Compared to subtractive manufacturing and casting,3D printing(additive manufacturing)offers advantages,such as the rapid production of complex structures,reduced material waste,and environmental friendliness.Direct in...Compared to subtractive manufacturing and casting,3D printing(additive manufacturing)offers advantages,such as the rapid production of complex structures,reduced material waste,and environmental friendliness.Direct ink writing(DIW)is one of the most popular 3D printing techniques owing to its ability to print multiple materials simultaneously and its high compatibility with printing inks.However,DIW presents significant challenges,particularly in the printing of high-performance polymers.The main challenges are as follows:1.The rigid structures and reaction kinetics of high-performance polymers make developing new inks difficult.2.The limited types of available high-performance polymers underscore the need for new DIW-suitable materials.3.Layer-by-layer stacking weakens interlayer bonding,affecting the mechanical properties of the printed product.4.The accuracy and speed of DIW printing are insufficient for large-scale manufacturing.After introducing the topic,the requirements for DIW printing inks are first reviewed,emphasizing the importance of thixotropic agents.Then,research progress regarding DIW printing of high-performance polymers is comprehensively reviewed according to the requirements of different polymer inks.Additionally,the applications of these materials across various fields are summarized.Finally,the challenges in DIW printing of high-performance polymers,along with corresponding solutions and future development prospects,are discussed in detail.展开更多
Di(4-bromophenyl)ketone and various aromatic diamines as the monomers,a series of novel poly(imino ketone)s (PIKs)have been synthesized via palladium-catalyzed aryl amination,which is Hartwig-Buchwald polycondensation...Di(4-bromophenyl)ketone and various aromatic diamines as the monomers,a series of novel poly(imino ketone)s (PIKs)have been synthesized via palladium-catalyzed aryl amination,which is Hartwig-Buchwald polycondensation reaction.The structures of PIKs are characterized by means of elemental analysis,FT-IR,~1H-NMR and UV-Vis spectroscopy. The results show a good agreement with the proposed structure.The general properties of PIKs are studied by DSC,TG and wide-angle X-ray diffraction,the solubility behavior is...展开更多
CONSPECTUS:Lignocellulosic biomass is an ideal feedstock for the next generation of sustainable,high-performance,polymeric materials.Although lignin is a highly available and low-cost source of natural aromatics,it is...CONSPECTUS:Lignocellulosic biomass is an ideal feedstock for the next generation of sustainable,high-performance,polymeric materials.Although lignin is a highly available and low-cost source of natural aromatics,it is commonly burned for heat or disposed of as waste.The use of lignin for new materials introduces both challenges and opportunities with respect to incumbent petrochemical-based compounds.These considerations are derived from two fundamental aspects of lignin:its recalcitrant/heterogeneous nature and aromatic methoxy substituents.展开更多
A low-cost 1D cobalt-based coordination polymer(CP)[Co(BGPD)(DMSO)_(2)(H_(2)O)_(2)](Co-BD;H2BGPD=N,N'-bis(glycinyl)pyromellitic diimide;DMSO=dimethyl sulfoxide)was synthesized by a simple method,and its crystal st...A low-cost 1D cobalt-based coordination polymer(CP)[Co(BGPD)(DMSO)_(2)(H_(2)O)_(2)](Co-BD;H2BGPD=N,N'-bis(glycinyl)pyromellitic diimide;DMSO=dimethyl sulfoxide)was synthesized by a simple method,and its crystal structure was characterized.In a three-electrode system,Co-BD,as the electrode material for supercapacitors,achieved a specific capacitance of 830 F·g^(-1)at 1 A·g^(-1),equivalent to a specific capacity of 116.4 mAh·g^(-1),and exhibited high-rate capability,reaching 212 F·g^(-1)at 20 A·g^(-1).Impressively,Co-BD||rGO(reduced graphene oxide),representing an asymmetrical supercapacitor,owns a higher energy density of 14.2 Wh·kg^(-1)at 0.80 kW·kg^(-1),and an excellent cycle performance(After 4000 cycles at 1 A·g^(-1),the capacitance retention was up to 94%).CCDC:2418872.展开更多
The practical application of poly(ethylene oxide)(PEO)-based solid polymer electrolytes in all-solid-state lithium-metal batteries(ASSLBs)still suffers from persistent challenges associated with low ionic conductivity...The practical application of poly(ethylene oxide)(PEO)-based solid polymer electrolytes in all-solid-state lithium-metal batteries(ASSLBs)still suffers from persistent challenges associated with low ionic conductivity and poor oxidative stability.To address these issues,we introduce a novel in-situ ionization strategy using radical polymer poly(2,2,6,6-tetramethyl-1-piperidinyloxy-4-yl acrylate)(PTPA)to enhance ionic conductivity and achieve a high electrochemical stability window in PEO-based electrolyte.Density functional theory(DFT)calculations and molecular dynamics(MD)simulations reveal that the in-situ generation of PTPA+from PTPA within the battery,not only exceptionally decreases the low Highest Occupied Molecular Orbital(HOMO)energy level,but also exhibits a robust anchoring effect on TFSI-anions in the electrolyte,which boosts Li^(+) migration and enables dense Li deposition behavior.As a result,the PEO/10 wt%PTPA/LiTFSI electrolyte demonstrates remarkable oxidative stability up to 5 V and a high Li^(+)transference number(0.57).Li-Li symmetric cells maintain stability over 1000 h at 0.2 mA cm^(-2),and LiFePO_(4)(LFP)//Li battery also presents an enduring cyclic performance over 500 cycles with a remarkable high-capacity retention of 91.8% at 0.5C.Impressively,by coupling with a high-voltage LiCoO_(2)(LCO)cathode(cut-off voltage 4.6 V),the assembled ASSLBs reach a capacity retention of 87.1% after 500 cycles at 1C.Our study explores the mechanism of radical polymer in PEO-based electrolyte and provides a fire-new strategy for construction of high-performance and multifunctional ASSLBs.展开更多
Quasi-solid-state composite electrolytes(QSCEs)show promise for high-performance solid-state batteries,while they still struggle with interfacial stability and cycling performance.Herein,a F-grafted QSCE(F-QSCE)was de...Quasi-solid-state composite electrolytes(QSCEs)show promise for high-performance solid-state batteries,while they still struggle with interfacial stability and cycling performance.Herein,a F-grafted QSCE(F-QSCE)was developed via copolymerizing the F monomers and ionic liquid monomers.The F-QSCE demonstrates better overall performance,such as high ionic conductivity of 1.21 mS cm^(-1)at 25℃,wide electrochemical windows of 5.20 V,and stable cycling stability for Li//Li symmetric cells over 4000 h.This is attributed to the significant electronegativity difference between C and F in the fluorinated chain(-CF_(2)-CF-CF_(3)),which causes the electron cloud to shift toward the F atom,surrounding it with a negative charge and producing the inductive effect.Furthermore,the interactions between Li^(+)and F,TFSI~-,and C are enhanced,reducing ion pair aggregation(Li^(+)-TFSI~--Li^(+))and promoting Li^(+)transport.Besides,-CF_(2)-CF-CF_(3)decomposes to form Li F preferentially over TFSI~-,resulting in better interfacial stability for F-QSCE.This work provides a pathway to enable the development of high-performance Li metal batteries.展开更多
