Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures,bringing challenges to the application of lithium-ion batteries(LIBs)at low temperatures.H...Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures,bringing challenges to the application of lithium-ion batteries(LIBs)at low temperatures.Herein,the ester solvent of methyl propionate(MP)with low melting point and low viscosity was used to tackle ion transport difficulty in electrolytes.Fluorinated ester was further added to accelerate interfacial transport through intermolecular interactions.The influence of fluorinated esters with different fluorination degrees on the solvation structure of electrolytes and the performance of batteries was further studied.As a result,methyl pentafluoropropionate(M5F)with five fluorine atoms was selected for its optimal interactions with both Li+and MP solvent in the primary solvation structure,contributing to desired solvation structure for fast interfacial transport.The LiFePO_(4)(LFP)||graphite cell with LiFSI-MP-M5F electrolyte exhibited a high cyclability of 85.8%after 120 cycles and retained 81.2%of room-temperature capacity when charged and discharged at−30℃.1 Ah LFP||graphite pouch cell with high cathode loading(20 mg/cm^(2))in LiFSI-MP-M5F electrolyte exhibited 0.85 Ah capacity when charged and discharged at−20℃.This work provides a guidance for electrolyte design by synergistic fluorinated and non-fluorinated solvents for LIBs at low-temperature application.展开更多
Composite solid-state electrolytes incorporating metal-organic frameworks(MOFs)demonstrate tremendous potential for ameliorating Li^(+)conduction in lithium metal batteries.However,their practical application is hinde...Composite solid-state electrolytes incorporating metal-organic frameworks(MOFs)demonstrate tremendous potential for ameliorating Li^(+)conduction in lithium metal batteries.However,their practical application is hindered by low ionic co nductivity and unstable Li^(+)transport at the electrode interfaces.To overcome these challenges,a previously unreported family of indium based MOFs(In-BDC-F_(x),x=0,4,6)with tunable fluorine content was synthesized and integrated into PVDF-HFP matrices to construct highperformance quasi-solid-state electrolytes.By systematically modulating linker fluorination,a bifunctional enhancement mechanism is revealed:fluorinated indium centers simultaneously suppress polymer crystallinity and establish preferential Li^(+)conduction pathways.Remarkably,In-BDC-F_(6) manifests exceptional synergistic interactions between-CF_(3) functionalities and indium coordination sites,amplifying Lewis acidity to facilitate LiTFSI dissociation and TFSI-immobilization,culminating in homogeneous LiF-enriched solid electrolyte interphases.The optimized electrolyte demonstrates compelling electrochemical performance:ionic conductivity of 9.68×10^(-4) S cm^(-1),Li^(+)transference number of 0.70,and electrochemical stability window of 4.96 V.Li‖Li symmetric cell demonstrated a critical current density of 3.5 mA cm^(-2) and stable plating/stripping for over 1000 h at 0.2 mA cm^(-2),while LiFePO_(4)‖Li cells retain96.66%capacity after 1300 cycles at 10C,underscoring the transformative potential of fluorinated MOF architectures in fast-charging solid-state batteries.展开更多
Fluorinated carbon is a prospective cathode material for lithium(Li)primary batteries,which are widely used as power sources for military applications,such as individual combat,spacecraft,and deep-sea detection.It off...Fluorinated carbon is a prospective cathode material for lithium(Li)primary batteries,which are widely used as power sources for military applications,such as individual combat,spacecraft,and deep-sea detection.It offers high gram-specific capacity but is hindered by its low intrinsic conductivity and large volume expansion.However,fluorinated Ketjen black(FKB),with enhanced conductivity and less volume expansion compared with other fluorinated analogs,has been the subject of extensive attention,with its discharge mechanism being unclear.Herein,the structural evolution and compositional changes of FKB at various depths of discharge are revealed through characterization and analysis:The three-dimensional(3D),chain-like aggregate structure of FKB has a high void ratio,which can provide a storage space for LiF formation,thereby inhibiting the volume deformation during discharge.The discharge reaction model is a synergistic mechanism of a surface uniform reaction and local structural reorganization.The surface and defect sites preferentially react with Li^(+)and the C-F bonds in the 3D,chain-like structure selectively break to form LiF.We anticipate that our study paves the way for implementing better Li/fluorinated carbon(Li/CF_(x))batteries.展开更多
In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still face...In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.展开更多
Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the sol...Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.展开更多
High-voltage Li metal batteries hold great promise for next-generation energy storage,but constructing robust and highly conductive electrode/electrolyte interfaces via electrolyte engineering to enhance the battery p...High-voltage Li metal batteries hold great promise for next-generation energy storage,but constructing robust and highly conductive electrode/electrolyte interfaces via electrolyte engineering to enhance the battery performance is still a challenge.Herein,we propose a non-coordinating solvent anchoring strategy to regulate fluorinated amide electrolyte to enhance the stability and ionic conductivity of the interfaces.Specifically,hexafluorobenzene is employed to anchor fluorinated amide solvent by the robust dipole–dipole interactions,which weaken the coordination between fluorinated amide and Li^(+),facilitate more anions coordinating with Li^(+),and form more ion aggregates.Consequently,stable and highly conductive electrode/electrolyte interfaces enriched with LiF and Li_(3)N are constructed,drastically improving the interfacial stability and reducing interface impedance of Li metal anodes and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathodes.Such a rationally designed electrolyte demonstrates excellent flame retardancy,high oxidation stability(5.1 V vs.Li^(+)/Li),and enhanced low-temperature ionic conductivity.As a result,this electrolyte substantially enhances the high-voltage cycle stability(-4.8 V),rate capability(-50 C)and low-temperature cycle performance(-20℃)of Li||NCM811 cells,which retain 80.0%of the initial capacity over 600 cycles at 4.7 V.This research offers a promising strategy to design ideal electrolytes for highperformance Li metal batteries.展开更多
