In this study,fluorinating vaporization combined with ETV-ICP-AES technique was used to determine yttrium for which refractory carbide is easily formed.The absolute detection limit is 12 pg,and three-order magnitude o...In this study,fluorinating vaporization combined with ETV-ICP-AES technique was used to determine yttrium for which refractory carbide is easily formed.The absolute detection limit is 12 pg,and three-order magnitude of improvement is obtained in comparison with the conventional vaporization ETV-ICP-AES.No memory effect is observed.The relative standard deviation is better than 5%.Some factors affecting fluorinating vaporization,including matrix effect are discussed.This technique is applied to determine yttrium in La_2O_3.展开更多
Treatment of N-t-butylbenzenesulfonamide with an excess of BuLi, followed by the reaction with methyl 2-(4-methylphenyl)propanoate, gave the corresponding 2-carboxybenzenesulfonamide, which underwent a sequence of c...Treatment of N-t-butylbenzenesulfonamide with an excess of BuLi, followed by the reaction with methyl 2-(4-methylphenyl)propanoate, gave the corresponding 2-carboxybenzenesulfonamide, which underwent a sequence of consecutive N-deprotective cyclization process mediated by TMSCI-NaI-MeCN reagent to afford the N-sulfonylimine. Following the bromination and ring expansion, 3-methyl-3-(4-methylphenyl)-2H-benzo[e][1,2]thiazine-l,l,4-trione was obtained. Optical resolution of the racemic benzosultam using (-)-menthoxyacetyl chloride, furnished the optically p.ure (+)- and (-)-3-methyl-3-(4-methylphenyl)-2H- benzo[e][1,2]thiazine-1,1,4-triones, which were fluorinated with FC103 to produce the corresponding chiral N-F agents.展开更多
The presence of aluminum(Al^(3+))and fluoride(F^(−))ions in the environment can be harmful to ecosystems and human health,highlighting the need for accurate and efficient monitoring.In this paper,an innovative approac...The presence of aluminum(Al^(3+))and fluoride(F^(−))ions in the environment can be harmful to ecosystems and human health,highlighting the need for accurate and efficient monitoring.In this paper,an innovative approach is presented that leverages the power of machine learning to enhance the accuracy and efficiency of fluorescence-based detection for sequential quantitative analysis of aluminum(Al^(3+))and fluoride(F^(−))ions in aqueous solutions.The proposed method involves the synthesis of sulfur-functionalized carbon dots(C-dots)as fluorescence probes,with fluorescence enhancement upon interaction with Al^(3+)ions,achieving a detection limit of 4.2 nmol/L.Subsequently,in the presence of F^(−)ions,fluorescence is quenched,with a detection limit of 47.6 nmol/L.The fingerprints of fluorescence images are extracted using a cross-platform computer vision library in Python,followed by data preprocessing.Subsequently,the fingerprint data is subjected to cluster analysis using the K-means model from machine learning,and the average Silhouette Coefficient indicates excellent model performance.Finally,a regression analysis based on the principal component analysis method is employed to achieve more precise quantitative analysis of aluminum and fluoride ions.The results demonstrate that the developed model excels in terms of accuracy and sensitivity.This groundbreaking model not only showcases exceptional performance but also addresses the urgent need for effective environmental monitoring and risk assessment,making it a valuable tool for safeguarding our ecosystems and public health.展开更多
All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercializat...All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites.Elemental doping is an effective and direct method to enhance the performance of SEs.Here,we report an Al-F co-doping strategy to improve the overall properties including ion conductivity,high voltage stability,and cathode and anode compatibility.Particularly,the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases,thereby constructing a relatively stable interface and promoting uniform Li deposition.The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series.ASSLBs assembled with these optimized electrolytes gain good electrochemical performance,demonstrating the universality of Al-F co-doping towards advanced SEs.展开更多
Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. Ho...Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. However, such fascinating properties do not bring long-term cyclability of h-LMBs. One of critical challenges is the interface instability in contacting with the Li metal anode, as fiuorinated solvents are highly susceptible to exceptionally reductive metallic Li attributed to its low lowest unoccupied molecular orbital(LUMO), which leads to significant consumption of the fiuorinated components upon cycling.Herein, attenuating reductive decomposition of fiuorinated electrolytes is proposed to circumvent rapid electrolyte consumption. Specifically, the vinylene carbonate(VC) is selected to tame the reduction decomposition by preferentially forming protective layer on the Li anode. This work, experimentally and computationally, demonstrates the importance of pre-passivation of Li metal anodes at high voltage to attenuate the decomposition of fiuoroethylene carbonate(FEC). It is expected to enrich the understanding of how VC attenuate the reactivity of FEC, thereby extending the cycle life of fiuorinated electrolytes in high-voltage Li-metal 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