One effective approach to strike the balance between ionic conductivity and mechanical strength in polymer electrolytes involves the design of a coupled polymer molecular structure comprising both rigid and flexible p...One effective approach to strike the balance between ionic conductivity and mechanical strength in polymer electrolytes involves the design of a coupled polymer molecular structure comprising both rigid and flexible phases.Nevertheless,the regulation of intermolecular interactions between plasticizers and rigid and flexible phases has been largely overlooked.Here,an intermolecular interaction engineering strategy is carried out with well-chosen dual-plasticize within qua si-sol id-state polymer electrolytes(QSPEs).Succinonitrile exhibits a stronger affinity towards rigid phase hydrogenated nitrile butadiene rubber(HNBR),while propene carbonate demonstrates a stronger affinity towards flexible segments poly(propylene carbonate)(PPC).This tailored intermolecular interaction engineering allows for differential plasticization of the polymer's rigid and flexible phases,thereby achieving a balance between ionic conductivity and mechanical strength.The QSPE have both higher ionic conductivity(1.04×10^(-4)S cm^(-1)at 30℃),t_(Li+)(0.55),and tensile strength(0.76 MPa).Li//Li symmetric cells maintaining performance over1100 h at 0.1 mA cm^(-2)and Li//LiFePO_(4)cells retaining 85.0%capacity after 700 cycles at 1.0 C.It is a unique angle to employ intermolecular interaction engineering in QSPEs through dual-plasticizer approach combined with CO_(2)-based polymer materials.This sustainable strategy combining dual-plasticizer engineering with CO_(2)-based polymers,offers insights for designing high-performance,eco-friendly lithium metal batteries.展开更多
Sodium-sulfur(Na-S)batteries are believed as the hopeful energy storage and conversion techniques owing to the high specific capacity and low cost.Nevertheless,unstable sodium(Na)deposition/stripping of Na metal anode...Sodium-sulfur(Na-S)batteries are believed as the hopeful energy storage and conversion techniques owing to the high specific capacity and low cost.Nevertheless,unstable sodium(Na)deposition/stripping of Na metal anode,low intrinsic conductivity of sulfur cathode,and severe shuttling effect of sodium polysulfides(NaPSs)pose significant challenges in the actual reversible capacity and cycle life of Na-S batteries.Herein,a self-supporting electrode made of nitrogen-doped carbon fiber embedded with cobalt nanoparticles(Co/NC-CF)is designed to load sulfur.Meanwhile,gel polymer electrolyte(GPE)with high ion transfer ability is obtained by in-situ polymerization inside the battery.During the polymerization process,an integrated electrode-electrolyte and a continuous ion-electron conduction network in a composite cathode are constructed inside the Na-S battery.It is noteworthy that the designed GPE demonstrates superior ionic conductivity and effective adsorption of NaPSs that can significantly suppress the shuttle effect.Leveraging the synergistic interplay between the designed GPE and self-supporting cathode,the assembled quasi-solid-state(QSS)Na-S battery exhibits great cycling stability.These experimental results are further corroborated by COMSOL Multiphysics simulations and density functional theory(DFT)calculations,which mechanistically validate the enhanced electrochemical performance.The findings of this study offer new and promising perspectives for advancing the development of nextgeneration solid-state batteries.展开更多
Solid-state polymer electrolytes are crucial for advancing solid-state lithium-metal batteries owing to their flexibility,excellent manufacturability,and strong interfacial compatibility.However,their widespread appli...Solid-state polymer electrolytes are crucial for advancing solid-state lithium-metal batteries owing to their flexibility,excellent manufacturability,and strong interfacial compatibility.However,their widespread applications are hindered by low ionic conductivity at room temperature and lithium dendrite growth.Herein,we report a novel solid-state composite membrane electrolyte design that combines the vertically aligned channel structure and copolymer with a radial gradient composition.Within the vertically aligned channels,the composition of poly(vinyl ethylene carbonate-co-poly(ethylene glycol)diacrylate)(P(VEC-PEGDA)varies in a gradient along the radial direction:from the center to the wall of vertically aligned channels,the proportion of vinyl ethylene carbonate(VEC)in the copolymer decreases,while the proportion of poly(ethylene glycol)diacrylate(PEGDA)increases accordingly.It can be functionally divided into a mechanical-reinforcement layer and a fast-ion-conducting layer.The resulting solid-state composite membrane electrolyte achieves a high critical current density of 1.2 mA cm^(-2)and high ionic conductivity of 2.03 mS cm^(-1)at room temperature.Employing this composite membrane electrolyte,a Li//Li symmetric cell exhibits stable cycling for over 1850 h at 0.2 m A cm^(-2)/0.2 m A h cm^(-2),and a Li//LiFePO4(LFP)battery maintains 77.3% capacity retention at 2 C after 300 cycles.Our work provides insight into the rational design of safer and more efficient solidstate batteries through electrolyte structural engineering.展开更多
This work focuses on the development of high temperature polymer electrolyte membranes(HT-PEMs)as key materials for HT-PEM fuel cells(HT-PEMFCs).Recognizing the challenges associated with the phosphoric acid(PA) doped...This work focuses on the development of high temperature polymer electrolyte membranes(HT-PEMs)as key materials for HT-PEM fuel cells(HT-PEMFCs).Recognizing the challenges associated with the phosphoric acid(PA) doped polybenzimidazole(PBI) membranes,including the use of carcinogenic monomers and complex synthesis procedures,this study aims to develop more cost-effective,readily synthesized,and high-performance alternatives.A series of superacid-catalyzed polyhydroxyalkylation reactions have been carefully designed between p-terphenyl and aldehydes bearing imidazole moieties,resulting in a new class of HT-PEMs.It is found that the chemical structure of aldehyde-substituted N-heterocycles significantly impacts the polymerization reaction.Specifically,the use of 1-methyl-2-imidazole-formaldehyde and 1 H-imidazole-4-formaldehyde monomers leads to the formation of high-viscosity,rigid,and ether-free polymers,denoted as PTIm-a and PTIm-b.Membranes fabricated from these polymers,due to their pendent imidazole groups,exhibit an exceptional capacity for PA absorption.Notably,PTIm-a,carrying methylimidazole moieties,demonstrates a superior chemical stability by maintaining morphology and structural stability during 350 h of Fenton testing.After being immersed in 75 wt% PA at 40℃,the PTIm-a membrane reaches a PA content of 152%,maintains a good tensile strength of 13.6 MPa,and exhibits a moderate conductivity of 50.2 mS cm^(-1) at 180℃.Under H_(2)/O_(2) operational conditions,a single cell based on the PTIm-a membrane attains a peak power density of 732 mW cm^(-2) at 180℃ without backpressure.Furthermore,the membrane demonstrates stable cycle stability over 173 h within 18 days at a current density of 200 mA cm^(-2),indicating its potential for practical application in HT-PEMFCs.This work highlights innovative strategies for the synthesis of advanced HT-PEMs,offering significant improvements in membrane properties and fuel cell performance,thus expanding the horizons of HT-PEMFC technology.展开更多
Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(te...Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(terphenyl piperidinium)s constructed from the m-and p-isomers of terphenyl were synthesized to regulate the microstructure of the membrane.Highly rigid p-terphenyl units prompt the formation of moderate PA aggregates,where the ion-pair interaction between piperidinium and biphosphate is reinforced,leading to a reduction in the plasticizing effect.As a result,there are trade-offs between the proton conductivity,mechanical strength,and PA retention of the membranes with varied m/p-isomer ratios.The designed PA-doped PTP-20m membrane exhibits superior ionic conductivity,good mechanical strength,and excellent PA retention over a wide range of temperature(80–160°C)as well as satisfactory resistance to harsh accelerated aging tests.As a result,the membrane presents a desirable combination of performance(1.462 W cm^(-2) under the H_(2)/O_(2)condition,which is 1.5 times higher than that of PBI-based membrane)and durability(300 h at 160°C and 0.2 A cm^(-2))in the fuel cell.The results of this study provide new insights that will guide molecular design from the perspective of microstructure to improve the performance and robustness of HT-PEMs.展开更多
Herein,an external crosslinker facilitated the hypercrosslinking of ferrocene and a nitrogen heterocyclic compound(either melamine or imidazole)through a direct Friedel-Crafts reaction,which led to the formation of ni...Herein,an external crosslinker facilitated the hypercrosslinking of ferrocene and a nitrogen heterocyclic compound(either melamine or imidazole)through a direct Friedel-Crafts reaction,which led to the formation of nitrogen-containing hypercrosslinked fer-rocene polymer precursors(HCP-FCs).Subsequent carbonization of these precursors results in the production of iron-nitrogen-doped por-ous carbon absorbers(Fe-NPCs).The Fe-NPCs demonstrate a porous structure comprising aggregated nanotubes and nanospheres.The porosity of this structure can be modulated by adjusting the iron and nitrogen contents to optimize impedance matching.The uniform dis-tribution of Fe-N_(x)C,N dipoles,andα-Fe within the carbon matrix can be ensured by using hypercrosslinked ferrocenes in constructing porous carbon,providing the absorber with numerous polarization sites and a conductive network.The electromagnetic wave absorption performance of the specially designed Fe-NPC-M_(2)absorbers is satisfactory,revealing a minimum reflection loss of-55.3 dB at 2.5 mm and an effective absorption bandwidth of 6.00 GHz at 2.0 mm.By utilizing hypercrosslinked polymers(HCPs)as precursors,a novel method for developing highly efficient carbon-based absorbing agents is introduced in this research.展开更多
Cholesteric liquid crystals(CLCs)exhibit unique helical superstructures that selectively reflect circularly polarized light,enabling them to dynamically respond to environmental changes with tunable structural colors....Cholesteric liquid crystals(CLCs)exhibit unique helical superstructures that selectively reflect circularly polarized light,enabling them to dynamically respond to environmental changes with tunable structural colors.This dynamic color-changing capability is crucial for applications that require adaptable optical properties,positioning CLCs as key materials in advanced photonic technologies.This review focuses on the mechanisms of dynamic color tuning in CLCs across various forms,including small molecules,cholesteric liquid crystal elastomers(CLCEs),and cholesteric liquid crystal networks(CLCNs),and emphasizes the distinct responsive coloration each structure provides.Key developments in photochromic mechanisms based on azobenzene,dithienylethene,and molecular motor switches,are discussed for their roles in enhancing the stability and tuning range of CLCs.We examine the color-changing behaviors of CLCEs under mechanical stimuli and CLCNs under swelling,highlighting the advantages of each form.Following this,applications of dynamic color-tuning CLCs in information encryption,adaptive camouflage,and smart sensing technologies are explored.The review concludes with an outlook on current challenges and future directions in CLC research,particularly in biomimetic systems and dynamic photonic devices,aiming to broaden their functional applications and impact.展开更多
As a typical bioflavonoid,diosmetin is desirable in the field of natural medicine,healthy food,and cosmetics by anti-cancer,antibacterial,antioxidant,estrogen-like and anti-inflammatory activities,and it comes from a ...As a typical bioflavonoid,diosmetin is desirable in the field of natural medicine,healthy food,and cosmetics by anti-cancer,antibacterial,antioxidant,estrogen-like and anti-inflammatory activities,and it comes from a wide range of sources in traditional Chinese medicine like spider fragrance,spearmint and chrysanthemum,as well as in Citrus fruit.However,traditional analytical methods such as silica gel column chromatography face multiple challenges in the selective extraction of diosmetin from biological materials and traditional Chinese medicinal materials.Therefore,it is urgent to develop a new type of absorbent with high efficiency,recyclability and good specificity to diosmetin.In this investigation,a magnetic surface molecularly imprinted polymer(labeled as Diosmetin/SMIPs)was synthesized employing magnetic nanoparticles as the carrier and 4-vinylpyridinyl(4-VP)as the functional monomer by surface imprinting technology.The functional monomer was screened by the binding energy(△E)between functional monomers and template molecules via computational simulation.The Diosmetin/SMIPs had a high level of specific recognition and adsorption capability towards diosmetin with a 20.25 mg g^(-1) adsorption capacity and an imprinting factor(IF)of 2.28.Additionally,it demonstrated excellent regeneration performance with 8 adsorption/desorption cycles.In addition,91.20%-94.16% of spiked diosmetin was recovered from the lemon peel samples.The strategy of constructing Diosmetin/SMIPs based on computational simulation can effectively enhance the specific adsorption performance of diosmetin.Meanwhile,Diosmetin/SMIPs synthesized by imprinting polymerization showed excellent anti-interference and reusability,and realized efficient targeted extraction of diosmetin from lemon peel samples.The results of this investigation provide a promising adsorbent for selective enrichment of diosmetin from Citrus fruit and complicated materials.展开更多
In recent years,smart materials have emerged as a groundbreaking innovation in the field of water filtration,offering sustainable,efficient,and environmentally friendly solutions to address the growing global water cr...In recent years,smart materials have emerged as a groundbreaking innovation in the field of water filtration,offering sustainable,efficient,and environmentally friendly solutions to address the growing global water crisis.This review explores the latest advancements in the application of smart materials—including biomaterials,nanocomposites,and stimuli-responsive polymers—specifically for water treatment.It examines their effectiveness in detecting and removing various types of pollutants,including organic contaminants,heavy metals,and microbial infections,while adapting to dynamic environmental conditions such as fluctuations in temperature,pH,and pressure.The review highlights the remarkable versatility of these materials,emphasizing their multifunctionality,which allows them to address a wide range of water quality issues with high efficiency and low environmental impact.Moreover,it explores the potential of smart materials to overcome significant challenges in water purification,such as the need for real-time pollutant detection and targeted removal processes.The research also discusses the scalability and future development of these materials,considering their cost-effectiveness and potential for large-scale application.By aligning with the principles of sustainable development,smart materials represent a promising direction for ensuring global water security,offering both innovative solutions for current water pollution issues and long-term benefits for the environment and public health.展开更多