The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application.To enhance the oxidative stability of ether-based electrolytes,the physicochemical properties o...The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application.To enhance the oxidative stability of ether-based electrolytes,the physicochemical properties of various glycol dimethyl ethers are screened,and diglyme(G2)is selected as the sole solvent for the electrolyte.Lithium bis(fluorosulfonyl)imide(LiFSI),a highly dissociative salt,is used as the primary salt;while lithium nitrate(LiNO_(3))and lithium difluorophosphate(LiDFP),which have small ionic sizes and strong binding energies,are added as secondary salts.The resulting electrolyte can modulate the electric double layer structure by NO_(3)^(-) and DFP^(-) on the cathode side,leading to an increased Liþconcentration that is originally repelled by the cathode.Additionally,the oxidation stability of the electrolyte is improved and the formed electrode-electrolyte interphase is more uniform and stable,thereby enhancing the electrochemical performance of the cells.As a result,cells assembled with a total of 1 M ternary lithium salts in G2 solvent can operate at high voltage of 4.4 V.The LijjNCM811 cells maintain 80.2%capacity retention after 270 cycles at room temperature,with an average Coulombic efficiency of 99.5%,and exhibit 88.4%capacity retention after 200 cycles at -30℃.展开更多
Sulfide-based all-solid-state lithium metal batteries(ASSLMBs)have garnered significant attention due to their potential for high energy density and enhanced safety.However,their practical application is hindered by c...Sulfide-based all-solid-state lithium metal batteries(ASSLMBs)have garnered significant attention due to their potential for high energy density and enhanced safety.However,their practical application is hindered by challenges such as uneven lithium(Li)deposition and the growth of Li dendrites.In this contribution,we propose an amorphous fluorinated interphase(AFI),composed of amorphous LiF and lithiated graphite,to regulate the interfacial Li-ion transport kinetics through in-situ interface chemistry.Amorphous LiF,which exhibits a significantly enhanced Li-ion diffusion compared to its crystalline counterpart,works synergistically with lithiated graphite to promote both short-range and long-range Li-ion transport kinetics at the Li/electrolyte interface.As a result,the Li anode with AFI demonstrates a remarkably enhanced critical current density of 1.6 mA cm^(−2)and an extended cycle life exceeding 1100 h.The Li||LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)full cell also achieves a high discharge capacity of 125.7 mA h g^(−1)and retains 71.2%of its initial capacity after 200 cycles.This work provides valuable insights into the rational design of artificial anodic interphase to regulate interfacial Li-ion transport kinetics in ASSLMBs.展开更多
Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the...Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.展开更多
Fluorinated graphene has a promising application prospect in lithium primary batteries(LPBs)and sodium primary batteries(SPBs).Herein,five fluorinated graphene materials with different fluorine contents(FG-x)are prepa...Fluorinated graphene has a promising application prospect in lithium primary batteries(LPBs)and sodium primary batteries(SPBs).Herein,five fluorinated graphene materials with different fluorine contents(FG-x)are prepared by a large-scale gas fluorination process.It is found that the structural characteristics of FG-x strongly depend on the fluorination temperature:the fluorine content(i.e.,F/C ratio)gradually increases with the fluorination temperature rising,resulting in the enlargement of interlayer spacing and the increase of average bonding strength between C and F.FG-0.75 sample with the intermediate degree of fluorination achieves the maximum energy densities in LPBs(2239.8 Wh·kg^(-1))and SPBs(1939.2 Wh·kg^(-1)).The interlayer distance is critical to the rate capability of FG-x,and FG-0.95 with the largest lattice spacing exhibits the best rate performance in both Li/CFx and Na/CFx batteries.The electrochemical reaction mechanism and the structural evolution of FG material revealed by ex situ X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD)characterization,and in situ Raman spectra further confirm the effect of interlayer distance.展开更多
Fluorinated gases(F-gases)play a vital role in the chemical industry and in the fields of air conditioning,refrigeration,health care,and organic synthesis.However,the direct emission of waste gases containing F-gases ...Fluorinated gases(F-gases)play a vital role in the chemical industry and in the fields of air conditioning,refrigeration,health care,and organic synthesis.However,the direct emission of waste gases containing F-gases into the atmosphere contributes to greenhouse effects and generates toxic substances.Developing porous materials for the energy-efficient capture,separation,and recovery of F-gases is highly desired.Recently,as a highly designable porous adsorbents,metal–organic frameworks(MOFs)exhibit excellent selective sorption performance toward F-gases,especially for the recognition and separation of different F-gases with highly similar properties,showing their great potential in F-gases control and recovery.In this review,we discuss the capture and separation of F-gases and their azeotropic,near-azeotropic,and isomeric mixtures in various application scenarios by MOFs,specifically classify and analyze molecular interaction between F-gases and MOFs,and interpret the mechanisms underlying their high performance regarding both adsorption capacity and selectivity,providing a repertoire for future materials design.Challenges faced in the transformation research roadmap of MOFs adsorbent separation technologies toward F-gases are also discussed,and areas for future research endeavors are highlighted.展开更多
Fluorinated electrolytes possess good antioxidant capacity that provides high compatibility to high-voltage cathode and flame retardance;thus,they are considered as a promising solution for advanced lithium-ion batter...Fluorinated electrolytes possess good antioxidant capacity that provides high compatibility to high-voltage cathode and flame retardance;thus,they are considered as a promising solution for advanced lithium-ion batteries carrying both high-energy density and high safety.Moreover,the fluorinated electrolytes are widely used to form stable electrolyte interphase,due to their chemical reactivity with lithiated graphite or lithium.However,the influence of this reactivity on the thermal safety of batteries is seldom discussed.Herein,we demonstrate that the flame-retardant fluorinated electrolytes help to reduce the flammability,while the lithium-ion batteries with flame-retardant fluorinated electrolytes still undergo thermal runaway and disclose their different thermal runaway pathway from that of battery with conventional electrolyte.The reduction in fluorinated components(e.g.,LiPF 6 and fluoroethylene carbonate(FEC))by fully lithiated graphite accounts for a significant heat release during battery thermal runaway.The 13%of total heat is sufficient to trigger the chain reactions during battery thermal runaway.This study deepens the understanding of the thermal runaway mechanism of lithium-ion batteries employing flame-retardant fluorinated electrolytes,providing guidance on the concept of electrolyte design for safer lithium-ion batteries.展开更多
