Multi-component polymer systems exhibit exceptional versatility and structural diversity,making them indispensable in the polymer industry as well as in advanced and high performance applications.However,constructing ...Multi-component polymer systems exhibit exceptional versatility and structural diversity,making them indispensable in the polymer industry as well as in advanced and high performance applications.However,constructing accurate phase diagrams for these systems remains challenging due to inhomogeneous structures arising from the introduction of block copolymer components.Here,we present a unified and model-agnostic framework for computing phase equilibria in multi-component polymeric systems based on the concept of“effective chemical potential”.This approach directly connects key thermodynamic variables in the canonical ensemble to other ensembles,unifying phase coexistence determination without requiring the reformulation of self-consistent field theory(SCFT)calculations across different ensembles.By decoupling phase equilibrium determination from specific ensemble formulations,our approach enables the reuse of existing SCFT solvers.Moreover,it provides a useful framework to develop highly efficient phase equilibrium solvers for multi-component polymer systems.展开更多
Advancing the integration of artificial intelligence and polymer science requires high-quality,open-source,and large-scale datasets.However,existing polymer databases often suffer from data sparsity,lack of polymer-pr...Advancing the integration of artificial intelligence and polymer science requires high-quality,open-source,and large-scale datasets.However,existing polymer databases often suffer from data sparsity,lack of polymer-property labels,and limited accessibility,hindering system-atic modeling across property prediction tasks.Here,we present OpenPoly,a curated experimental polymer database derived from extensive lit-erature mining and manual validation,comprising 3985 unique polymer-property data points spanning 26 key properties.We further develop a multi-task benchmarking framework that evaluates property prediction using four encoding methods and eight representative models.Our re-sults highlight that the optimized degree-of-polymerization encoding coupled with Morgan fingerprints achieves an optimal trade-off between computational cost and accuracy.In data-scarce condition,XGBoost outperforms deep learning models on key properties such as dielectric con-stant,glass transition temperature,melting point,and mechanical strength,achieving R2 scores of 0.65-0.87.To further showcase the practical utility of the database,we propose potential polymers for two energy-relevant applications:high temperature polymer dielectrics and fuel cell membranes.By offering a consistent and accessible benchmark and database,OpenPoly paves the way for more accurate polymer-property modeling and fosters data-driven advances in polymer genome engineering.展开更多
The facile synthesis of high-valued polymers from waste molecules or low-cost common chemicals presents a significant challenge.Here,we develop a series of degradable poly(thiocarbonate)s from the new step-growth poly...The facile synthesis of high-valued polymers from waste molecules or low-cost common chemicals presents a significant challenge.Here,we develop a series of degradable poly(thiocarbonate)s from the new step-growth polymerization of diols,carbonyl sulfide(CoS,or carbon disulfide,CS_(2)),and dichlorides.Diols and dichlorides are common chemicals,and CoS(CS_(2))is released as industrial waste.In addition to abun-dant feedstocks,the method is efficient and performed under mild conditions,using common organic bases as catalysts,and affording unprece-dented polymers.When cos,diols,and dihalides were used as monomers,optimized conditions could completely suppress the oxygen-sulfur exchange reaction,enabling the efficient synthesis of well-defined poly(monothiocarbonate)s with melting points ranging from 48°C to 101°C.These polymers,which have a structure similar to polyethylene with low-density in-chain polar groups,exhibit remarkable toughness and ductili-ty that rival those of high-density polyethylene(melting point:90°C,tensile strength:21.6±0.7 MPa,and elongation at break:576%).Moreover,the obtained poly(monothiocarbonate)s can be chemically degraded by alcoholysis to yield small-molecule diols and dithiols.When CS_(2)was used in place of cos,a pronounced oxygen-sulfur exchange reaction occurred.By optimizing reaction condition,it was found that polymers with-S(C=O)S-and-S(C=S)S-as the main repeating units exhibited high thermal stability and crystallinity.Thus,a new approach for regulat-ing the structure of polythiocarbonates via the oxygen-sulfur exchange reaction is developed.Overall,the polymers hold great potential for green materials due to their facile synthesis,readily available feedstocks,excellent performance,and chemical degradability.展开更多