Practical application of Na3SbS4(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-s...Practical application of Na3SbS4(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-site doped Na_(3-2x)Sb_(1-x)W_(x)S_(4-x)F_(x)(x=0,0.12,0.24,0.36)electrolytes through high-energy ball milling followed by high-temperature sintering is prepared,where tungsten(W)substitutes for antimony(Sb)and fluorine(F)replaces sulfur(S)in the NSS lattice.The co-doping of W and F not only broadens the interplanar spacing of NSS but also promotes the stable formation of the cubic phase of NSS,thereby effectively enhancing the transport ability of sodium ions within NSS.Among them,Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24) exhibits the highest ionic conductivity of 4.45 mS·cm^(-1).Furthermore,F doping facilitates the in-situ formation of NaF between the electrolyte and metallic sodium,significantly improving interfacial stability.Electrochemical evaluation shows that the Na/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na symmetric cell achieves a high critical current density of 1.65 mA·cm^(-2) and maintains stable sodium plating/stripping cycling for 500 h at 0.1 mA·cm^(-2).Additionally,the TiS2/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na full cell exhibits outstanding cycling stability and rate capability.展开更多
Fluorine(F)-enriched soils,resulting from geogenic processes or superimposed by anthropogenic activities,have raised significant concerns due to their phytotoxicity and potential threats to human health.Soils in centr...Fluorine(F)-enriched soils,resulting from geogenic processes or superimposed by anthropogenic activities,have raised significant concerns due to their phytotoxicity and potential threats to human health.Soils in central Guizhou Province exhibit F enrichment,with a mean F concentration of 1067 mg/kg.However,the associated human health risks and geochemical mechanisms driving F enrichment in these soils remain insufficiently understood.In areas with a natural geological background,the average concentrations of F in rice,vegetables,drinking water,and ambient air are 1.54 mg/kg,0.54 mg/kg,0.16 mg/L,and 0.29μg/m^(3),respectively.In contrast,samples collected near phosphorous chemical plants demonstrate elevated F concentrations:1.78 mg/kg in rice,1.53 mg/kg in vegetables,0.20 mg/L in drinking water,and 11.98μg/m^(3) in ambient air.Fluorine in soils was immobilized by apatite and clay minerals,and hardly transferred into water and crops.The fixation of F-by Ca^(2+)in water and by Fe/Al hydroxides and clay minerals in bottom sediment further reduces F concentrations in water.As a result,hazard quotient(HQ)values below 1.0 indicate negligible fluorine-related health risk in geological background regions.However,ambient air near phosphorous chemical plant exhibited a 41.3-fold increase in F concentration compared to geological background regions.Fluorine-laden emissions can be directly inhaled or deposited on vegetable leaves and orally ingested into human bodies.Improvement of F-rich waste gas disposal and restricted leafy vegetable cultivation are effective measures to reduce F health risks in phosphorous chemical plant regions.展开更多
The direct preparation of a kind of fluorinating reagent 1[F-TEDA-N(SO_(2)Ph)_(2)]was realized in high yield via the complexation of N-fluorobenzenesulfonimide(NFSI)with 1-(chloromethyl)-1,4-diazabicyclo[2.2.2]octan-1...The direct preparation of a kind of fluorinating reagent 1[F-TEDA-N(SO_(2)Ph)_(2)]was realized in high yield via the complexation of N-fluorobenzenesulfonimide(NFSI)with 1-(chloromethyl)-1,4-diazabicyclo[2.2.2]octan-1-ium N',N'-bis-(benzenesulfonylimide)salt.In its fluorination to oxindoles,the fluorinating products 6 were afforded in moderate to high yields.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
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
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