X-ray detectors show potential applications in medical imaging,materials science,and nuclear energy.To achieve high detection efficiency and spatial resolution,many conventional semiconductor materials,such as amorpho...X-ray detectors show potential applications in medical imaging,materials science,and nuclear energy.To achieve high detection efficiency and spatial resolution,many conventional semiconductor materials,such as amorphous selenium,cadmium telluride zinc,and perovskites,have been utilized in direct conversion X-ray detectors.However,these semiconductor materials are susceptible to temperature-induced performance degradation,crystallization,delamination,uneven lattice growth,radiation damage,and high dark current.This study explores a new approach by coupling an FC40 electronic fluorinated liquid with a specialized high-resolution and high-readout-speed complementary metal-oxide-semiconductor(CMOS)pixel array,specifically the Topmetal II−chip,to fabricate a direct conversion X-ray detector.The fluorinated liquid FC40(molecular formula:C_(21)F_(48)N_(2))is an electronic medium that is minimally affected by temperature and displays no issues with uniform conductivity.It exhibits a low dark current and minimal radiation damage and enables customizable thickness in X-ray absorption.This addresses the limitations inherent in conventional semiconductor-based detectors.In this study,simple X-ray detector imaging tests were conducted,demonstrating the excellent coupling capability between FC40 electronic fluorinated liquid and CMOS chips by the X-ray detector.A spatial resolution of 4.0 lp/mm was measured using a striped line par card,and a relatively clear image of a cockroach was displayed in the digital radiography imaging results.Preliminary test results indicated the feasibility of fabricating an X-ray detector by combining FC40 electronic fluorinated liquid and CMOS chips.Owing to the absence of issues related to chip-material coupling,a high spatial resolution could be achieved by reducing the chip pixel size.This method presents a new avenue for studies on novel liquid-based direct conversion X-ray detectors.展开更多
The structure evolution of fluorinated graphite （CFx） upon the Li/Na intercalation has been studied by first- principles calculations. The Li/Na adsorption on single CF layer and intercalated into bulk CF have been ...The structure evolution of fluorinated graphite （CFx） upon the Li/Na intercalation has been studied by first- principles calculations. The Li/Na adsorption on single CF layer and intercalated into bulk CF have been calculated. The better cycling performance of Na intercalation into the CF cathode, comparing to that of Li intercalation, is attributed to the different strength and characteristics of the Li-F and Na-F interactions. The interactions between Li and F are stronger and more localized than those between Na and E The strong and localized Coulomb attraction between Li and F atoms breaks the C-F bonds and pulls the F atoms away, and graphene sheets are formed upon Li intercalation.展开更多
Fluorinated carbons CF_xhold the highest theoretical energy density(e.g.,2180 W h kg^(-1)when x=1)among all cathode materials of lithium primary batteries.However,the low conductivity and severe polarization limit it ...Fluorinated carbons CF_xhold the highest theoretical energy density(e.g.,2180 W h kg^(-1)when x=1)among all cathode materials of lithium primary batteries.However,the low conductivity and severe polarization limit it to achieve its theory.In this study,we design a new electrolyte,namely 1 M LiBF_(4)DMSO:DOL(1:9 vol.),achieving a high energy density in Li/CF_xprimary cells.The DMSO with a small molecular size and high donor number successfully solvates Li^(+)into a defined Li^(+)-solvation structure.Such solvated Li^(+)can intercalate into the large-spacing carbon layers and achieve an improved capacity.Consequently,when discharged to 1.0 V,the CF_(1.12)cathode demonstrates a specific capacity of 1944 m A h g^(-1)with a specific energy density of 3793 W h kg^(-1).This strategy demonstrates that designing the electrolyte is powerful in improving the electrochemical performance of CF_(x) cathode.展开更多
Ethyl acetate (EA) shows low viscosity for its relative permittivity. Monofluorinated organic solvents exert the polar effect on the various properties. We have investigated the effect of position isomerism on the phy...Ethyl acetate (EA) shows low viscosity for its relative permittivity. Monofluorinated organic solvents exert the polar effect on the various properties. We have investigated the effect of position isomerism on the physical and electrochemical properties of two monofluorinated carboxylates: 2-fluoroethyl acetate (2FEA) and ethyl fluoroacetate (EFA). Relative permittivity of 2FEA was lower than that of EFA, whereas viscosity of 2FEA was higher. Electrolytic conductivity of a LiPF6 solution in 2FEA was lower than that in EFA, but higher than that in EA at high temperatures. The use of 2FEA as a co-solvent improved cycling efficiency and suppressed fading of discharge capacity of a Li|LiCoO2 coin cell at high cycle numbers.展开更多
High-voltage solid-state lithium-ion batteries(SSLIBs)have attracted considerable research attention in recent years due to their high-energy-density and superior safety characteristics.However,the integration of high...High-voltage solid-state lithium-ion batteries(SSLIBs)have attracted considerable research attention in recent years due to their high-energy-density and superior safety characteristics.However,the integration of high-voltage cathodes with solid electrolytes(SEs)presents multiple challenges,including the formation of high-impedance layers from spontaneous chemical reactions,electrochemical instability,insufficient interfacial contact,and lattice expansion.These issues significantly impair battery performance and potentially lead to battery failure,thus impeding the commercialization of high-voltage SSLIBs.The incorporation of fluorides,known for their robust bond strength and high free energy of formation,has emerged as an effective strategy to address these challenges.Fluorinated electrolytes and electrode/electrolyte interfaces have been demonstrated to significantly influence the reaction reversibility/kinetics,safety,and stability of rechargeable batteries,particularly under high voltage.This review summarizes recent advancements in fluorination treatment for high-voltage SEs,focusing on solid polymer electrolytes(SPEs),inorganic solid electrolytes(ISEs),and composite solid electrolytes(CSEs),along with the performance enhancements these strategies afford.This review aims to provide a comprehensive understanding of the structure-property relationships,the characteristics of fluorinated interfaces,and the application of fluorinated SEs in high-voltage SSLIBs.Further,the impacts of residual moisture and the challenges of fluorinated SEs are discussed.Finally,the review explores potential future directions for the development of fluorinated SSLIBs.展开更多
