydrophilic 0D perovskite materials for high-efficiency MEG and pave the way for next-generation sustainable power applications.展开更多
Ionic liquids (ILs) and deep eutectic solvents (DESs) as green solvents have attracted dramatic attention recently due to their highly tunable properties. However, traditional experimental screening methods are ineffi...Ionic liquids (ILs) and deep eutectic solvents (DESs) as green solvents have attracted dramatic attention recently due to their highly tunable properties. However, traditional experimental screening methods are inefficient and resource-intensive. The article provides a comprehensive overview of various ML algorithms, including artificial neural network (ANN), support vector machine (SVM), random forest (RF), and gradient boosting trees (GBT), etc., which have demonstrated exceptional performance in handling complex and high-dimensional data. Furthermore, the integration of ML with quantum chemical calculations and conductor-like screening model-real solvent (COSMO-RS) has significantly enhanced predictive accuracy, enabling the rapid screening and design of novel solvents. Besides, recent ML applications in the prediction and design of ILs and DESs focused on solubility, melting point, electrical conductivity, and other physicochemical properties become more and more. This paper emphasizes the potential of ML in solvent design, overviewing an efficient approach to accelerate the development of sustainable and high-performance materials, providing guidance for their widespread application in a variety of industrial processes.展开更多
Perovs kite-type Li_(0.33)La_(0.56)TiO_(3)(LLTO)shows greate r advantages than organic liquid electrolytes to be used in all-so lid-state lithium-ion batteries with high energy densities.Ionic liquid[BMIM][BF4]was use...Perovs kite-type Li_(0.33)La_(0.56)TiO_(3)(LLTO)shows greate r advantages than organic liquid electrolytes to be used in all-so lid-state lithium-ion batteries with high energy densities.Ionic liquid[BMIM][BF4]was used to improve the properties of Li_(0.33)La_(0.56)TiO_(3)by attrition milling in this study.The microstructure,crystallinity and lithium-ion conductivity of the samples were measured by scanning electron microscopy(SEM),X-ray diffraction(XRD),and impedance spectroscopy(IS).The total ionic conductivities of the samples LLTO+x wt%[BMIM][BF4]increase upon adding[BMIM][BF4]and the maximum conductivity reaches4.71×10^(-4)S/cm when x=12.5 wt%.The enhancement of the total conductivity is ascribed to the bridging role of the ionic liquid among grains,as evidenced by the low activation energy of 0.17-0.25 eV and the SEM observation.The Li+transference numbers of the hybrid samples are all lower than that of the pure LLTO,indicating the existence of electronic conductions.The hybrid mate rial with a mixed conductivity and good stability in the atmosphere can find uses in all-solid-state lithium-ion batteries to improve the interface contact between electrolytes and electrodes.展开更多
基金the Na-tional Natural Science Foundation of China(Nos.21922813,21776278,and 21736003)the Beijing Natural Science Foundation(2182068)+1 种基金DNL Cooperation Fund,CAS(DNL180202)Youth Innovation Promotion Association,CAS(2017066)。
文摘lonic liquids with stimuli-responsive characteristics are an essential branch in the comprehensive ionic liquids'family,which can meet the controllable and reversible needs in practical applications with different stimulation means.In this review,we summarize the recent research progress of these stimuli-responsive ionic liquids,mainly focusing on their chemical structures,properties,responsive mechanism,aggregation structures,and phase behaviors,which were driven by external stimuli,such as CO2,magnetism,light,temperature,redox,and pH.Then,the particular or potential applications of stimuli-responsive ionic liquids are expounded in various fields of science,including catalytic reaction,extraction,separation,nano-material preparation,and gas absorption.In the end,the challenges and strategies of the subject are briefly presented.It is expected that this review will contribute to the rational design and applications of stimu-liresponsive ionic liquids in the future.
基金supported by Petronas Research Sdn Bhd(PRSB)with grant number(015M20-129)Centre of Research in Ionic Liquids(CORIL)Universiti Teknologi PETRONAS for the facilities and support provided。
文摘The study introduces eco-friendly leaching agents as alternatives to traditional rare earth element(REE)extraction solvents,addressing environmental concerns associated with ammonium sulfate.Bio-based ionic liquids(ILs),known for their non-toxic and biodegradable properties,were screened using the COSMO-RS software.Initially,105 ILs involving 7 cations and 15 anions were computationally screened to find the best ILs for REE extraction.The chosen criteria were based on hydrogen bond formation,affinity screening,hydrophobicity,viscosity,and eco-toxicity test.Based on the COSMO-RS screening,choline oleate,choline decanoate,and choline hexanoate exhibit high solubility for REEs,with a chemical potential of 17.60,17.01,and 18.37 kcal/mol at REE oxidation state+2.Choline glycinate,choline oleate,choline decanoate,choline hexanoate,choline lysinate,and choline leucinate were selected for their strong affinity to extract REE dissociate ions.Experimental results show slightly higher REE extraction from ammonium sulfate(3.17 ppm)compared to choline glycinate(3.15 ppm).For long-term applications,choline glycinate offers a promising eco-friendly and cost-effective alternative to traditional leaching agents,promoting economic feasibility and environmental friendliness.