Chemically engineered extracts represent a promising source of new bioactive semi-synthetic molecules.Prepared through direct derivatization of natural extracts,they can include constituents enriched with elements and...Chemically engineered extracts represent a promising source of new bioactive semi-synthetic molecules.Prepared through direct derivatization of natural extracts,they can include constituents enriched with elements and sub-structures that are less common in natural products compared to drugs.Fourteen such extracts were prepared through sequential reactions with hydrazine and a fluorinating reagent,and their α-glucosidase inhibition properties were compared.For the most bioactive mixture,a chemically modified propolis extract,enzyme inhibition increased 22 times due to the reaction sequence.Bio-guided fractionation led to the isolation of a new fluorinated pyrazole produced within the extract by chemical transformation of the flavonoid chrysin.The inhibitor results from the action of the two reagents used on four common functional groups present in natural products(carbonyl,phenol,aromatic carbon,and a double bond).The reactions led to the opening of a 6-member oxygenated heterocycle to produce a 5-member nitrogenated one,as well as the dehydroxylation and fluorination in two different positions of one of the aromatic rings of the natural starting material,all within a complex mixture of natural products.Overall,these transformations led to an approximately 20-fold increase in the α-glucosidase inhibition by the isolated inhibitor compared to its natural precursor.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
It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible d...It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible display technologies.Herein,a series of fluorinated polyimide films(FPIs)were fabricated by the condensation of 5,5′-(perfluoropropane-2,2-diyl)bis(isobenzofuran-1,3-dione)(6FDA)and the fluorinated triphenylmethane diamine monomer(EDA,MEDA and DMEDA)with heat-crosslinkable tetrafluorostyrene side groups,which was incorporated by different numbers of methyl groups pendant in the ortho position of amino groups.Subsequently,the FPI films underwent heating to produce crosslinking FPIs(C-FPIs)through the self-crosslinking of double bonds in the tetrafluorostyrene.The transparency,solvent resistance,thermal stability,mechanical robustness and dielectric properties of FPI and C-FPI films can be tuned by the number of methyl groups and crosslinking,which were deeply investigated by virtue of molecular dynamics(MD)simulations and density functional theory(DFT).As a result,all the films exhibited exceptional optically colorless and transparent,with transmittance in the visible region of 450-700 nm exceeding 79.9%,and the cut-off wavelengths(λ_(off))were nearly 350 nm.The thermal decomposition temperatures at 5% weight loss(T_(d5%))for all samples exceeded 504℃.These films exhibited a wide range of tunable tensile strength(46.5-75.1 MPa).Significantly,they showed exceptional dielectric properties with the dielectric constant of 2.3-2.5 at full frequency(10^(7)-20 Hz).This study not only highlights the relationship between the polymer molecular structure and properties,but offer insights for balancing optical transparency,heat resistance and low dielectric constant in PI films.展开更多
Fluorination is a critical surface modification technique for enhancing the electrical performance of composite insulators.This study employs molecular simulations to examine the microstructure and space charge behavi...Fluorination is a critical surface modification technique for enhancing the electrical performance of composite insulators.This study employs molecular simulations to examine the microstructure and space charge behavior of fluorinated and non-fluorinated silicone rubber under an electric field,with experimental validation.The results show that fluorinated silicone rubber exhibits lower total energy,higher polarization,and stronger dipole moments compared to its non-fluorinated counterpart,shifting the material from an insulating to a conductive state.Under lower electric field strengths,the carbon-silicon bonds in fluorinated silicone rubber are longer,but it maintains geometric stability under higher fields.The energy gap changes across different fluorination modes and varies with electric field strength,indicating that fluorination affects conductivity differently at various field intensities.Both fluorination methods improve conductivity in the 0–3.8 V/nm range,with substitutional fluorination showing superior performance between 3.8 and 8.9 V/nm.Above 9.1 V/nm,fluorination maximizes conductivity.The fluorinated samples exhibit a greater redshift at higher electric fields,resulting in enhanced conductivity and improved surface charge distribution.These findings offer insights into the microscopic effects of fluorination on silicone rubber’s electrical properties,while experiments confirm that fluorination increases hydrophobicity and boosts DC flashover voltage,further enhancing the material’s performance.展开更多