In recent years,ultrathin polymer-based electrolytes(UPEs)have emerged as a promising strategy to enhance the energy density of rechargeable batteries for wearable devices by minimizing electrolyte volume,demonstratin...In recent years,ultrathin polymer-based electrolytes(UPEs)have emerged as a promising strategy to enhance the energy density of rechargeable batteries for wearable devices by minimizing electrolyte volume,demonstrating higher ionic conductance and lower internal resistance,and more compact battery stacking compared to conventional thick polymer-based electrolyte.This mini review systematically summarizes recent advances in ultrathin solid-state and gel-state electrolytes,focusing on their preparation strategies,advantages,and disadvantages,where the energy density,interfacial stability,mechanical properties,and ion-transport mechanisms are also analyzed for understanding the UPE application.Moreover,the challenges such as dendrite penetration and instability(thermal,chemical and interface),along with their solutions are also introduced through interfacial engineering,polymer matrix design,and fillers incorporation.Furthermore,for practical application,the demands of working current density,operating temperature and scale-up production are also illustrated.This mini review is hoped to spark insights into improving the energy density of batteries and ultimately bring us a step closer to realizing superior rechargeable batteries.展开更多
Given the increasing demand for distributed electricity,there is a burning desire to harvest electricity from renewable sources using environmentally friendly methods.Thermoelectric (TE) materials can meet this requir...Given the increasing demand for distributed electricity,there is a burning desire to harvest electricity from renewable sources using environmentally friendly methods.Thermoelectric (TE) materials can meet this requirement not only because of their ability to convert heat directly into electricity,enabling energy harvesting from waste heat and natural heat resources,but also because more than 60%of the energy is lost as waste heat [1].The discovery of the TE effect dates back to the 1820s when T.M.Seebeck observed electricity generation at the junction of two conductors with different temperatures.Additionally,when a voltage is applied to TE materials,they can create a temperature difference to enable solid-state cooling (known as the Peltier effect).Therefore,the TE effect promises both sustainable energy solutions and temperature control technologies.Over the past two decades,the urgent demand for powering ubiquitous Internet of Things devices has sparked significant interest in flexible thermoelectrics(F-TEs),which raises an intriguing question:Is the intrinsically flexible polymer an important candidate for state-of-the-art F-TEs applications?展开更多
Owing to their excellent biocompatibility and potential for durability enhancement,polymeric heart valves(PHVs)are emerging as a promising alternative to traditional prostheses.Unlike conventional materials,PHVs can b...Owing to their excellent biocompatibility and potential for durability enhancement,polymeric heart valves(PHVs)are emerging as a promising alternative to traditional prostheses.Unlike conventional materials,PHVs can be manufactured under precise design criteria,enabling targeted performance improvements.This study introduces a geometric optimization strategy for enhancing the durability of PHVs.The finite element method(FEM)is combined with a dip-molding technique to develop a novel polymeric aortic valve with improved mechanical properties.The tri-leaflet geometry is parameterized using B-spline curves,and the maximum stress in the valve is reduced from 2.4802 to 1.7773 MPa using a multiobjective optimization algorithm NSGA-II(non-dominated sorting genetic algorithm II).Pre-optimized and optimized valve prototypes were fabricated via dip-molding and evaluated during pulsatile-flow tests and accelerated wear tests.The optimized design meets the ISO 5840 standards,with an effective orifice area of 2.019 cm^(2),a regurgitant fraction of 5.693%,and a transvalvular pressure gradient of 7.576 mmHg.Moreover,the optimized valve maintained its structural integrity and functionality over 14 million cycles of the accelerated wear test,whereas the unoptimized valve failed after two million cycles.These findings confirm that the FEM-based geometric optimization method enhances both the mechanical performance and durability of PHVs.展开更多