We report five coordination polymers(CPs)based on fluorescent ligands[1,6-di(1H-imidazol-1-yl)pyrene(dip),9,10-di(1H-imidazol-1-yl)anthracene(dia)]and anionic ligands[cyclohexane-1,4-dicarboxylic acid(H_(2)cda),campho...We report five coordination polymers(CPs)based on fluorescent ligands[1,6-di(1H-imidazol-1-yl)pyrene(dip),9,10-di(1H-imidazol-1-yl)anthracene(dia)]and anionic ligands[cyclohexane-1,4-dicarboxylic acid(H_(2)cda),camphoric acid(H_(2)cpa)].In[Cd(dip)(cda)]·4H_(2)O}_(n)(1),the Cd^(2+)ions,acting as tetrahedral nodes,are linked by dipand cda^(2-)ligands with four Cd^(2+)ions into five-fold interpenetrating network array of topology of dia.In{[Cd(dip)(cpa)]·4H_(2)O}_(n)(2),the Cd^(2+)ions,acting as a 4-connector,are linked by cpa^(2-)and dip ligands into a 3D framework ofcds topology.In{[Ni(dia)_(2)Cl_(2)]·DMF}_(n)(3),the Ni^(2+)ion is linked by four dia ligands into a layer structure,and 1Dchannels of a cross-section of 1.35 nm×0.96 nm are formed.In{[Cd(dia)_(2)(H_(2)O)_(2)](NO_(3))_(2)·2DMSO}n(4),the dia ligandsconnected Cd^(2+)ions into a 2D layer,and 1D channels are formed between adjacent layers with a cross-section of0.87 nm×0.43 nm.In[Zn(dip)Cl_(2)]_(n)(5),the Zn^(2+)ion is linked by dip ligands into an infinite 1D chain.The infrared,thermal gravimetric,and fluorescent emission data were collected and analyzed for these coordination polymers.CCDC:2356055,1;2440075,2;2356057,3;2356057,4;2356059,5.展开更多
Six coordination polymers based on 9,10-di(pyridine-4-yl)-anthracene(DPA)and 1,6-di(1H-imidazol-1-yl)pyrene(DIP)were obtained by solvothermal reactions.{[Zn(DPA)Cl_(2)]·DMF·2H_(2)O}n(1)and{[Zn_(1.5)(DPA)_(1....Six coordination polymers based on 9,10-di(pyridine-4-yl)-anthracene(DPA)and 1,6-di(1H-imidazol-1-yl)pyrene(DIP)were obtained by solvothermal reactions.{[Zn(DPA)Cl_(2)]·DMF·2H_(2)O}n(1)and{[Zn_(1.5)(DPA)_(1.5)Cl_(3)]·5H_(2)O}n(2)are framework isomers,which both contain zigzag chains formed by DPA,Zn^(2+),and Cl-.The zigzag chains in 1 are further assembled by C—H…Cl interactions into layers,and these layers exhibit two different orientations,displaying a rare 2D to 3D interpenetration mode.The zigzag chains in 2 are parallelly arranged.{[Zn_(3)(DPA)_(3)Br_(6)]·2DMF·_(1.5)H_(2)O}n(3)is isostructural to 2.3 was obtained using ZnBr_(2)instead of ZnCl_(2).[M(DPA)(formate)_(2)(H_(2)O)_(2)]n[M=Co(4),Cu(5)]are isostructural,contain chain structures formed by DPA,Cu^(2+)/Co^(2+),and for-mate ions,which were formed in situ in the solvothermal reaction.{[Zn(DIP)_(2)Cl]ClO_(4)}n(6)contains a layer structure formed by DIP and Zn^(2+).Free DPA and DIP ligands exhibited high fluorescence at room temperature,and coordina-tion polymers 3 and 6 displayed enhanced fluorescent emissions.展开更多
Tactile perception plays a vital role for the human body and is also highly desired for smart prosthesis and advanced robots.Compared to active sensing devices,passive piezoelectric and triboelectric tactile sensors c...Tactile perception plays a vital role for the human body and is also highly desired for smart prosthesis and advanced robots.Compared to active sensing devices,passive piezoelectric and triboelectric tactile sensors consume less power,but lack the capability to resolve static stimuli.Here,we address this issue by utilizing the unique polarization chemistry of conjugated polymers for the first time and propose a new type of bioinspired,passive,and bio-friendly tactile sensors for resolving both static and dynamic stimuli.Specifically,to emulate the polarization process of natural sensory cells,conjugated polymers(including poly(3,4-ethylenedioxythiophen e):poly(styrenesulfonate),polyaniline,or polypyrrole)are controllably polarized into two opposite states to create artificial potential differences.The controllable and reversible polarization process of the conjugated polymers is fully in situ characterized.Then,a micro-structured ionic electrolyte is employed to imitate the natural ion channels and to encode external touch stimulations into the variation in potential difference outputs.Compared with the currently existing tactile sensing devices,the developed tactile sensors feature distinct characteristics including fully organic composition,high sensitivity(up to 773 mV N^(−1)),ultralow power consumption(nW),as well as superior bio-friendliness.As demonstrations,both single point tactile perception(surface texture perception and material property perception)and two-dimensional tactile recognitions(shape or profile perception)with high accuracy are successfully realized using self-defined machine learning algorithms.This tactile sensing concept innovation based on the polarization chemistry of conjugated polymers opens up a new path to create robotic tactile sensors and prosthetic electronic skins.展开更多
Two new Mn(Ⅱ)coordination polymers,namely{[Mn_(2)(HL)(phen)_(3)(H_(2)O)_(2)]·7.5H_(2)O}_n(1)and[Mn_(4)(HL)_(2)(1,4-bib)_(3)(H_(2)O)_(2)]_n(2),were synthesized under hydrothermal conditions by using Mn(Ⅱ)ions an...Two new Mn(Ⅱ)coordination polymers,namely{[Mn_(2)(HL)(phen)_(3)(H_(2)O)_(2)]·7.5H_(2)O}_n(1)and[Mn_(4)(HL)_(2)(1,4-bib)_(3)(H_(2)O)_(2)]_n(2),were synthesized under hydrothermal conditions by using Mn(Ⅱ)ions and 6-(3',4'-dicarboxylphenoxy)-1,2,4-benzenetricarboxylic acid(H_(5)L)in the presence of N-auxiliary ligands 1,10-phenanthroline(phen)and1,4-bis(1H-imidazol-1-yl)benzene(1,4-bib).The structures of coordination polymers 1 and 2 were characterized by infrared spectroscopy,single-crystal X-ray diffraction,thermogravimetric analysis,and powder X-ray diffraction.Single-crystal X-ray diffraction reveals that 1 has a 1D chain structure based on binuclear Mn(Ⅱ)units,while 2 features a(3,8)-connected 3D network structure based on tetranuclear Mn(Ⅱ)units.Magnetic studies show that 1 and 2exhibit antiferromagnetic interactions between manganese ions.2 shows stronger antiferromagnetic interactions due to the shorter Mn…Mn distances within the tetranuclear manganese units.CCDC:2357601,1;2357602,2.展开更多
Mixed matrix membranes(MMMs)have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers.However,achieving a sim...Mixed matrix membranes(MMMs)have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers.However,achieving a simultaneous enhancement of permeability and selectivity remains a formidable challenge,due to the difficulty of achieving an optimal match between polymers and fillers.In this study,we incorporate a porous carbon-based zinc oxide composite(C@ZnO)into high-permeability polymers of intrinsic microporosity(PIMs)to fabricate MMMs.The dipole–dipole interaction between C@ZnO and PIMs ensures their exceptional compatibility,mitigating the formation of non-selective voids in the resulting MMMs.Concurrently,C@ZnO with abundant interconnected pores can provide additional low-resistance pathways for gas transport in MMMs.As a result,the CO_(2) permeability of the optimized C@ZnO/PIM-1 MMMs is elevated to 13,215 barrer,while the CO_(2)/N_(2) and CO_(2)/CH_(4) selectivity reached 21.5 and 14.4,respectively,substantially surpassing the 2008 Robeson upper bound.Additionally,molecular simulation results further corroborate that the augmented membrane gas selectivity is attributed to the superior CO_(2) affinity of C@ZnO.In summary,we believe that this work not only expands the application of MMMs for gas separation but also heralds a paradigm shift in the application of porous carbon materials.展开更多
基金supported by National Key Research and Development Program of China(Grant No.2022YFB3809000)Major Science and Technology Project of Gansu Province(Grant No.23ZDGA011)+1 种基金National Natural Science Foundation of China(Grant No.22275199,52105224)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB04701022021).