To improve the friction and wear performance at room and elevated temperatures,Ti48Al2Nb2Cr(at.%)alloy was anodically fluorinated in an NH_(4)F-containing electrolyte.The effects of anodic fluorination on the friction...To improve the friction and wear performance at room and elevated temperatures,Ti48Al2Nb2Cr(at.%)alloy was anodically fluorinated in an NH_(4)F-containing electrolyte.The effects of anodic fluorination on the friction coefficient,wear rate,wear track morphology,and adhesion strength between the oxide scale and substrate were investigated.Results showed that the in-situ formation of Al_(2)O_(3)-enriched oxide scale was promoted due to fluorine effect,by which the surface hardness and wear resistance were both enhanced.After the friction and wear test,no noticeable changes were found on the fluorinated Ti48Al2Nb2Cr,whilst severe abrasion was evident on the GCr15 counterpart.This indicates that anodic fluorination could effectively enhance the friction and wear performance of Ti48Al2Nb2Cr alloy.At elevated temperatures,the dominant wear mechanism of the fluorinated Ti48Al2Nb2Cr/GCr15 pair was oxidation wear and adhesive wear.展开更多
In the research and production of fluorinated materials,large volumes of unstructured textual data are generated,characterized by high heterogeneity and fragmentation.These issues hinder systematic knowledge integrati...In the research and production of fluorinated materials,large volumes of unstructured textual data are generated,characterized by high heterogeneity and fragmentation.These issues hinder systematic knowledge integration and efficient utilization.Constructing a knowledge graph for fluorinated materials processing is essential for enabling structured knowledge management and intelligent applications.Among its core components,Named Entity Recognition(NER)plays an essential role,as its accuracy directly impacts relation extraction and semantic modeling,which ultimately affects the knowledge graph construction for fluorinated materials.However,NER in this domain faces challenges such as fuzzy entity boundaries,inconsistent terminology,and a lack of high-quality annotated corpora.To address these problems,(i)We first construct a domain-specific NER dataset by combining manual annotation with an improved Easy Data Augmentation(EDA)strategy;(ii)Secondly,we propose a novel model,RRC-ADV,which integrates RoBERTa-wwm for dynamic contextual word representation,adversarial training to improve robustness against boundary ambiguity,and a Residual BiLSTM(ResBiLSTM)to enhance sequential feature modeling.Further,a Conditional Random Field(CRF)layer is incorporated for globally optimized label prediction.Experimental results demonstrate that RRC-ADV achieves an average F1 score of 89.23%on the self-constructed dataset,significantly outperforming baseline models.The model exhibits strong robustness and adaptability within the domain of fluorinated materials.Our work enhances the accuracy of NER in the fluorinated materials processing domain and paves the way for downstream tasks such as relation extraction in knowledge graph construction.展开更多
The construction of monodisperse microporous organic microspheres is deemed a challenging issue,primarily due to the difficulty in achieving both high microporosity and uniformity within the microspheres.In this study...The construction of monodisperse microporous organic microspheres is deemed a challenging issue,primarily due to the difficulty in achieving both high microporosity and uniformity within the microspheres.In this study,a series of fluorinated monodisperse microporous microspheres are fabricated by solvothermal precipitation polymerization.The resulting fluorous methacrylate-based microspheres achieved higher than 400 m^(2)/g surface area,along with a yield of over 90%for the microspheres.Through comprehensive characterization and simulation methods,we discovered that the introduction of fluorous methacrylate monomers at high loading levels is the key factor contributing to the formation of the microporosity within the microspheres.The controlled temperature profile was found to be advantageous for achieving a high yield of microspheres and increased uniformity.Two-dimensional assemblies of these fluorinated microsphere arrays exhibited superhydrophobicity,superolephilicity,and water sliding angles below 10°.Furthermore,a three-dimensional assembly of the fluorinated microporous microsphere in a chromatographic column demonstrated significant improvement in the separation of Engelhardt agent compared to commercial columns.Our work offers a novel approach to constructing fluorinated monodisperse microporous microspheres for advanced applications.展开更多
基金supported by the National Key R&D Program of China(No.2022YFB3803400)National Natural Science Foundation of China(Nos.52102054,52020105010,51927803,52188101 and 52072378)+1 种基金Liaoning Province Science and Technology Planning Project(No.2022-BS-007)Fujian Science and Technology Program(No.2023T3025).
文摘Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures,bringing challenges to the application of lithium-ion batteries(LIBs)at low temperatures.Herein,the ester solvent of methyl propionate(MP)with low melting point and low viscosity was used to tackle ion transport difficulty in electrolytes.Fluorinated ester was further added to accelerate interfacial transport through intermolecular interactions.The influence of fluorinated esters with different fluorination degrees on the solvation structure of electrolytes and the performance of batteries was further studied.As a result,methyl pentafluoropropionate(M5F)with five fluorine atoms was selected for its optimal interactions with both Li+and MP solvent in the primary solvation structure,contributing to desired solvation structure for fast interfacial transport.The LiFePO_(4)(LFP)||graphite cell with LiFSI-MP-M5F electrolyte exhibited a high cyclability of 85.8%after 120 cycles and retained 81.2%of room-temperature capacity when charged and discharged at−30℃.1 Ah LFP||graphite pouch cell with high cathode loading(20 mg/cm^(2))in LiFSI-MP-M5F electrolyte exhibited 0.85 Ah capacity when charged and discharged at−20℃.This work provides a guidance for electrolyte design by synergistic fluorinated and non-fluorinated solvents for LIBs at low-temperature application.