Although the certified power conversion efficiency(PCE)of single-junction perovskite solar cells(PSCs)has achieved a high level of 27%,approaching the single-crystalline silicon solar cells,the device stability remain...Although the certified power conversion efficiency(PCE)of single-junction perovskite solar cells(PSCs)has achieved a high level of 27%,approaching the single-crystalline silicon solar cells,the device stability remains an urgent issue to be resolved for the commercialization.Defect passivation emerged as a viable approach to enhance the operational stability of the solar devices.Herein,phenylthiourea(PhTu)derivatives are selected as effective passivation agents to enhance the optoelectronic properties of printed methylammonium lead iodide(MAPbI_(3))films.It is demonstrated that incorporating a small amount of 1-(4-carboxyphenyl)-2-thiourea(PhTu-COOH)significantly reduces the trap-state density and leads to longer carrier lifetime of the perovskite films.As a result,the inverted solar device made of Ph Tu-COOH-modified MAPbI_(3) perovskite film shows remarkably improved efficiency(from 17.29%to 20.22%)and obviously increased open-circuit voltage(V_(OC))(from 1.043 to 1.143 V),as compared with the pristine device.Moreover,the Ph Tu-COOH-modified PSCs exhibit enhanced operational stability due to the significantly reduced trap-state density.Finally,the optimized solar module fabricated with an active area of 11.28 cm^(2) delivers a high PCE of 17.07%with negligible V_(OC)loss,demonstrating the feasibility of the blade-coating method for large-area perovskite film deposition.展开更多
Dynamic melt modification of polyethylene via the direct grafting of peroxide fragments shows promise for the development of processable functionalized materials.In this study,four linear low-density polyethylenes(LLD...Dynamic melt modification of polyethylene via the direct grafting of peroxide fragments shows promise for the development of processable functionalized materials.In this study,four linear low-density polyethylenes(LLDPEs)with comparable molecular weights but different short-chain branch(SCB)contents(ranging of 5-66 per 1000 carbon atoms)were modified via dynamic melt mixing using 2 wt% benzoyl peroxide at 145℃ and 50 r/min for 30 min.The influence of SCB content on the processability and structure of the resulting products was systematically investigated.All modified products exhibited good melt processability with melt flow rates(MFR)ranging from 0.46 g/10min to 1.07 g/10min.Products derived from low-SCB LLDPEs showed a lower MFR,higher cross-linking content,a larger number of long-chain branches,and a higher degree of benzoyl grafting.In contrast,those produced from high-SCB LLDPEs exhibited improved processability,reduced cross-linking,fewer long-chain branches,and lower benzoyl grafting levels.A detailed structural investigation of the soluble and insoluble fractions,which were separated using trichlorobenzene fractionation,was conducted to analyze the structural features of various modified products and demonstrate that the SCB content(i.e.,tertiary carbon density)significantly influences radical coupling during dynamic modification.Elevated tertiary carbon density,by introducing greater steric hindrance,suppresses radical coupling during dynamic modification,thereby reducing the efficiency of both crosslinking and peroxide fragment grafting.These findings provide new insights into the structure-reactivity relationships in peroxide-induced polyethylene modification and lay the foundation for tailoring material properties via dynamic processing.展开更多
With the rapid advancements in biomedical engineering,bioprinting has emerged as a pivotal solution to address the shortage of organ transplants and advance disease model research.The evolution of bioprinting has prog...With the rapid advancements in biomedical engineering,bioprinting has emerged as a pivotal solution to address the shortage of organ transplants and advance disease model research.The evolution of bioprinting has progressed from the fabrication of simple models(1.0)to the fabrication of permanent implants(2.0),tissue engineering scaffolds(3.0),and complex biostructures utilizing living cells(4.0).Nevertheless,significant challenges remain,particularly in accurately replicating the structure and function of host tissues,selecting appropriate materials,and optimizing printing parameters.The integration of artificial intelligence(AI),especially machine learning,provides promising novel opportunities in bioprinting(5.0).This review systematically summarizes the current applications of AI in bioprinting,discussing both construction strategies and application scenarios.It also explores the potential of AI to improve bioprinting in the preparation of complex functional tissues and in situ tissue repair.Overall,the synergy between AI and bioprinting is poised to drive the development of personalized medicine,facilitate high-throughput preparation of in vitro models,and provide robust tools for regenerative medicine and precision healthcare.展开更多