文摘Compared to subtractive manufacturing and casting,3D printing(additive manufacturing)offers advantages,such as the rapid production of complex structures,reduced material waste,and environmental friendliness.Direct ink writing(DIW)is one of the most popular 3D printing techniques owing to its ability to print multiple materials simultaneously and its high compatibility with printing inks.However,DIW presents significant challenges,particularly in the printing of high-performance polymers.The main challenges are as follows:1.The rigid structures and reaction kinetics of high-performance polymers make developing new inks difficult.2.The limited types of available high-performance polymers underscore the need for new DIW-suitable materials.3.Layer-by-layer stacking weakens interlayer bonding,affecting the mechanical properties of the printed product.4.The accuracy and speed of DIW printing are insufficient for large-scale manufacturing.After introducing the topic,the requirements for DIW printing inks are first reviewed,emphasizing the importance of thixotropic agents.Then,research progress regarding DIW printing of high-performance polymers is comprehensively reviewed according to the requirements of different polymer inks.Additionally,the applications of these materials across various fields are summarized.Finally,the challenges in DIW printing of high-performance polymers,along with corresponding solutions and future development prospects,are discussed in detail.
基金This work was financially supported by the National Natural Science Foundation of China(No.15076017).
文摘Di(4-bromophenyl)ketone and various aromatic diamines as the monomers,a series of novel poly(imino ketone)s (PIKs)have been synthesized via palladium-catalyzed aryl amination,which is Hartwig-Buchwald polycondensation reaction.The structures of PIKs are characterized by means of elemental analysis,FT-IR,~1H-NMR and UV-Vis spectroscopy. The results show a good agreement with the proposed structure.The general properties of PIKs are studied by DSC,TG and wide-angle X-ray diffraction,the solubility behavior is...
基金the Army Research Office under Cooperative Agreement Number W911NF-22-2-0257the National Science Foundation(NSF)Growing Convergence Research program(NSF GCR CMMI 1934887)in Materials Life Cycle Management for financial support during the writing of this manuscript.
文摘CONSPECTUS:Lignocellulosic biomass is an ideal feedstock for the next generation of sustainable,high-performance,polymeric materials.Although lignin is a highly available and low-cost source of natural aromatics,it is commonly burned for heat or disposed of as waste.The use of lignin for new materials introduces both challenges and opportunities with respect to incumbent petrochemical-based compounds.These considerations are derived from two fundamental aspects of lignin:its recalcitrant/heterogeneous nature and aromatic methoxy substituents.
文摘A low-cost 1D cobalt-based coordination polymer(CP)[Co(BGPD)(DMSO)_(2)(H_(2)O)_(2)](Co-BD;H2BGPD=N,N'-bis(glycinyl)pyromellitic diimide;DMSO=dimethyl sulfoxide)was synthesized by a simple method,and its crystal structure was characterized.In a three-electrode system,Co-BD,as the electrode material for supercapacitors,achieved a specific capacitance of 830 F·g^(-1)at 1 A·g^(-1),equivalent to a specific capacity of 116.4 mAh·g^(-1),and exhibited high-rate capability,reaching 212 F·g^(-1)at 20 A·g^(-1).Impressively,Co-BD||rGO(reduced graphene oxide),representing an asymmetrical supercapacitor,owns a higher energy density of 14.2 Wh·kg^(-1)at 0.80 kW·kg^(-1),and an excellent cycle performance(After 4000 cycles at 1 A·g^(-1),the capacitance retention was up to 94%).CCDC:2418872.
基金supported by the National Natural Science Foundation of China(51973236,51573213)Zhuhai Industry University-Research Cooperation Program(2320004002721)。
文摘The practical application of poly(ethylene oxide)(PEO)-based solid polymer electrolytes in all-solid-state lithium-metal batteries(ASSLBs)still suffers from persistent challenges associated with low ionic conductivity and poor oxidative stability.To address these issues,we introduce a novel in-situ ionization strategy using radical polymer poly(2,2,6,6-tetramethyl-1-piperidinyloxy-4-yl acrylate)(PTPA)to enhance ionic conductivity and achieve a high electrochemical stability window in PEO-based electrolyte.Density functional theory(DFT)calculations and molecular dynamics(MD)simulations reveal that the in-situ generation of PTPA+from PTPA within the battery,not only exceptionally decreases the low Highest Occupied Molecular Orbital(HOMO)energy level,but also exhibits a robust anchoring effect on TFSI-anions in the electrolyte,which boosts Li^(+) migration and enables dense Li deposition behavior.As a result,the PEO/10 wt%PTPA/LiTFSI electrolyte demonstrates remarkable oxidative stability up to 5 V and a high Li^(+)transference number(0.57).Li-Li symmetric cells maintain stability over 1000 h at 0.2 mA cm^(-2),and LiFePO_(4)(LFP)//Li battery also presents an enduring cyclic performance over 500 cycles with a remarkable high-capacity retention of 91.8% at 0.5C.Impressively,by coupling with a high-voltage LiCoO_(2)(LCO)cathode(cut-off voltage 4.6 V),the assembled ASSLBs reach a capacity retention of 87.1% after 500 cycles at 1C.Our study explores the mechanism of radical polymer in PEO-based electrolyte and provides a fire-new strategy for construction of high-performance and multifunctional ASSLBs.
基金conducted in a project within M-ERA.NET 3 with support from the European Union’s Horizon 2020 research,innovation program under grant agreement No.958174,Vinnova(Swedish Governmental Agency for Innovation Systems)the financial support from the LTU CREATERNITY program+1 种基金the J.Gust Richert Foundationthe National Natural Science Foundation of China(No.U23A20122)。
文摘Quasi-solid-state composite electrolytes(QSCEs)show promise for high-performance solid-state batteries,while they still struggle with interfacial stability and cycling performance.Herein,a F-grafted QSCE(F-QSCE)was developed via copolymerizing the F monomers and ionic liquid monomers.The F-QSCE demonstrates better overall performance,such as high ionic conductivity of 1.21 mS cm^(-1)at 25℃,wide electrochemical windows of 5.20 V,and stable cycling stability for Li//Li symmetric cells over 4000 h.This is attributed to the significant electronegativity difference between C and F in the fluorinated chain(-CF_(2)-CF-CF_(3)),which causes the electron cloud to shift toward the F atom,surrounding it with a negative charge and producing the inductive effect.Furthermore,the interactions between Li^(+)and F,TFSI~-,and C are enhanced,reducing ion pair aggregation(Li^(+)-TFSI~--Li^(+))and promoting Li^(+)transport.Besides,-CF_(2)-CF-CF_(3)decomposes to form Li F preferentially over TFSI~-,resulting in better interfacial stability for F-QSCE.This work provides a pathway to enable the development of high-performance Li metal batteries.