In the present study,we investigated the influence of surface fluorine(F)on TiO_(2)for the photocatalytic oxidation(PCO)of toluene.TiO_(2)modified with different F content was prepared and tested.It was found that wit...In the present study,we investigated the influence of surface fluorine(F)on TiO_(2)for the photocatalytic oxidation(PCO)of toluene.TiO_(2)modified with different F content was prepared and tested.It was found that with the increasing of F content,the toluene conversion rate first increased and then decreased.However,CO_(2)mineralization efficiency showed the opposite trend.Based on the characterizations,we revealed that F substitutes the surface hydroxyl of TiO_(2)to form the structure of≡Ti-F.The presence of the appropriate amount of surface≡Ti-F on TiO_(2)greatly enhanced the separation of photogenerated carriers,which facilitated the generation of·OH and promoted the activity for the PCO of toluene.It was further revealed that the increase of only·OH promoted the conversion of toluene to ring-containing intermediates,causing the accumulation of intermediates and then conversely inhibited the·OH generation,which led to the decrease of the CO_(2)mineralization efficiency.The above results could provide guidance for the rational design of photocatalysts for toluene oxidation.展开更多
To advance the application of layered oxide cathodes in fast-charging sodium-ion batteries,it is crucial to not only suppress irreversible phase transitions but also improve the rate capability of cathode materials an...To advance the application of layered oxide cathodes in fast-charging sodium-ion batteries,it is crucial to not only suppress irreversible phase transitions but also improve the rate capability of cathode materials and optimize Na^(+)diffusion kinetics to ensure high capacity output at various charge-discharge rates.In this research,the targeted F-substitution with a heavy ratio in oxygen anion layer optimizes the Na^(+)diffusion path and electronic conductivity of the material,thereby decreasing the Na^(+)diffusion barrier and imparting high-rate performance.At a 20 C rate,the cathode achieves a capacity of over 80 mAh g^(-1)with stable cycling performance.Additionally,the dual rivet effect between the transition metal layer and oxygen layer prevents significant phase transitions during charge/discharge within the 2-4.2 V range for the modified cathode.As a result,the F-substituted oxygen anion layer improved Na^(+)diffusion,electronic conductivity,and crystal plane structure stability,which led to the development of a highperformance,fast-charging sodium-ion battery(SIB),opening new avenues for commercial applications.展开更多
Rate coefficients of the gas-phase reactions of Cl atoms with a series of fluorinated diketones(FDKs):CF_(3)C(O)CH_(2)C(O)CH_(3)(TFP),CF_(3)C(O)CH_(2)C(O)CH_(2)CH_(3)(TFH)and CF_(3)C(O)CH_(2)C(O)CH(CH_(3))2(TFMH),have...Rate coefficients of the gas-phase reactions of Cl atoms with a series of fluorinated diketones(FDKs):CF_(3)C(O)CH_(2)C(O)CH_(3)(TFP),CF_(3)C(O)CH_(2)C(O)CH_(2)CH_(3)(TFH)and CF_(3)C(O)CH_(2)C(O)CH(CH_(3))2(TFMH),have been measured at(298±2)K and under atmospheric pressure.The experiments were performed using the relative-rate method with a GC-FID detection system.From different determinations and references used,the following rate coefficients were obtained(in cm3/(molecule·sec)):k_(4)(TFP+Cl)=(1.75±0.21)×10^(−10),k_(5)(TFH+Cl)=(2.05±0.23)×10^(−10),k_(6)(TFMH+Cl)=(2.71±0.34)×10^(−10).Reactivity trends of FDKs were discussed and Free Energy Relationships analysis was developed.The expression lgkOH=1.68 lgkCl+5.71 was obtained for the reactivity of the studied FDKs together with similar unsaturated VOCs with Cl and OH radicals Additionally,acetic acid(CH_(3)C(O)OH)and trifluoroacetic acid(CF_(3)C(O)OH)were positively identified and quantified as degradation products using in situ FTIR spectroscopy.According to the identified products,atmospheric chemical mechanisms were proposed.The atmospheric implications of the studied reactions were assessed by the estimation of the tropospheric lifetimes of TFP,TFH,and TFMH concerning their reaction with Cl atoms to be 48,41,and 31 hours,respectively.The relatively short residence in the atmosphere of the fluorocarbons studied will have a local/regional impact with restricted transport.Global warming potential(GWP(20 yr))calculated for the studied fluoro diketones were 0.014,0.003 and 0.001 for TFP,TFH and TFMH,respectively with a negligible contribution to the greenhouse effect.展开更多
Ferroelectrics(FEs)have shown great potential in sensors,actuators,and electrocaloric cooling due to their direct cross-couplings between electric polarization and mechanical,thermal,and dielectric properties[1−3]Comp...Ferroelectrics(FEs)have shown great potential in sensors,actuators,and electrocaloric cooling due to their direct cross-couplings between electric polarization and mechanical,thermal,and dielectric properties[1−3]Compared with oxide FEs,polymer FEs possess good flexible and shape adaptability,making them promising candidates for flexible electronics and biocompatible devices[4].展开更多
文摘In this study,fluorinating vaporization combined with ETV-ICP-AES technique was used to determine yttrium for which refractory carbide is easily formed.The absolute detection limit is 12 pg,and three-order magnitude of improvement is obtained in comparison with the conventional vaporization ETV-ICP-AES.No memory effect is observed.The relative standard deviation is better than 5%.Some factors affecting fluorinating vaporization,including matrix effect are discussed.This technique is applied to determine yttrium in La_2O_3.