Self-healing materials have been developed over the past decade with the recovery ability after damage.However,most researches focused on the self-healing process at three-dimension.Herein,we prepare monolayer self-he...Self-healing materials have been developed over the past decade with the recovery ability after damage.However,most researches focused on the self-healing process at three-dimension.Herein,we prepare monolayer self-healing hydrogen-bond-based supramolecular polymer film and explore the self-healing process at the two-dimensional limit.The healing process,which can be reversibly repeated for at least three times,is influenced by the temperature,the molecule-substrate interaction and the substrate roughness.In the application,the monolayer self-healing polymer film can be used to modify the SiO2 dielectric for copper phthalocyanine field effect transistor with improved mobility.This work will be valuable for developing two-dimensional functional self-healing materials in the future.展开更多
Lateral flow immunoassays(LFIAs)provide a powerful tool for rapid real-time assay of cancer biomarkers,which is vital for cancer detection and treatment follow-up.Lanthanide-based LFIAs is one of the most widely used ...Lateral flow immunoassays(LFIAs)provide a powerful tool for rapid real-time assay of cancer biomarkers,which is vital for cancer detection and treatment follow-up.Lanthanide-based LFIAs is one of the most widely used methods,especially Eu(Ⅲ)chelates,which possess distinctive and attractive characteristics,such as time-resolved fluorescence and large Stokes shift.Herein,we adopted a new onestep mini-emulsion polymerization method to synthesize carboxyl-modified fluorescent microsphere(OS-EuCM),which shows good stability,resistance to non-specific adhesion and uniform particle size distribution compared with traditional microspheres synthesized through the swelling method.Benefiting from the above advantages,OS-EuCM was successfully used in LFIAs to detect tumor marker Alpha-fetoprotein with high sensitivity and selectivity in concentration as high as 320 ng/mL,as well as a detection limit of 0.683 ng/mL This lanthanide-based microsphere holds great potential for rapid pointof-care screening and clinical application.展开更多
A facile technique is herein reported to fabricate three-dimensional （3D） polymeric porous scaffolds with interior surfaces of a topographic microstructure favorable for cell adhesion. As demonstration, a well-known...A facile technique is herein reported to fabricate three-dimensional （3D） polymeric porous scaffolds with interior surfaces of a topographic microstructure favorable for cell adhesion. As demonstration, a well-known biodegradable polymer poly（lactide-co-glycolide） （PLGA） was employed as matrix. Under the porogen-leaching strategy, the large and soft porogens of paraffin were modified by colliding with small and hard salt particles, which generated micropits on the surfaces of paraffin spheres. The eventual PLGA scaffolds after leaching the modified porogens had thus interior surfaces of microscale roughness imprinted by those micropits. The microrough scaffolds were confirmed to benefit adhesion of bone marrow stromal cells （BMSCs） of rats and meanwhile not to hamper the proliferation and osteogenic differentiation of the cells. The insight and technique might be helpful for biomaterial designing in tissue engineering and regenerative medicine.展开更多
Three-dimensional graphene/conducting polymer（3DGCP） composites have received significant attention in recent years due to their unique structures and promising applications in energy storage.With the structural div...Three-dimensional graphene/conducting polymer（3DGCP） composites have received significant attention in recent years due to their unique structures and promising applications in energy storage.With the structural diversity of graphene and π-functional conducting polymers via rich chemical routes,a number of 3DGCP composites with novel structures and attractive performance have been developed.Particularly,the hierarchical porosity,the interactions between graphene and conducting polymers as well as the their synergetic effects within 3DGCP composites can be well combined and elaborated by various synthetic methods,which made 3DGCP composites show unique electrochemical properties and significantly improved performance in energy storage fields compared to other graphenebased composites.In this short review,we present recent advances in 3DGCP composites in developing effective strategies to prepare 3DGCP composites and exploring them as a unique platform for supercapacitors with unprecedented performance.The challenges and future opportunities are also discussed for promotion of further study.展开更多