基金supported by the National Key Research and Development Program(2019YFA0705701)National Natural Science Foundation of China(22075329,22008267,21978332 and 22179149)+1 种基金Research and Development Project of Henan Academy Sciences China(232018002)Guangdong Basic and Applied Basic Research Foundation(2021A1515010731)。
文摘One effective approach to strike the balance between ionic conductivity and mechanical strength in polymer electrolytes involves the design of a coupled polymer molecular structure comprising both rigid and flexible phases.Nevertheless,the regulation of intermolecular interactions between plasticizers and rigid and flexible phases has been largely overlooked.Here,an intermolecular interaction engineering strategy is carried out with well-chosen dual-plasticize within qua si-sol id-state polymer electrolytes(QSPEs).Succinonitrile exhibits a stronger affinity towards rigid phase hydrogenated nitrile butadiene rubber(HNBR),while propene carbonate demonstrates a stronger affinity towards flexible segments poly(propylene carbonate)(PPC).This tailored intermolecular interaction engineering allows for differential plasticization of the polymer's rigid and flexible phases,thereby achieving a balance between ionic conductivity and mechanical strength.The QSPE have both higher ionic conductivity(1.04×10^(-4)S cm^(-1)at 30℃),t_(Li+)(0.55),and tensile strength(0.76 MPa).Li//Li symmetric cells maintaining performance over1100 h at 0.1 mA cm^(-2)and Li//LiFePO_(4)cells retaining 85.0%capacity after 700 cycles at 1.0 C.It is a unique angle to employ intermolecular interaction engineering in QSPEs through dual-plasticizer approach combined with CO_(2)-based polymer materials.This sustainable strategy combining dual-plasticizer engineering with CO_(2)-based polymers,offers insights for designing high-performance,eco-friendly lithium metal batteries.
基金supported by the National Natural Science Foundation of China(No.52130101)the Project of Science and Technology Development Plan of Jilin Province in China(Nos.20210402058GH and 20220201114GX)。
文摘Sodium-sulfur(Na-S)batteries are believed as the hopeful energy storage and conversion techniques owing to the high specific capacity and low cost.Nevertheless,unstable sodium(Na)deposition/stripping of Na metal anode,low intrinsic conductivity of sulfur cathode,and severe shuttling effect of sodium polysulfides(NaPSs)pose significant challenges in the actual reversible capacity and cycle life of Na-S batteries.Herein,a self-supporting electrode made of nitrogen-doped carbon fiber embedded with cobalt nanoparticles(Co/NC-CF)is designed to load sulfur.Meanwhile,gel polymer electrolyte(GPE)with high ion transfer ability is obtained by in-situ polymerization inside the battery.During the polymerization process,an integrated electrode-electrolyte and a continuous ion-electron conduction network in a composite cathode are constructed inside the Na-S battery.It is noteworthy that the designed GPE demonstrates superior ionic conductivity and effective adsorption of NaPSs that can significantly suppress the shuttle effect.Leveraging the synergistic interplay between the designed GPE and self-supporting cathode,the assembled quasi-solid-state(QSS)Na-S battery exhibits great cycling stability.These experimental results are further corroborated by COMSOL Multiphysics simulations and density functional theory(DFT)calculations,which mechanistically validate the enhanced electrochemical performance.The findings of this study offer new and promising perspectives for advancing the development of nextgeneration solid-state batteries.
基金supported by the National Natural Science Foundation of China(52372099,52202328,22461142135,22479046)the Shanghai Sailing Program(22YF1455500)the Shanghai Magnolia Talent Plan Pujiang Project(24PJD128)。
文摘Solid-state polymer electrolytes are crucial for advancing solid-state lithium-metal batteries owing to their flexibility,excellent manufacturability,and strong interfacial compatibility.However,their widespread applications are hindered by low ionic conductivity at room temperature and lithium dendrite growth.Herein,we report a novel solid-state composite membrane electrolyte design that combines the vertically aligned channel structure and copolymer with a radial gradient composition.Within the vertically aligned channels,the composition of poly(vinyl ethylene carbonate-co-poly(ethylene glycol)diacrylate)(P(VEC-PEGDA)varies in a gradient along the radial direction:from the center to the wall of vertically aligned channels,the proportion of vinyl ethylene carbonate(VEC)in the copolymer decreases,while the proportion of poly(ethylene glycol)diacrylate(PEGDA)increases accordingly.It can be functionally divided into a mechanical-reinforcement layer and a fast-ion-conducting layer.The resulting solid-state composite membrane electrolyte achieves a high critical current density of 1.2 mA cm^(-2)and high ionic conductivity of 2.03 mS cm^(-1)at room temperature.Employing this composite membrane electrolyte,a Li//Li symmetric cell exhibits stable cycling for over 1850 h at 0.2 m A cm^(-2)/0.2 m A h cm^(-2),and a Li//LiFePO4(LFP)battery maintains 77.3% capacity retention at 2 C after 300 cycles.Our work provides insight into the rational design of safer and more efficient solidstate batteries through electrolyte structural engineering.
基金Natural Science Foundation of China (51603031)Liaoning Provincial Natural Science Foundation of China (2020-MS-087)China Scholarship Council(202306080157)。
文摘This work focuses on the development of high temperature polymer electrolyte membranes(HT-PEMs)as key materials for HT-PEM fuel cells(HT-PEMFCs).Recognizing the challenges associated with the phosphoric acid(PA) doped polybenzimidazole(PBI) membranes,including the use of carcinogenic monomers and complex synthesis procedures,this study aims to develop more cost-effective,readily synthesized,and high-performance alternatives.A series of superacid-catalyzed polyhydroxyalkylation reactions have been carefully designed between p-terphenyl and aldehydes bearing imidazole moieties,resulting in a new class of HT-PEMs.It is found that the chemical structure of aldehyde-substituted N-heterocycles significantly impacts the polymerization reaction.Specifically,the use of 1-methyl-2-imidazole-formaldehyde and 1 H-imidazole-4-formaldehyde monomers leads to the formation of high-viscosity,rigid,and ether-free polymers,denoted as PTIm-a and PTIm-b.Membranes fabricated from these polymers,due to their pendent imidazole groups,exhibit an exceptional capacity for PA absorption.Notably,PTIm-a,carrying methylimidazole moieties,demonstrates a superior chemical stability by maintaining morphology and structural stability during 350 h of Fenton testing.After being immersed in 75 wt% PA at 40℃,the PTIm-a membrane reaches a PA content of 152%,maintains a good tensile strength of 13.6 MPa,and exhibits a moderate conductivity of 50.2 mS cm^(-1) at 180℃.Under H_(2)/O_(2) operational conditions,a single cell based on the PTIm-a membrane attains a peak power density of 732 mW cm^(-2) at 180℃ without backpressure.Furthermore,the membrane demonstrates stable cycle stability over 173 h within 18 days at a current density of 200 mA cm^(-2),indicating its potential for practical application in HT-PEMFCs.This work highlights innovative strategies for the synthesis of advanced HT-PEMs,offering significant improvements in membrane properties and fuel cell performance,thus expanding the horizons of HT-PEMFC technology.