基金the support of the Shenzhen Science and Technology Program(no.JCYJ20220818100405012)National Natural Science Foundation of China(NSFC,no.62374080)Shenzhen Key Laboratory of Intelligent Manufacturing for Continuous Carbon Fiber Reinforced Composites(no.ZDSYS20220527171404011)。
文摘Composite solid-state electrolytes incorporating metal-organic frameworks(MOFs)demonstrate tremendous potential for ameliorating Li^(+)conduction in lithium metal batteries.However,their practical application is hindered by low ionic co nductivity and unstable Li^(+)transport at the electrode interfaces.To overcome these challenges,a previously unreported family of indium based MOFs(In-BDC-F_(x),x=0,4,6)with tunable fluorine content was synthesized and integrated into PVDF-HFP matrices to construct highperformance quasi-solid-state electrolytes.By systematically modulating linker fluorination,a bifunctional enhancement mechanism is revealed:fluorinated indium centers simultaneously suppress polymer crystallinity and establish preferential Li^(+)conduction pathways.Remarkably,In-BDC-F_(6) manifests exceptional synergistic interactions between-CF_(3) functionalities and indium coordination sites,amplifying Lewis acidity to facilitate LiTFSI dissociation and TFSI-immobilization,culminating in homogeneous LiF-enriched solid electrolyte interphases.The optimized electrolyte demonstrates compelling electrochemical performance:ionic conductivity of 9.68×10^(-4) S cm^(-1),Li^(+)transference number of 0.70,and electrochemical stability window of 4.96 V.Li‖Li symmetric cell demonstrated a critical current density of 3.5 mA cm^(-2) and stable plating/stripping for over 1000 h at 0.2 mA cm^(-2),while LiFePO_(4)‖Li cells retain96.66%capacity after 1300 cycles at 10C,underscoring the transformative potential of fluorinated MOF architectures in fast-charging solid-state batteries.
基金supported by 2025 High-Quality Development Special Project(No.CEIEC-2025-ZM02-0008)the National Natural Science Foundation of China(No.52472233)+1 种基金the Natural Science Foundation of Tianjin(No.23JCYBJC01870)the Seed Foundation of Tianjin University(Nos.2025XJ1-0005,2025XJ1-0011)。
文摘Fluorinated carbon is a prospective cathode material for lithium(Li)primary batteries,which are widely used as power sources for military applications,such as individual combat,spacecraft,and deep-sea detection.It offers high gram-specific capacity but is hindered by its low intrinsic conductivity and large volume expansion.However,fluorinated Ketjen black(FKB),with enhanced conductivity and less volume expansion compared with other fluorinated analogs,has been the subject of extensive attention,with its discharge mechanism being unclear.Herein,the structural evolution and compositional changes of FKB at various depths of discharge are revealed through characterization and analysis:The three-dimensional(3D),chain-like aggregate structure of FKB has a high void ratio,which can provide a storage space for LiF formation,thereby inhibiting the volume deformation during discharge.The discharge reaction model is a synergistic mechanism of a surface uniform reaction and local structural reorganization.The surface and defect sites preferentially react with Li^(+)and the C-F bonds in the 3D,chain-like structure selectively break to form LiF.We anticipate that our study paves the way for implementing better Li/fluorinated carbon(Li/CF_(x))batteries.
基金the financial support from the National Natural Science Foundation of China (No. 52072390)the National High-Level Talents Special Support Program (Leading Talent of Technological Innovation)+2 种基金the China Postdoctoral Science Foundation (No. 2023M743648)the Young Scientists Fund of the National Natural Science Foundation of China (No. 52302330)the support from the Shanghai Emperor of Cleaning Hi-Tech Co.,LTD
文摘In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.
基金support from the National Natural Science Foundation of China(No.U2333210)the Sichuan Science and Technology Program,China(No.21SYSX0011)。
文摘Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.
基金supported by the Science Foundation of High-Level Talents of Wuyi University(2019AL017,2021AL002)。
文摘High-voltage Li metal batteries hold great promise for next-generation energy storage,but constructing robust and highly conductive electrode/electrolyte interfaces via electrolyte engineering to enhance the battery performance is still a challenge.Herein,we propose a non-coordinating solvent anchoring strategy to regulate fluorinated amide electrolyte to enhance the stability and ionic conductivity of the interfaces.Specifically,hexafluorobenzene is employed to anchor fluorinated amide solvent by the robust dipole–dipole interactions,which weaken the coordination between fluorinated amide and Li^(+),facilitate more anions coordinating with Li^(+),and form more ion aggregates.Consequently,stable and highly conductive electrode/electrolyte interfaces enriched with LiF and Li_(3)N are constructed,drastically improving the interfacial stability and reducing interface impedance of Li metal anodes and LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cathodes.Such a rationally designed electrolyte demonstrates excellent flame retardancy,high oxidation stability(5.1 V vs.Li^(+)/Li),and enhanced low-temperature ionic conductivity.As a result,this electrolyte substantially enhances the high-voltage cycle stability(-4.8 V),rate capability(-50 C)and low-temperature cycle performance(-20℃)of Li||NCM811 cells,which retain 80.0%of the initial capacity over 600 cycles at 4.7 V.This research offers a promising strategy to design ideal electrolytes for highperformance Li metal batteries.