Recent development of self-healing material has attracted tremendous attention,owing to its biomimetic ability to restore structure and functionality when encountering damages.Here,we develop a threedimensional(3D)pri...Recent development of self-healing material has attracted tremendous attention,owing to its biomimetic ability to restore structure and functionality when encountering damages.Here,we develop a threedimensional(3D)printable self-healing composite conductive polymer by mixing hydrogen-bond-based supramolecular polymer with low-cost carbon black.It has a room-temperature self-healing capability in both conductivity and mechanical property,while its shear-thinning behavior enables fabrication of a self-healable circuit by 3D printing technology.As an application,the circuit shows an excellent temperature-dependent behavior of the resistance,indicating its great potential fo r practical application in the artificial intelligence field.展开更多
Modifying polypropylene membranes with interpenetrating polymer networks(IPNs) through the incorporation of poly(glycidyl methacrylate-N-methyl-D-glucamine)(P(GMA-NMG)) was performed by in situ synthesis via radical p...Modifying polypropylene membranes with interpenetrating polymer networks(IPNs) through the incorporation of poly(glycidyl methacrylate-N-methyl-D-glucamine)(P(GMA-NMG)) was performed by in situ synthesis via radical polymerization. The surface of the polypropylene membrane was activated by hydrophilic grafted polyelectrolyte, and then, pressure injection was used for the impregnation of the reactive solution in the membrane.Two types of pore-filled membranes were synthesized, chelating interpenetrating homopolymer networks of P(GMA-NMG), and chelating-ion exchange interpenetrating polymer networks(e.g., P(GMA-NMG)/P(AA),P(GMA-NMG)/P(AMPSA), and P(GMA-NMG)/P(Cl VBTA)). After their synthesis, the modified polypropylene membranes were characterized using techniques such as the electrokinetic potential, SEM, FT-IR, and Donnan dialysis to corroborate the chromium ion transport. The P(GMA-NMG) and complex network membranes exhibited a hydrophilic character with a water-uptake capacity between 20% and 35% and a percentage of modification between 4.0% and 7.0% in comparison with the behavior of the unmodified polypropylene membrane.Hexavalent chromium ions were efficiently transported from the food chamber at p H 9.0 when the 65.2%MTA1 P(Cl VBTA) homopolymer IPN membrane and 48.5% MTAG P(GMA-NMG)/P(Cl VBTA) IPN membrane were used. Similarly, hexavalent chromium ions were removed from the food chamber at pH 3.0 when MTAG(63.30%) and MTA1(35.68%) were used in 1 mol·L^(-1)Na Cl solution as the extraction reagent.展开更多
Photo-controlled reversible-deactivation radical polymerizati on(photo-RDRP)has been investigated as a"green"and spatiotem-porally controlling pathway for polymer synthesis.While the combination of photo-RDR...Photo-controlled reversible-deactivation radical polymerizati on(photo-RDRP)has been investigated as a"green"and spatiotem-porally controlling pathway for polymer synthesis.While the combination of photo-RDRP and flow chemistry has offered opportunities to increase light intensity and enable uniform light irradiation,problems associated with flow approaches still remain for photoflow-RDRP,which has hindered merging flow polymerization with other cutting-edge techniques.Herein,we summarize challenges and recent achievements in photoflow-RDRP including the development of(a)droplet/slug-flow to regulate reside nee time distribution,(b)mixing techniques to tailor polymer,(c)polymerization in duced self-assembly,and(d)computer-aided synthesis.We hope this work will provide in formative knowledge to people in related fields and stimulate novel ideas to promote polymer synthesis in both academia and industry.展开更多