基金supported by The National Key Research and Development Program of China(2021YFB4001204)National Natural Science Foundation of China(22379143)。
文摘Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(terphenyl piperidinium)s constructed from the m-and p-isomers of terphenyl were synthesized to regulate the microstructure of the membrane.Highly rigid p-terphenyl units prompt the formation of moderate PA aggregates,where the ion-pair interaction between piperidinium and biphosphate is reinforced,leading to a reduction in the plasticizing effect.As a result,there are trade-offs between the proton conductivity,mechanical strength,and PA retention of the membranes with varied m/p-isomer ratios.The designed PA-doped PTP-20m membrane exhibits superior ionic conductivity,good mechanical strength,and excellent PA retention over a wide range of temperature(80–160°C)as well as satisfactory resistance to harsh accelerated aging tests.As a result,the membrane presents a desirable combination of performance(1.462 W cm^(-2) under the H_(2)/O_(2)condition,which is 1.5 times higher than that of PBI-based membrane)and durability(300 h at 160°C and 0.2 A cm^(-2))in the fuel cell.The results of this study provide new insights that will guide molecular design from the perspective of microstructure to improve the performance and robustness of HT-PEMs.
基金supported by the National Natural Science Foundation of China(No.51803041)the University and Local Integration Development Project of Yantai,China(No.2022 XDRHXMXK08).
文摘Herein,an external crosslinker facilitated the hypercrosslinking of ferrocene and a nitrogen heterocyclic compound(either melamine or imidazole)through a direct Friedel-Crafts reaction,which led to the formation of nitrogen-containing hypercrosslinked fer-rocene polymer precursors(HCP-FCs).Subsequent carbonization of these precursors results in the production of iron-nitrogen-doped por-ous carbon absorbers(Fe-NPCs).The Fe-NPCs demonstrate a porous structure comprising aggregated nanotubes and nanospheres.The porosity of this structure can be modulated by adjusting the iron and nitrogen contents to optimize impedance matching.The uniform dis-tribution of Fe-N_(x)C,N dipoles,andα-Fe within the carbon matrix can be ensured by using hypercrosslinked ferrocenes in constructing porous carbon,providing the absorber with numerous polarization sites and a conductive network.The electromagnetic wave absorption performance of the specially designed Fe-NPC-M_(2)absorbers is satisfactory,revealing a minimum reflection loss of-55.3 dB at 2.5 mm and an effective absorption bandwidth of 6.00 GHz at 2.0 mm.By utilizing hypercrosslinked polymers(HCPs)as precursors,a novel method for developing highly efficient carbon-based absorbing agents is introduced in this research.
基金financially supported by the National Natural Science Foundation of China(Nos.52233001,51927805,and 52173110)the Innovation Program of Shanghai Municipal Education Commission(No.2023ZKZD07)the Shanghai Rising-Star Program(No.22QA1401200)。
文摘Cholesteric liquid crystals(CLCs)exhibit unique helical superstructures that selectively reflect circularly polarized light,enabling them to dynamically respond to environmental changes with tunable structural colors.This dynamic color-changing capability is crucial for applications that require adaptable optical properties,positioning CLCs as key materials in advanced photonic technologies.This review focuses on the mechanisms of dynamic color tuning in CLCs across various forms,including small molecules,cholesteric liquid crystal elastomers(CLCEs),and cholesteric liquid crystal networks(CLCNs),and emphasizes the distinct responsive coloration each structure provides.Key developments in photochromic mechanisms based on azobenzene,dithienylethene,and molecular motor switches,are discussed for their roles in enhancing the stability and tuning range of CLCs.We examine the color-changing behaviors of CLCEs under mechanical stimuli and CLCNs under swelling,highlighting the advantages of each form.Following this,applications of dynamic color-tuning CLCs in information encryption,adaptive camouflage,and smart sensing technologies are explored.The review concludes with an outlook on current challenges and future directions in CLC research,particularly in biomimetic systems and dynamic photonic devices,aiming to broaden their functional applications and impact.
基金supported by the National Natural Science Foundation of China(Nos.32301259,32101228,32271527 and 32371536)the“Pioneer”and“Leading Goose”R&D Program of Zhejiang(Nos.2022C02023 and 2023C02015)+1 种基金the Research Foundation of Talented Scholars of Zhejiang A&F University(No.2021LFR058)the Dean-ship of Scientific Research at Northern Border University,Arar,KSA for funding this research work through the project number“NBU-FPEJ-2024-177-01”.
文摘As a typical bioflavonoid,diosmetin is desirable in the field of natural medicine,healthy food,and cosmetics by anti-cancer,antibacterial,antioxidant,estrogen-like and anti-inflammatory activities,and it comes from a wide range of sources in traditional Chinese medicine like spider fragrance,spearmint and chrysanthemum,as well as in Citrus fruit.However,traditional analytical methods such as silica gel column chromatography face multiple challenges in the selective extraction of diosmetin from biological materials and traditional Chinese medicinal materials.Therefore,it is urgent to develop a new type of absorbent with high efficiency,recyclability and good specificity to diosmetin.In this investigation,a magnetic surface molecularly imprinted polymer(labeled as Diosmetin/SMIPs)was synthesized employing magnetic nanoparticles as the carrier and 4-vinylpyridinyl(4-VP)as the functional monomer by surface imprinting technology.The functional monomer was screened by the binding energy(△E)between functional monomers and template molecules via computational simulation.The Diosmetin/SMIPs had a high level of specific recognition and adsorption capability towards diosmetin with a 20.25 mg g^(-1) adsorption capacity and an imprinting factor(IF)of 2.28.Additionally,it demonstrated excellent regeneration performance with 8 adsorption/desorption cycles.In addition,91.20%-94.16% of spiked diosmetin was recovered from the lemon peel samples.The strategy of constructing Diosmetin/SMIPs based on computational simulation can effectively enhance the specific adsorption performance of diosmetin.Meanwhile,Diosmetin/SMIPs synthesized by imprinting polymerization showed excellent anti-interference and reusability,and realized efficient targeted extraction of diosmetin from lemon peel samples.The results of this investigation provide a promising adsorbent for selective enrichment of diosmetin from Citrus fruit and complicated materials.
文摘In recent years,smart materials have emerged as a groundbreaking innovation in the field of water filtration,offering sustainable,efficient,and environmentally friendly solutions to address the growing global water crisis.This review explores the latest advancements in the application of smart materials—including biomaterials,nanocomposites,and stimuli-responsive polymers—specifically for water treatment.It examines their effectiveness in detecting and removing various types of pollutants,including organic contaminants,heavy metals,and microbial infections,while adapting to dynamic environmental conditions such as fluctuations in temperature,pH,and pressure.The review highlights the remarkable versatility of these materials,emphasizing their multifunctionality,which allows them to address a wide range of water quality issues with high efficiency and low environmental impact.Moreover,it explores the potential of smart materials to overcome significant challenges in water purification,such as the need for real-time pollutant detection and targeted removal processes.The research also discusses the scalability and future development of these materials,considering their cost-effectiveness and potential for large-scale application.By aligning with the principles of sustainable development,smart materials represent a promising direction for ensuring global water security,offering both innovative solutions for current water pollution issues and long-term benefits for the environment and public health.