基金the Scientific Research Foundation for the Returned Oversea Chinese Scholars of Shandong University.
文摘Treatment of N-t-butylbenzenesulfonamide with an excess of BuLi, followed by the reaction with methyl 2-(4-methylphenyl)propanoate, gave the corresponding 2-carboxybenzenesulfonamide, which underwent a sequence of consecutive N-deprotective cyclization process mediated by TMSCI-NaI-MeCN reagent to afford the N-sulfonylimine. Following the bromination and ring expansion, 3-methyl-3-(4-methylphenyl)-2H-benzo[e][1,2]thiazine-l,l,4-trione was obtained. Optical resolution of the racemic benzosultam using (-)-menthoxyacetyl chloride, furnished the optically p.ure (+)- and (-)-3-methyl-3-(4-methylphenyl)-2H- benzo[e][1,2]thiazine-1,1,4-triones, which were fluorinated with FC103 to produce the corresponding chiral N-F agents.
基金supported by the National Natural Science Foundation of China(No.U21A20290)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515011656)+2 种基金the Projects of Talents Recruitment of GDUPT(No.2023rcyj1003)the 2022“Sail Plan”Project of Maoming Green Chemical Industry Research Institute(No.MMGCIRI2022YFJH-Y-024)Maoming Science and Technology Project(No.2023382).
文摘The presence of aluminum(Al^(3+))and fluoride(F^(−))ions in the environment can be harmful to ecosystems and human health,highlighting the need for accurate and efficient monitoring.In this paper,an innovative approach is presented that leverages the power of machine learning to enhance the accuracy and efficiency of fluorescence-based detection for sequential quantitative analysis of aluminum(Al^(3+))and fluoride(F^(−))ions in aqueous solutions.The proposed method involves the synthesis of sulfur-functionalized carbon dots(C-dots)as fluorescence probes,with fluorescence enhancement upon interaction with Al^(3+)ions,achieving a detection limit of 4.2 nmol/L.Subsequently,in the presence of F^(−)ions,fluorescence is quenched,with a detection limit of 47.6 nmol/L.The fingerprints of fluorescence images are extracted using a cross-platform computer vision library in Python,followed by data preprocessing.Subsequently,the fingerprint data is subjected to cluster analysis using the K-means model from machine learning,and the average Silhouette Coefficient indicates excellent model performance.Finally,a regression analysis based on the principal component analysis method is employed to achieve more precise quantitative analysis of aluminum and fluoride ions.The results demonstrate that the developed model excels in terms of accuracy and sensitivity.This groundbreaking model not only showcases exceptional performance but also addresses the urgent need for effective environmental monitoring and risk assessment,making it a valuable tool for safeguarding our ecosystems and public health.
基金supported by the National Natural Science Foundation of China(Nos.52172243,52371215)。
文摘All-solid-state Li batteries(ASSLBs)using solid electrolytes(SEs)have gained significant attention in recent years considering the safety issue and their high energy density.Despite these advantages,the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites.Elemental doping is an effective and direct method to enhance the performance of SEs.Here,we report an Al-F co-doping strategy to improve the overall properties including ion conductivity,high voltage stability,and cathode and anode compatibility.Particularly,the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases,thereby constructing a relatively stable interface and promoting uniform Li deposition.The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series.ASSLBs assembled with these optimized electrolytes gain good electrochemical performance,demonstrating the universality of Al-F co-doping towards advanced SEs.
基金supported by the National Natural Science Foundation of China (Nos. 22379121, 62005216)Basic Public Welfare Research Program of Zhejiang (No. LQ22F050013)+1 种基金Zhejiang Province Key Laboratory of Flexible Electronics Open Fund (2023FE005)Shenzhen Foundation Research Program (No. JCYJ20220530112812028)。
文摘Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. However, such fascinating properties do not bring long-term cyclability of h-LMBs. One of critical challenges is the interface instability in contacting with the Li metal anode, as fiuorinated solvents are highly susceptible to exceptionally reductive metallic Li attributed to its low lowest unoccupied molecular orbital(LUMO), which leads to significant consumption of the fiuorinated components upon cycling.Herein, attenuating reductive decomposition of fiuorinated electrolytes is proposed to circumvent rapid electrolyte consumption. Specifically, the vinylene carbonate(VC) is selected to tame the reduction decomposition by preferentially forming protective layer on the Li anode. This work, experimentally and computationally, demonstrates the importance of pre-passivation of Li metal anodes at high voltage to attenuate the decomposition of fiuoroethylene carbonate(FEC). It is expected to enrich the understanding of how VC attenuate the reactivity of FEC, thereby extending the cycle life of fiuorinated electrolytes in high-voltage Li-metal 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.