文摘The poor oxidation stability of ether-based solvents has long been a major challenge limiting their practical application.To enhance the oxidative stability of ether-based electrolytes,the physicochemical properties of various glycol dimethyl ethers are screened,and diglyme(G2)is selected as the sole solvent for the electrolyte.Lithium bis(fluorosulfonyl)imide(LiFSI),a highly dissociative salt,is used as the primary salt;while lithium nitrate(LiNO_(3))and lithium difluorophosphate(LiDFP),which have small ionic sizes and strong binding energies,are added as secondary salts.The resulting electrolyte can modulate the electric double layer structure by NO_(3)^(-) and DFP^(-) on the cathode side,leading to an increased Liþconcentration that is originally repelled by the cathode.Additionally,the oxidation stability of the electrolyte is improved and the formed electrode-electrolyte interphase is more uniform and stable,thereby enhancing the electrochemical performance of the cells.As a result,cells assembled with a total of 1 M ternary lithium salts in G2 solvent can operate at high voltage of 4.4 V.The LijjNCM811 cells maintain 80.2%capacity retention after 270 cycles at room temperature,with an average Coulombic efficiency of 99.5%,and exhibit 88.4%capacity retention after 200 cycles at -30℃.
基金supported by the Beijing Municipal Natural Science Foundation(L223009)the National Natural Science Foundation of China(22209014,22479012)+1 种基金the Hebei Natural Science Foundation(E2024208084)the Fundamental Research Funds for the Central Universities(2023CX01031)。
文摘Sulfide-based all-solid-state lithium metal batteries(ASSLMBs)have garnered significant attention due to their potential for high energy density and enhanced safety.However,their practical application is hindered by challenges such as uneven lithium(Li)deposition and the growth of Li dendrites.In this contribution,we propose an amorphous fluorinated interphase(AFI),composed of amorphous LiF and lithiated graphite,to regulate the interfacial Li-ion transport kinetics through in-situ interface chemistry.Amorphous LiF,which exhibits a significantly enhanced Li-ion diffusion compared to its crystalline counterpart,works synergistically with lithiated graphite to promote both short-range and long-range Li-ion transport kinetics at the Li/electrolyte interface.As a result,the Li anode with AFI demonstrates a remarkably enhanced critical current density of 1.6 mA cm^(−2)and an extended cycle life exceeding 1100 h.The Li||LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)full cell also achieves a high discharge capacity of 125.7 mA h g^(−1)and retains 71.2%of its initial capacity after 200 cycles.This work provides valuable insights into the rational design of artificial anodic interphase to regulate interfacial Li-ion transport kinetics in ASSLMBs.
基金the financial supports from the KeyArea Research and Development Program of Guangdong Province (2020B090919001)the National Natural Science Foundation of China (22078144)the Guangdong Natural Science Foundation for Basic and Applied Basic Research (2021A1515010138 and 2023A1515010686)。
文摘Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.
基金financially supported by the National Natural Science Foundation of China(No.22078179)Taishan Scholar Foundation(No.tsqn201812063)。
文摘Fluorinated graphene has a promising application prospect in lithium primary batteries(LPBs)and sodium primary batteries(SPBs).Herein,five fluorinated graphene materials with different fluorine contents(FG-x)are prepared by a large-scale gas fluorination process.It is found that the structural characteristics of FG-x strongly depend on the fluorination temperature:the fluorine content(i.e.,F/C ratio)gradually increases with the fluorination temperature rising,resulting in the enlargement of interlayer spacing and the increase of average bonding strength between C and F.FG-0.75 sample with the intermediate degree of fluorination achieves the maximum energy densities in LPBs(2239.8 Wh·kg^(-1))and SPBs(1939.2 Wh·kg^(-1)).The interlayer distance is critical to the rate capability of FG-x,and FG-0.95 with the largest lattice spacing exhibits the best rate performance in both Li/CFx and Na/CFx batteries.The electrochemical reaction mechanism and the structural evolution of FG material revealed by ex situ X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD)characterization,and in situ Raman spectra further confirm the effect of interlayer distance.
基金funded by the National Key Research and Development Program of China(2022YFE0110500)National Natural Science Foundation of China(22376161,52373154,52103181)+1 种基金the Fundamental Research Funds for the Central Universities of Chinathe Interdisciplinary Project in Environmental Science and Engineering of Tongji University(2023-3-YB-02)。
文摘Fluorinated gases(F-gases)play a vital role in the chemical industry and in the fields of air conditioning,refrigeration,health care,and organic synthesis.However,the direct emission of waste gases containing F-gases into the atmosphere contributes to greenhouse effects and generates toxic substances.Developing porous materials for the energy-efficient capture,separation,and recovery of F-gases is highly desired.Recently,as a highly designable porous adsorbents,metal–organic frameworks(MOFs)exhibit excellent selective sorption performance toward F-gases,especially for the recognition and separation of different F-gases with highly similar properties,showing their great potential in F-gases control and recovery.In this review,we discuss the capture and separation of F-gases and their azeotropic,near-azeotropic,and isomeric mixtures in various application scenarios by MOFs,specifically classify and analyze molecular interaction between F-gases and MOFs,and interpret the mechanisms underlying their high performance regarding both adsorption capacity and selectivity,providing a repertoire for future materials design.Challenges faced in the transformation research roadmap of MOFs adsorbent separation technologies toward F-gases are also discussed,and areas for future research endeavors are highlighted.
基金This work is funded by National Natural Science Foundation of China(Grant No.52006115)Ministry of Science and Technology of China(Grant No.2019YFE0100200)+3 种基金National Natural Science Foundation of China(Grant No.52076121)China National Postdoctoral Program for Innovative Talents(Grant No.BX20190162)China Postdoctoral Science Foundation(Grant No.2019M660631)the Tsinghua University Initiative Scientific Research Program(Grant No.2019Z02UTY06).