文摘We report five coordination polymers(CPs)based on fluorescent ligands[1,6-di(1H-imidazol-1-yl)pyrene(dip),9,10-di(1H-imidazol-1-yl)anthracene(dia)]and anionic ligands[cyclohexane-1,4-dicarboxylic acid(H_(2)cda),camphoric acid(H_(2)cpa)].In[Cd(dip)(cda)]·4H_(2)O}_(n)(1),the Cd^(2+)ions,acting as tetrahedral nodes,are linked by dipand cda^(2-)ligands with four Cd^(2+)ions into five-fold interpenetrating network array of topology of dia.In{[Cd(dip)(cpa)]·4H_(2)O}_(n)(2),the Cd^(2+)ions,acting as a 4-connector,are linked by cpa^(2-)and dip ligands into a 3D framework ofcds topology.In{[Ni(dia)_(2)Cl_(2)]·DMF}_(n)(3),the Ni^(2+)ion is linked by four dia ligands into a layer structure,and 1Dchannels of a cross-section of 1.35 nm×0.96 nm are formed.In{[Cd(dia)_(2)(H_(2)O)_(2)](NO_(3))_(2)·2DMSO}n(4),the dia ligandsconnected Cd^(2+)ions into a 2D layer,and 1D channels are formed between adjacent layers with a cross-section of0.87 nm×0.43 nm.In[Zn(dip)Cl_(2)]_(n)(5),the Zn^(2+)ion is linked by dip ligands into an infinite 1D chain.The infrared,thermal gravimetric,and fluorescent emission data were collected and analyzed for these coordination polymers.CCDC:2356055,1;2440075,2;2356057,3;2356057,4;2356059,5.
文摘Six coordination polymers based on 9,10-di(pyridine-4-yl)-anthracene(DPA)and 1,6-di(1H-imidazol-1-yl)pyrene(DIP)were obtained by solvothermal reactions.{[Zn(DPA)Cl_(2)]·DMF·2H_(2)O}n(1)and{[Zn_(1.5)(DPA)_(1.5)Cl_(3)]·5H_(2)O}n(2)are framework isomers,which both contain zigzag chains formed by DPA,Zn^(2+),and Cl-.The zigzag chains in 1 are further assembled by C—H…Cl interactions into layers,and these layers exhibit two different orientations,displaying a rare 2D to 3D interpenetration mode.The zigzag chains in 2 are parallelly arranged.{[Zn_(3)(DPA)_(3)Br_(6)]·2DMF·_(1.5)H_(2)O}n(3)is isostructural to 2.3 was obtained using ZnBr_(2)instead of ZnCl_(2).[M(DPA)(formate)_(2)(H_(2)O)_(2)]n[M=Co(4),Cu(5)]are isostructural,contain chain structures formed by DPA,Cu^(2+)/Co^(2+),and for-mate ions,which were formed in situ in the solvothermal reaction.{[Zn(DIP)_(2)Cl]ClO_(4)}n(6)contains a layer structure formed by DIP and Zn^(2+).Free DPA and DIP ligands exhibited high fluorescence at room temperature,and coordina-tion polymers 3 and 6 displayed enhanced fluorescent emissions.
基金financially supported by the Sichuan Science and Technology Program(2022YFS0025 and 2024YFFK0133)supported by the“Fundamental Research Funds for the Central Universities of China.”。
文摘Tactile perception plays a vital role for the human body and is also highly desired for smart prosthesis and advanced robots.Compared to active sensing devices,passive piezoelectric and triboelectric tactile sensors consume less power,but lack the capability to resolve static stimuli.Here,we address this issue by utilizing the unique polarization chemistry of conjugated polymers for the first time and propose a new type of bioinspired,passive,and bio-friendly tactile sensors for resolving both static and dynamic stimuli.Specifically,to emulate the polarization process of natural sensory cells,conjugated polymers(including poly(3,4-ethylenedioxythiophen e):poly(styrenesulfonate),polyaniline,or polypyrrole)are controllably polarized into two opposite states to create artificial potential differences.The controllable and reversible polarization process of the conjugated polymers is fully in situ characterized.Then,a micro-structured ionic electrolyte is employed to imitate the natural ion channels and to encode external touch stimulations into the variation in potential difference outputs.Compared with the currently existing tactile sensing devices,the developed tactile sensors feature distinct characteristics including fully organic composition,high sensitivity(up to 773 mV N^(−1)),ultralow power consumption(nW),as well as superior bio-friendliness.As demonstrations,both single point tactile perception(surface texture perception and material property perception)and two-dimensional tactile recognitions(shape or profile perception)with high accuracy are successfully realized using self-defined machine learning algorithms.This tactile sensing concept innovation based on the polarization chemistry of conjugated polymers opens up a new path to create robotic tactile sensors and prosthetic electronic skins.
文摘Two new Mn(Ⅱ)coordination polymers,namely{[Mn_(2)(HL)(phen)_(3)(H_(2)O)_(2)]·7.5H_(2)O}_n(1)and[Mn_(4)(HL)_(2)(1,4-bib)_(3)(H_(2)O)_(2)]_n(2),were synthesized under hydrothermal conditions by using Mn(Ⅱ)ions and 6-(3',4'-dicarboxylphenoxy)-1,2,4-benzenetricarboxylic acid(H_(5)L)in the presence of N-auxiliary ligands 1,10-phenanthroline(phen)and1,4-bis(1H-imidazol-1-yl)benzene(1,4-bib).The structures of coordination polymers 1 and 2 were characterized by infrared spectroscopy,single-crystal X-ray diffraction,thermogravimetric analysis,and powder X-ray diffraction.Single-crystal X-ray diffraction reveals that 1 has a 1D chain structure based on binuclear Mn(Ⅱ)units,while 2 features a(3,8)-connected 3D network structure based on tetranuclear Mn(Ⅱ)units.Magnetic studies show that 1 and 2exhibit antiferromagnetic interactions between manganese ions.2 shows stronger antiferromagnetic interactions due to the shorter Mn…Mn distances within the tetranuclear manganese units.CCDC:2357601,1;2357602,2.
基金financial support from the National Natural Science Foundation of China(Nos.22108258 and 52003251)Program for Science&Technology Innovation Talents in Universities of Henan Province(24HASTIT004)+1 种基金Outstanding Youth Fund of Henan Scientific Committee(222300420085)Science and Technology Joint Project of Henan Province(222301420041)。
文摘Mixed matrix membranes(MMMs)have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers.However,achieving a simultaneous enhancement of permeability and selectivity remains a formidable challenge,due to the difficulty of achieving an optimal match between polymers and fillers.In this study,we incorporate a porous carbon-based zinc oxide composite(C@ZnO)into high-permeability polymers of intrinsic microporosity(PIMs)to fabricate MMMs.The dipole–dipole interaction between C@ZnO and PIMs ensures their exceptional compatibility,mitigating the formation of non-selective voids in the resulting MMMs.Concurrently,C@ZnO with abundant interconnected pores can provide additional low-resistance pathways for gas transport in MMMs.As a result,the CO_(2) permeability of the optimized C@ZnO/PIM-1 MMMs is elevated to 13,215 barrer,while the CO_(2)/N_(2) and CO_(2)/CH_(4) selectivity reached 21.5 and 14.4,respectively,substantially surpassing the 2008 Robeson upper bound.Additionally,molecular simulation results further corroborate that the augmented membrane gas selectivity is attributed to the superior CO_(2) affinity of C@ZnO.In summary,we believe that this work not only expands the application of MMMs for gas separation but also heralds a paradigm shift in the application of porous carbon materials.