文摘Practical application of Na3SbS4(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-site doped Na_(3-2x)Sb_(1-x)W_(x)S_(4-x)F_(x)(x=0,0.12,0.24,0.36)electrolytes through high-energy ball milling followed by high-temperature sintering is prepared,where tungsten(W)substitutes for antimony(Sb)and fluorine(F)replaces sulfur(S)in the NSS lattice.The co-doping of W and F not only broadens the interplanar spacing of NSS but also promotes the stable formation of the cubic phase of NSS,thereby effectively enhancing the transport ability of sodium ions within NSS.Among them,Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24) exhibits the highest ionic conductivity of 4.45 mS·cm^(-1).Furthermore,F doping facilitates the in-situ formation of NaF between the electrolyte and metallic sodium,significantly improving interfacial stability.Electrochemical evaluation shows that the Na/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na symmetric cell achieves a high critical current density of 1.65 mA·cm^(-2) and maintains stable sodium plating/stripping cycling for 500 h at 0.1 mA·cm^(-2).Additionally,the TiS2/Na_(2.52)Sb|_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na full cell exhibits outstanding cycling stability and rate capability.
基金supported by the projects of the China Geological Survey(DD20230543,DD20221770).
文摘Fluorine(F)-enriched soils,resulting from geogenic processes or superimposed by anthropogenic activities,have raised significant concerns due to their phytotoxicity and potential threats to human health.Soils in central Guizhou Province exhibit F enrichment,with a mean F concentration of 1067 mg/kg.However,the associated human health risks and geochemical mechanisms driving F enrichment in these soils remain insufficiently understood.In areas with a natural geological background,the average concentrations of F in rice,vegetables,drinking water,and ambient air are 1.54 mg/kg,0.54 mg/kg,0.16 mg/L,and 0.29μg/m^(3),respectively.In contrast,samples collected near phosphorous chemical plants demonstrate elevated F concentrations:1.78 mg/kg in rice,1.53 mg/kg in vegetables,0.20 mg/L in drinking water,and 11.98μg/m^(3) in ambient air.Fluorine in soils was immobilized by apatite and clay minerals,and hardly transferred into water and crops.The fixation of F-by Ca^(2+)in water and by Fe/Al hydroxides and clay minerals in bottom sediment further reduces F concentrations in water.As a result,hazard quotient(HQ)values below 1.0 indicate negligible fluorine-related health risk in geological background regions.However,ambient air near phosphorous chemical plant exhibited a 41.3-fold increase in F concentration compared to geological background regions.Fluorine-laden emissions can be directly inhaled or deposited on vegetable leaves and orally ingested into human bodies.Improvement of F-rich waste gas disposal and restricted leafy vegetable cultivation are effective measures to reduce F health risks in phosphorous chemical plant regions.
基金the National Natural Science Foundation of China(No.21372077)for their financial supports.
文摘The direct preparation of a kind of fluorinating reagent 1[F-TEDA-N(SO_(2)Ph)_(2)]was realized in high yield via the complexation of N-fluorobenzenesulfonimide(NFSI)with 1-(chloromethyl)-1,4-diazabicyclo[2.2.2]octan-1-ium N',N'-bis-(benzenesulfonylimide)salt.In its fluorination to oxindoles,the fluorinating products 6 were afforded in moderate to high yields.
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.
基金support by Universidad Nacional de Rosario(80020180300114UR and 80020180100128UR)CONICET(PIP No 11220200102423)FONCYT(PICT2019-02232 and PICT2021-1034)for the development of this work.