文摘Fluorinated electrolytes possess good antioxidant capacity that provides high compatibility to high-voltage cathode and flame retardance;thus,they are considered as a promising solution for advanced lithium-ion batteries carrying both high-energy density and high safety.Moreover,the fluorinated electrolytes are widely used to form stable electrolyte interphase,due to their chemical reactivity with lithiated graphite or lithium.However,the influence of this reactivity on the thermal safety of batteries is seldom discussed.Herein,we demonstrate that the flame-retardant fluorinated electrolytes help to reduce the flammability,while the lithium-ion batteries with flame-retardant fluorinated electrolytes still undergo thermal runaway and disclose their different thermal runaway pathway from that of battery with conventional electrolyte.The reduction in fluorinated components(e.g.,LiPF 6 and fluoroethylene carbonate(FEC))by fully lithiated graphite accounts for a significant heat release during battery thermal runaway.The 13%of total heat is sufficient to trigger the chain reactions during battery thermal runaway.This study deepens the understanding of the thermal runaway mechanism of lithium-ion batteries employing flame-retardant fluorinated electrolytes,providing guidance on the concept of electrolyte design for safer lithium-ion batteries.
基金supported by the National Natural Science Foundation of China(No.12235006)the National Key Research and Development Program of China(No.2020YFE0202002.
文摘X-ray detectors show potential applications in medical imaging,materials science,and nuclear energy.To achieve high detection efficiency and spatial resolution,many conventional semiconductor materials,such as amorphous selenium,cadmium telluride zinc,and perovskites,have been utilized in direct conversion X-ray detectors.However,these semiconductor materials are susceptible to temperature-induced performance degradation,crystallization,delamination,uneven lattice growth,radiation damage,and high dark current.This study explores a new approach by coupling an FC40 electronic fluorinated liquid with a specialized high-resolution and high-readout-speed complementary metal-oxide-semiconductor(CMOS)pixel array,specifically the Topmetal II−chip,to fabricate a direct conversion X-ray detector.The fluorinated liquid FC40(molecular formula:C_(21)F_(48)N_(2))is an electronic medium that is minimally affected by temperature and displays no issues with uniform conductivity.It exhibits a low dark current and minimal radiation damage and enables customizable thickness in X-ray absorption.This addresses the limitations inherent in conventional semiconductor-based detectors.In this study,simple X-ray detector imaging tests were conducted,demonstrating the excellent coupling capability between FC40 electronic fluorinated liquid and CMOS chips by the X-ray detector.A spatial resolution of 4.0 lp/mm was measured using a striped line par card,and a relatively clear image of a cockroach was displayed in the digital radiography imaging results.Preliminary test results indicated the feasibility of fabricating an X-ray detector by combining FC40 electronic fluorinated liquid and CMOS chips.Owing to the absence of issues related to chip-material coupling,a high spatial resolution could be achieved by reducing the chip pixel size.This method presents a new avenue for studies on novel liquid-based direct conversion X-ray detectors.
基金support of National High Technology Research and Development Program of China ("863" Program) (2015AA034201)the National Natural Science Foundation of China (11234013 and 11264014)+1 种基金Natural Science Foundation of Jiangxi Province (20133ACB21010, 20142BAB212002,20132BAB212005)Foundation of Jiangxi Education Committee (GJJ14254 and KJLD14024)
文摘The structure evolution of fluorinated graphite （CFx） upon the Li/Na intercalation has been studied by first- principles calculations. The Li/Na adsorption on single CF layer and intercalated into bulk CF have been calculated. The better cycling performance of Na intercalation into the CF cathode, comparing to that of Li intercalation, is attributed to the different strength and characteristics of the Li-F and Na-F interactions. The interactions between Li and F are stronger and more localized than those between Na and E The strong and localized Coulomb attraction between Li and F atoms breaks the C-F bonds and pulls the F atoms away, and graphene sheets are formed upon Li intercalation.
基金supported by the National Natural Science Foundation of China(Nos.52072061,22322903,12174162)the Natural Science Foundation of Sichuan,China(No.2023NSFSC1914)21C Innovation Laboratory,Contemporary Amperex Technology Ltd.by project No.21C-OP-202103。
文摘Fluorinated carbons CF_xhold the highest theoretical energy density(e.g.,2180 W h kg^(-1)when x=1)among all cathode materials of lithium primary batteries.However,the low conductivity and severe polarization limit it to achieve its theory.In this study,we design a new electrolyte,namely 1 M LiBF_(4)DMSO:DOL(1:9 vol.),achieving a high energy density in Li/CF_xprimary cells.The DMSO with a small molecular size and high donor number successfully solvates Li^(+)into a defined Li^(+)-solvation structure.Such solvated Li^(+)can intercalate into the large-spacing carbon layers and achieve an improved capacity.Consequently,when discharged to 1.0 V,the CF_(1.12)cathode demonstrates a specific capacity of 1944 m A h g^(-1)with a specific energy density of 3793 W h kg^(-1).This strategy demonstrates that designing the electrolyte is powerful in improving the electrochemical performance of CF_(x) cathode.
文摘Ethyl acetate (EA) shows low viscosity for its relative permittivity. Monofluorinated organic solvents exert the polar effect on the various properties. We have investigated the effect of position isomerism on the physical and electrochemical properties of two monofluorinated carboxylates: 2-fluoroethyl acetate (2FEA) and ethyl fluoroacetate (EFA). Relative permittivity of 2FEA was lower than that of EFA, whereas viscosity of 2FEA was higher. Electrolytic conductivity of a LiPF6 solution in 2FEA was lower than that in EFA, but higher than that in EA at high temperatures. The use of 2FEA as a co-solvent improved cycling efficiency and suppressed fading of discharge capacity of a Li|LiCoO2 coin cell at high cycle numbers.