文摘Rare earth elements(REEs) were extracted from phosphogypsum(PG) using an indirect leaching method that produces CaCO_(3).The carbonation process transforms PG into CaCO_(3),and a potential source of value is the(NH_(4))_(2)SO_(4) fertilizer.The calcium carbonate byproduct is rich in REEs that are originally present in PG.Calcium carbonate,a byproduct of PG carbonation and a rich source of REEs,could dissolve in nitric acid to produce a calcium nitrate leach solution that contains RE nitrate.Subsequently,the most widely used solvent extraction technique can make use of an environmentally benign nitrate ionic liquid.Cyphos IL 101(trihexyl(tetradecyl)phosphonium chloride) is transformed into trihexyl(tetradecyl)phosphonium nitrate([P_(66614)][NO_(3)]) ionic liquid by adding 2.5 mol/L potassium nitrate.The extraction examinations were tested by equilibration of 2 mL of [P_(66614)][NO_(3)] with 2 mL of a synthetic solution of 1000 mg/L of individual La,Ce,and Nd to gain the optimal extraction conditions.The high extraction efficiency of La,Ce,and Nd was gained by stirring a 1/1 aqueous/organic phase ratio and 3 mol/L NH_(4)NO_(3)(as salting out) at 800 r/min for 40 min at 50℃ to decrease the viscosity of [P_(66614)][NO_(3)].The La(Ⅲ),Ce(Ⅲ),and Nd(Ⅲ) stripping efficiencies were examined from their loaded [P_(66614)][NO_(3)] ionic liquid by 1/1 A/O ratio of acidified water,800 r/min stirring speed,and 25℃.After nine cycles,the extraction and stirring efficiency for the La,Ce,and Nd drop to about 80%.The extraction and stripping parameters are applied to the RE leachate from PG to gain the RE oxide with an assay of 92.67%.
基金the German Federal Ministry for Education and Research(BMBF)for financial support within the FB2-Hybrid project(03XP0428B)Moreover,D.Bresser and T.Diemant would like to acknowledge financial support from the Helmholtz Association.
文摘In the quest for the development of safer lithium-metal batteries(LMBs),the integration of inorganic fillers and ionic liquids into polymer matrices has emerged as a promising strategy to enhance safety,ionic conductivity and battery performance.This study introduces a novel composite ionogel(IG)synthesized through a facile one-pot method,incorporating butyl methacrylate(BMA)and poly(ethylene glycol)diacrylate(PEGDA)with the ionic liquid 1-butyl-1-methylpyrrolidinium bis(fluorosulfonyl)imide(PYR_(14)FSI)and garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)nanoparticles.A distinctive feature of the approach is the use of an organosilane functionalization of the LLZTO nanoparticles,which ensures their full integration into the polymer matrix during free-radical polymerization.Moreover,this method effectively eliminates the Li_(2)CO_(3)passivation layer that typically forms on the surface of the LLZTO nanoparticles,thus,further contributing to an enhanced performance.As a result,a LMB with the functionalized LLZTO IG electrolyte delivered more than 160 mA h g^(−1)with a very good capacity retention of 97.7%after 400 cycles in Li|IG|LFP cells.
基金financial support received from the National Key R&D Program of China (2023YFB2504000)the financial support from the National Outstanding Youth Foundation of China (52125104)+2 种基金the National Natural Science Foundation of China (52071285)the Fundamental Research Funds for the Central Universities (226-2024-00075)the National Youth Top-Notch Talent Support Program。
文摘Solid-state batteries(SSBs) are highly attractive on account of their high energy density and good safety.In high-voltage and high-current conditions,however,the interface reactions,structural changes,and decomposition of the electrolyte impede the transmission of lithium ions in all-solid-state lithium batteries(ASSLBs),significantly reducing the charging and discharging capacity and cycling stability of the battery and therefore restricting its practical applications.The main content of review is to conduct an in-depth analysis of the existing problems of solid-state batteries from the aspects of interface reactions,material failure,ion migration,and dendrite growth,and points out the main factors influencing the electrochemical performance of ASSLBs.Additionally,the compatibility and ion conduction mechanisms between polymer electrolytes,inorganic solid electrolytes,and composite electrolytes and the electrode materials are discussed.Furthermore,the perspectives of electrode materials,electrolyte properties,and interface modification are summarized and prospected,providing new optimization directions for the future commercialization of high-voltage solid-state electrolytes.