文摘Chemically engineered extracts represent a promising source of new bioactive semi-synthetic molecules.Prepared through direct derivatization of natural extracts,they can include constituents enriched with elements and sub-structures that are less common in natural products compared to drugs.Fourteen such extracts were prepared through sequential reactions with hydrazine and a fluorinating reagent,and their α-glucosidase inhibition properties were compared.For the most bioactive mixture,a chemically modified propolis extract,enzyme inhibition increased 22 times due to the reaction sequence.Bio-guided fractionation led to the isolation of a new fluorinated pyrazole produced within the extract by chemical transformation of the flavonoid chrysin.The inhibitor results from the action of the two reagents used on four common functional groups present in natural products(carbonyl,phenol,aromatic carbon,and a double bond).The reactions led to the opening of a 6-member oxygenated heterocycle to produce a 5-member nitrogenated one,as well as the dehydroxylation and fluorination in two different positions of one of the aromatic rings of the natural starting material,all within a complex mixture of natural products.Overall,these transformations led to an approximately 20-fold increase in the α-glucosidase inhibition by the isolated inhibitor compared to its natural precursor.
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financially supported by the Natural Science Foundation of Shandong Province(Nos.ZR2021ME055,ZR2022QB170 and ZR2022MB034)the Foundation(No.GZKF202128)of State Key Laboratory of Biobased Material and Green Papermaking,Qilu University of Technology,Shandong Academy of Sciencesthe Development Program Project of Young Innovation Team of Institutions of Higher Learning in Shandong Province.
文摘It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible display technologies.Herein,a series of fluorinated polyimide films(FPIs)were fabricated by the condensation of 5,5′-(perfluoropropane-2,2-diyl)bis(isobenzofuran-1,3-dione)(6FDA)and the fluorinated triphenylmethane diamine monomer(EDA,MEDA and DMEDA)with heat-crosslinkable tetrafluorostyrene side groups,which was incorporated by different numbers of methyl groups pendant in the ortho position of amino groups.Subsequently,the FPI films underwent heating to produce crosslinking FPIs(C-FPIs)through the self-crosslinking of double bonds in the tetrafluorostyrene.The transparency,solvent resistance,thermal stability,mechanical robustness and dielectric properties of FPI and C-FPI films can be tuned by the number of methyl groups and crosslinking,which were deeply investigated by virtue of molecular dynamics(MD)simulations and density functional theory(DFT).As a result,all the films exhibited exceptional optically colorless and transparent,with transmittance in the visible region of 450-700 nm exceeding 79.9%,and the cut-off wavelengths(λ_(off))were nearly 350 nm.The thermal decomposition temperatures at 5% weight loss(T_(d5%))for all samples exceeded 504℃.These films exhibited a wide range of tunable tensile strength(46.5-75.1 MPa).Significantly,they showed exceptional dielectric properties with the dielectric constant of 2.3-2.5 at full frequency(10^(7)-20 Hz).This study not only highlights the relationship between the polymer molecular structure and properties,but offer insights for balancing optical transparency,heat resistance and low dielectric constant in PI films.
基金supported in part by the National Natural Science Foundation of China under Grant 52277139 and 52367014in part by the Guangxi Science Fund for Distinguished Young Scholars under Grant 2024GXNSFFA999017.
文摘Fluorination is a critical surface modification technique for enhancing the electrical performance of composite insulators.This study employs molecular simulations to examine the microstructure and space charge behavior of fluorinated and non-fluorinated silicone rubber under an electric field,with experimental validation.The results show that fluorinated silicone rubber exhibits lower total energy,higher polarization,and stronger dipole moments compared to its non-fluorinated counterpart,shifting the material from an insulating to a conductive state.Under lower electric field strengths,the carbon-silicon bonds in fluorinated silicone rubber are longer,but it maintains geometric stability under higher fields.The energy gap changes across different fluorination modes and varies with electric field strength,indicating that fluorination affects conductivity differently at various field intensities.Both fluorination methods improve conductivity in the 0–3.8 V/nm range,with substitutional fluorination showing superior performance between 3.8 and 8.9 V/nm.Above 9.1 V/nm,fluorination maximizes conductivity.The fluorinated samples exhibit a greater redshift at higher electric fields,resulting in enhanced conductivity and improved surface charge distribution.These findings offer insights into the microscopic effects of fluorination on silicone rubber’s electrical properties,while experiments confirm that fluorination increases hydrophobicity and boosts DC flashover voltage,further enhancing the material’s performance.
基金supported by the National Natural Science Foundation of China(Nos.21976196,22276204).