基金supported by the A*STAR MTC Programmatic Project(No.M23L9b0052)the Indonesia-NTU Singapore Institute of Research for Sustainability and Innovation(INSPIRASI)(No.6635/E3/KL.02.02/2023)+2 种基金the Singapore NRF Singapore-China Flagship Program(No.023740-00001)the National Natural Science Foundation of China(Nos.11975043 and 11475300)the China Scholarship Council(No.202306460087)。
文摘High-voltage solid-state lithium-ion batteries(SSLIBs)have attracted considerable research attention in recent years due to their high-energy-density and superior safety characteristics.However,the integration of high-voltage cathodes with solid electrolytes(SEs)presents multiple challenges,including the formation of high-impedance layers from spontaneous chemical reactions,electrochemical instability,insufficient interfacial contact,and lattice expansion.These issues significantly impair battery performance and potentially lead to battery failure,thus impeding the commercialization of high-voltage SSLIBs.The incorporation of fluorides,known for their robust bond strength and high free energy of formation,has emerged as an effective strategy to address these challenges.Fluorinated electrolytes and electrode/electrolyte interfaces have been demonstrated to significantly influence the reaction reversibility/kinetics,safety,and stability of rechargeable batteries,particularly under high voltage.This review summarizes recent advancements in fluorination treatment for high-voltage SEs,focusing on solid polymer electrolytes(SPEs),inorganic solid electrolytes(ISEs),and composite solid electrolytes(CSEs),along with the performance enhancements these strategies afford.This review aims to provide a comprehensive understanding of the structure-property relationships,the characteristics of fluorinated interfaces,and the application of fluorinated SEs in high-voltage SSLIBs.Further,the impacts of residual moisture and the challenges of fluorinated SEs are discussed.Finally,the review explores potential future directions for the development of fluorinated SSLIBs.
基金financially supported by the National Natural Science Foundation of China(No.52271084)the Guangdong Basic and Applied Basic Research Foundation,China(No.2021B1515020056)the Open Research Fund of Songshan Lake Materials Laboratory,China(No.2022SLABFK06)。
文摘To improve the friction and wear performance at room and elevated temperatures,Ti48Al2Nb2Cr(at.%)alloy was anodically fluorinated in an NH_(4)F-containing electrolyte.The effects of anodic fluorination on the friction coefficient,wear rate,wear track morphology,and adhesion strength between the oxide scale and substrate were investigated.Results showed that the in-situ formation of Al_(2)O_(3)-enriched oxide scale was promoted due to fluorine effect,by which the surface hardness and wear resistance were both enhanced.After the friction and wear test,no noticeable changes were found on the fluorinated Ti48Al2Nb2Cr,whilst severe abrasion was evident on the GCr15 counterpart.This indicates that anodic fluorination could effectively enhance the friction and wear performance of Ti48Al2Nb2Cr alloy.At elevated temperatures,the dominant wear mechanism of the fluorinated Ti48Al2Nb2Cr/GCr15 pair was oxidation wear and adhesive wear.
基金funded by the Opening Fund of Key Laboratory of Higher Education of Sichuan Province for Enterprise Informationalization and Internet of Things(No.2023WYJ06)the Yadong Wu Talent Program(No.H31225001)+1 种基金supported in part by the Defense Industrial Technology Development Program(No.JCKY2022404C001)by the Sichuan Provincial Key Lab of Process Equipment and Control’s Project(No.GK201509)。
文摘In the research and production of fluorinated materials,large volumes of unstructured textual data are generated,characterized by high heterogeneity and fragmentation.These issues hinder systematic knowledge integration and efficient utilization.Constructing a knowledge graph for fluorinated materials processing is essential for enabling structured knowledge management and intelligent applications.Among its core components,Named Entity Recognition(NER)plays an essential role,as its accuracy directly impacts relation extraction and semantic modeling,which ultimately affects the knowledge graph construction for fluorinated materials.However,NER in this domain faces challenges such as fuzzy entity boundaries,inconsistent terminology,and a lack of high-quality annotated corpora.To address these problems,(i)We first construct a domain-specific NER dataset by combining manual annotation with an improved Easy Data Augmentation(EDA)strategy;(ii)Secondly,we propose a novel model,RRC-ADV,which integrates RoBERTa-wwm for dynamic contextual word representation,adversarial training to improve robustness against boundary ambiguity,and a Residual BiLSTM(ResBiLSTM)to enhance sequential feature modeling.Further,a Conditional Random Field(CRF)layer is incorporated for globally optimized label prediction.Experimental results demonstrate that RRC-ADV achieves an average F1 score of 89.23%on the self-constructed dataset,significantly outperforming baseline models.The model exhibits strong robustness and adaptability within the domain of fluorinated materials.Our work enhances the accuracy of NER in the fluorinated materials processing domain and paves the way for downstream tasks such as relation extraction in knowledge graph construction.
基金supported by Natural Science Foundation of Shandong Province(No.ZR2022MB033)Science and Technology Bureau of Jinan City(No.2021GXRC105)University of Jinan Disciplinary Cross-Convergence Construction Project 2023(No.XKJC-202302)。
文摘The construction of monodisperse microporous organic microspheres is deemed a challenging issue,primarily due to the difficulty in achieving both high microporosity and uniformity within the microspheres.In this study,a series of fluorinated monodisperse microporous microspheres are fabricated by solvothermal precipitation polymerization.The resulting fluorous methacrylate-based microspheres achieved higher than 400 m^(2)/g surface area,along with a yield of over 90%for the microspheres.Through comprehensive characterization and simulation methods,we discovered that the introduction of fluorous methacrylate monomers at high loading levels is the key factor contributing to the formation of the microporosity within the microspheres.The controlled temperature profile was found to be advantageous for achieving a high yield of microspheres and increased uniformity.Two-dimensional assemblies of these fluorinated microsphere arrays exhibited superhydrophobicity,superolephilicity,and water sliding angles below 10°.Furthermore,a three-dimensional assembly of the fluorinated microporous microsphere in a chromatographic column demonstrated significant improvement in the separation of Engelhardt agent compared to commercial columns.Our work offers a novel approach to constructing fluorinated monodisperse microporous microspheres for advanced applications.