文摘The rising need for efficient and sustainable energy storage systems has led to increased interest in the use of advanced electrolytes consisting of deep eutectic solvents(DESs) and ionic liquids(ILs).These electrolytes are appealing candidates for supercapacitors,next-generation lithium-ion batteries,and different energy storage systems because of their special features including non-flammability,low volatility,lowtoxicity,good electrochemical stability,and good thermal and chemical stability.This review explores the advantages of the proposed electrolytes by examining their potential to address the critical challenges in lithium battery technology,including safety concerns,energy density limitations,and operational stability.To achieve this,a comprehensive overview of the lithium salts commonly employed in rechargeable lithium battery electrolytes is presented.Moreover,key physicochemical and functional attributes of ILs and DESs,such as electrochemical stability,ionic conductivity,nonflammability,and viscosity are also discussed with a focus on how these features impact battery performance.The integration of lithium salts with ILs and DESs in modern lithium battery technologies,including lithium-ion(Li-ion) batteries,lithium-oxygen(Li-O_(2)) batteries,and lithium-sulfur(Li-S) batteries,are further examined in the study.Various electrochemical performance metrics including cycling stability,charge/discharge profiles,retention capacity and battery's couiombic efficiency(CE) are also analyzed for the above-mentioned systems.By summarizing recent advances and challenges,this review also highlights the potential of electrolytes consisting of DESs and ILs to enhance energy density,durability,and safety in future energy storage applications.Additionally future research directions,including the molecular optimization of ILs and DESs,optimizing lithium salt compositions,and developing scalable synthesis methods to accelerate their practical implementation in next-generation energy storage applications are also explored.
基金funded by the National Natural Science Foundation of China(no.22075155)the Zhejiang Provincial Natural Science Foundation of China(No.LY24B030002)+2 种基金Ningbo Natural Science Foundation(2023J089)the China Scholarship Council(CSC)the Ningbo Science and Technology Bureau(2024QL036).
文摘Battery safety is influenced by various factors,with thermal runaway being one of the most significant concerns.While most studies have concentrated on developing one-time,self-activating mechanism for thermal protection,such as temperature-responsive electrodes,and thermal-shutdown separators,these methods only provide irreversible protection.Recently,reversible temperature-sensitive electrolytes have emerged as promising alternatives,offering both thermo-reversibility and self-protective properties.However,further research is crucial to fully understand these thermal-shutdown electrolytes.In this study,we propose lower critical solution temperature(LCST)phase behavior poly(benzyl methacrylate)/imidazolium-based ionic liquid mixtures to prepare temperature-sensitive electrolytes that provide reversible thermal shutdown protection of batteries.This electrolyte features an appropriate protection temperature(~105℃)and responds quickly within a 1 min at 105℃,causing cells to hardly discharge as the voltage suddenly drops to 3.38 V,and providing efficient thermal shutdown protection within 30 min.Upon cooling back to room temperature,the battery regains its original performance.Additionally,the electrolyte exhibits excellent cycling stability with the capacity retention of the battery is 91.6%after 500 cycles.This work provides a viable solution for preventing batteries from thermal runaway triggered by overheating.
基金National Key R&D Program of China (grant no. 2022YFB3807700)National Natural Science Foundation of China (Grant No. U1964205, U21A2075, 52172253,52102326, 52250610214, 22309194, 52372244)+4 种基金Ningbo S&T Innovation 2025 Major Special Programme (Grant No.2019B10044, 2021Z122, 2023Z106)Zhejiang Provincial Key R&D Program of China (Grant No. 2022C01072, 2024C01095)Jiangsu Provincial S&T Innovation Special Programme for carbon peak and carbon neutrality (Grant No. BE2022007)Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation of China (LBMHD24E020001)Youth Innovation Promotion Association CAS (Y2021080)。
文摘Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium batteries.However,the poor chemical stability and compatibility with lithium metal limit their application.Herein,Li_(5.4)PS_(4.4)Cl1.4I0.2solid electrolyte with high ionic conductivity of 11.49 m S ccm^(-1)and improved chemical stability is synthesized by iodine doping.An ultra-thin Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane with thickness of 10μm can be obtained by wet coating process,exhibiting a high ionic conductivity of 2.09 mS ccm^(-1)and low areal resistance of 1.17Ωcm^(-2).Moreover,iodine doping could in-situ form LiI at the lithium/electrolyte interface and improve the critical current density of Li_(5.4)PS_(4.4)Cl_(1.6)from 0.8 to 1.35 mA cm^(-2).The resultant LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)/Li battery shows excellent cycling stability at 1 C,with a reversible specific capacity of 110.1 mA h g^(-1)and a retention of 80.5% after 1000 cycles.In addition,the assembled LiCoO_(2)/Li_(5.4)PS_(4.4)Cl_(1.4)I_(0.2)membrane/Li pouch cell delivers an initial discharge capacity of 110.4 mA h g^(-1)and 80.5% capacity retention after 100 cycles.