文摘In the present study,we investigated the influence of surface fluorine(F)on TiO_(2)for the photocatalytic oxidation(PCO)of toluene.TiO_(2)modified with different F content was prepared and tested.It was found that with the increasing of F content,the toluene conversion rate first increased and then decreased.However,CO_(2)mineralization efficiency showed the opposite trend.Based on the characterizations,we revealed that F substitutes the surface hydroxyl of TiO_(2)to form the structure of≡Ti-F.The presence of the appropriate amount of surface≡Ti-F on TiO_(2)greatly enhanced the separation of photogenerated carriers,which facilitated the generation of·OH and promoted the activity for the PCO of toluene.It was further revealed that the increase of only·OH promoted the conversion of toluene to ring-containing intermediates,causing the accumulation of intermediates and then conversely inhibited the·OH generation,which led to the decrease of the CO_(2)mineralization efficiency.The above results could provide guidance for the rational design of photocatalysts for toluene oxidation.
基金supported by the National Natural Science Foundation of China(Nos.22178221,22208221)the Shenzhen Science and Technology Program(Nos.JCYJ20220818095805012,JCYJ20230808105109019)+2 种基金the Natural Science Foundation of Guangdong Province(Nos.2024A1515011078,2024A1515011507)the Scientific Foundation for Youth Scholars of Shenzhen University(868-000001032522,827-0001004)the Instrumental Analysis Center of Shenzhen University for the assistance with the Electron Microscope technical support。
文摘To advance the application of layered oxide cathodes in fast-charging sodium-ion batteries,it is crucial to not only suppress irreversible phase transitions but also improve the rate capability of cathode materials and optimize Na^(+)diffusion kinetics to ensure high capacity output at various charge-discharge rates.In this research,the targeted F-substitution with a heavy ratio in oxygen anion layer optimizes the Na^(+)diffusion path and electronic conductivity of the material,thereby decreasing the Na^(+)diffusion barrier and imparting high-rate performance.At a 20 C rate,the cathode achieves a capacity of over 80 mAh g^(-1)with stable cycling performance.Additionally,the dual rivet effect between the transition metal layer and oxygen layer prevents significant phase transitions during charge/discharge within the 2-4.2 V range for the modified cathode.As a result,the F-substituted oxygen anion layer improved Na^(+)diffusion,electronic conductivity,and crystal plane structure stability,which led to the development of a highperformance,fast-charging sodium-ion battery(SIB),opening new avenues for commercial applications.
文摘Rate coefficients of the gas-phase reactions of Cl atoms with a series of fluorinated diketones(FDKs):CF_(3)C(O)CH_(2)C(O)CH_(3)(TFP),CF_(3)C(O)CH_(2)C(O)CH_(2)CH_(3)(TFH)and CF_(3)C(O)CH_(2)C(O)CH(CH_(3))2(TFMH),have been measured at(298±2)K and under atmospheric pressure.The experiments were performed using the relative-rate method with a GC-FID detection system.From different determinations and references used,the following rate coefficients were obtained(in cm3/(molecule·sec)):k_(4)(TFP+Cl)=(1.75±0.21)×10^(−10),k_(5)(TFH+Cl)=(2.05±0.23)×10^(−10),k_(6)(TFMH+Cl)=(2.71±0.34)×10^(−10).Reactivity trends of FDKs were discussed and Free Energy Relationships analysis was developed.The expression lgkOH=1.68 lgkCl+5.71 was obtained for the reactivity of the studied FDKs together with similar unsaturated VOCs with Cl and OH radicals Additionally,acetic acid(CH_(3)C(O)OH)and trifluoroacetic acid(CF_(3)C(O)OH)were positively identified and quantified as degradation products using in situ FTIR spectroscopy.According to the identified products,atmospheric chemical mechanisms were proposed.The atmospheric implications of the studied reactions were assessed by the estimation of the tropospheric lifetimes of TFP,TFH,and TFMH concerning their reaction with Cl atoms to be 48,41,and 31 hours,respectively.The relatively short residence in the atmosphere of the fluorocarbons studied will have a local/regional impact with restricted transport.Global warming potential(GWP(20 yr))calculated for the studied fluoro diketones were 0.014,0.003 and 0.001 for TFP,TFH and TFMH,respectively with a negligible contribution to the greenhouse effect.
基金support from the Natural Science Fund for Colleges and Universities in Jiangsu Province(24KJB430029)the Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(NY224032,NY225006).
文摘Ferroelectrics(FEs)have shown great potential in sensors,actuators,and electrocaloric cooling due to their direct cross-couplings between electric polarization and mechanical,thermal,and dielectric properties[1−3]Compared with oxide FEs,polymer FEs possess good flexible and shape adaptability,making them promising candidates for flexible electronics and biocompatible devices[4].