基金supported by the National Natural Science Foundation of China(Nos.52102217,52102332)the Natural Science Foundation of Fujian Province(2021J05120).
文摘Moisture enabled electric generation(MEG)is an innovative green energy technology that converts the chemical potential energy of atmospheric water vapor into electricity.Here,we report a novel molecular-level zero-dimensional(0D)perovskite-based MEG device that efficiently harvests ambient moisture to generate electric power,which makes perovskite a new kind of potential MEG.The 0D perovskite,DAP₂PbI₆,(where DAP is 1,3-bis(ammonium)-2-hydroxypropane diiodide.)features a unique hydrogen-bonding network formed between its ammonium(–NH_(3)^(+))and hydroxyl(–OH)groups,imparting water stability and remarkable hydrophilicity.Such robust interactions facilitate water adsorption and the subsequent release of hydrogen ions under humid conditions.These protonic species establish an ion gradient,driving a directional current via the ion-gradient diffusion–induced voltage.We demonstrated a maximum volumetric power density of 45 mW·cm^(–3)—substantially exceeding previously reported values for protein-or carbon-based MEG.Additionally,SEM and AFM analyses confirm DAP₂PbI₆is stable upon moisture exposure,while temperature-dependent impedance spectroscopy and theoretical calculations reveal that proton diffusion is the primary mechanism for the observed moisture-driven electricity.These findings underscore the promise of hydrophilic 0D perovskite materials for high-efficiency MEG and pave the way for next-generation sustainable power applications.
基金supported by the National Key Research and Development Program of China(2022YFB3504702)support from Horizon-EIC,Pathfinder challenges(101070976)+3 种基金support from the National Natural Science Foundation of China(22278402,22478389)the Key Research and Development Program of Henan Province(231111241800)State Key Laboratory of Mesoscience and Engineering(MESO-23-A08)the Frontier Basic Research Projects of Institute of Process Engineering,CAS(QYJC-2023-03).
文摘Ionic liquids (ILs) and deep eutectic solvents (DESs) as green solvents have attracted dramatic attention recently due to their highly tunable properties. However, traditional experimental screening methods are inefficient and resource-intensive. The article provides a comprehensive overview of various ML algorithms, including artificial neural network (ANN), support vector machine (SVM), random forest (RF), and gradient boosting trees (GBT), etc., which have demonstrated exceptional performance in handling complex and high-dimensional data. Furthermore, the integration of ML with quantum chemical calculations and conductor-like screening model-real solvent (COSMO-RS) has significantly enhanced predictive accuracy, enabling the rapid screening and design of novel solvents. Besides, recent ML applications in the prediction and design of ILs and DESs focused on solubility, melting point, electrical conductivity, and other physicochemical properties become more and more. This paper emphasizes the potential of ML in solvent design, overviewing an efficient approach to accelerate the development of sustainable and high-performance materials, providing guidance for their widespread application in a variety of industrial processes.
基金supported by the Natural Science Foundation of Hebei Province(E2021502013)Key Research and Development Projects of Hebei Province(21373805D)。
文摘Perovs kite-type Li_(0.33)La_(0.56)TiO_(3)(LLTO)shows greate r advantages than organic liquid electrolytes to be used in all-so lid-state lithium-ion batteries with high energy densities.Ionic liquid[BMIM][BF4]was used to improve the properties of Li_(0.33)La_(0.56)TiO_(3)by attrition milling in this study.The microstructure,crystallinity and lithium-ion conductivity of the samples were measured by scanning electron microscopy(SEM),X-ray diffraction(XRD),and impedance spectroscopy(IS).The total ionic conductivities of the samples LLTO+x wt%[BMIM][BF4]increase upon adding[BMIM][BF4]and the maximum conductivity reaches4.71×10^(-4)S/cm when x=12.5 wt%.The enhancement of the total conductivity is ascribed to the bridging role of the ionic liquid among grains,as evidenced by the low activation energy of 0.17-0.25 eV and the SEM observation.The Li+transference numbers of the hybrid samples are all lower than that of the pure LLTO,indicating the existence of electronic conductions.The hybrid mate rial with a mixed conductivity and good stability in the atmosphere can find uses in all-solid-state lithium-ion batteries to improve the interface contact between electrolytes and electrodes.