The activation and deactivation of the chain-transfer agent were achieved by oxygen initiation and regulation with triethylborane under ambient temperature and atmosphere.The autoxidation of triethylborane overcame th...The activation and deactivation of the chain-transfer agent were achieved by oxygen initiation and regulation with triethylborane under ambient temperature and atmosphere.The autoxidation of triethylborane overcame the oxygen inhilbition and produced initiating radicals that selectively activate the chain-transfer agent for the chain growth or deactivate the active chain-end of polymer in controlled radical polymerization.Both activation and deactivation were highly efficient with broad scope for various polymers with different chain-transfer agents in both organic and aqueous systems.Oxygen molecule was particularly used as an external regulator to initiate and achieve the temporal control of both activation and deactivation by simply feeding the air.展开更多
Biological stimuli-responsive polymers have increasingly attracted attention in recent years because it can satisfy many requirements of applications related with human body while traditional systems do not meet.Due t...Biological stimuli-responsive polymers have increasingly attracted attention in recent years because it can satisfy many requirements of applications related with human body while traditional systems do not meet.Due to the importance of this burgeoning field,great efforts have been devoted and,up to now,polymer chemists have made a remarkable success in this prospective research topic.In this review,we systematically generalize the present state of biological stimuli-responsive polymer systems.We highlight several representative examples to specify the current problems and look ahead a clear sense of direction in this area.展开更多
Heterogeneous membranes were obtained by using styrene-acrylonitrile copolymer（SAN）blends with low content of ion-exchanger particles（5 wt.%）. The membranes obtained by phase inversion were used for the removal of...Heterogeneous membranes were obtained by using styrene-acrylonitrile copolymer（SAN）blends with low content of ion-exchanger particles（5 wt.%）. The membranes obtained by phase inversion were used for the removal of copper ions from synthetic wastewater solutions by electrodialytic separation. The electrodialysis was conducted in a three cell unit, without electrolyte recirculation. The process, under potentiostatic or galvanostatic control, was followed by p H and conductivity measurements in the solution. The electrodialytic performance,evaluated in terms of extraction removal degree（rd） of copper ions, was better under potentiostatic control then by the galvanostatic one and the highest（over 70%） was attained at8 V. The membrane efficiency at small ion-exchanger load was explained by the migration of resin particles toward the pores surface during the phase inversion. The prepared membranes were characterized by various techniques i.e. optical microscopy, Fourier transform infrared spectroscopy, scanning electron microscopy, thermogravimetric analysis and differential thermal analysis and contact angle measurements.展开更多
An optimized and high-performance Monte Carlo simulation is developed to take thorough account of four different cases of termination in styrene ATRP. According to the simulation results, the bimolecular termination r...An optimized and high-performance Monte Carlo simulation is developed to take thorough account of four different cases of termination in styrene ATRP. According to the simulation results, the bimolecular termination rate constant sharply drops throughout the polymerization when either chain-length dependency of termination rate constant, gel effect, or both together is applied to the simulation. In addition, as expected, the initiator is quickly decomposed at the early stages of the polymerization. The concentration of the catalyst in lower oxidation state decreases at first and then plateaus at higher conversion; furthermore, the steady concentration of Ml^nY/L in the polymerization is the highest when the chain-lengthdependent diffusion-controlled termination rate constant is employed in the simulation. The rates of deactivation and chain end degradation reactions are also smaller in this case. Therefore, the fraction of dormant chains is higher throughout the reaction and consequently the portion of dead polymers decreases. Besides, molecular weight increases linearly with conversion; however, when neither gel effect nor chain-length dependency of termination rate constant is considered, the molecular weight deviates from linearity at the end of the reaction. The peak of chain length distribution shifts toward higher molecular weight too during the reaction. Finally, the molecular weight distribution broadens at higher conversion; however, the chain length distribution of polymers produced under conditions of applying chain-length-dependent diffusion-controlled termination rate constant is narrower.展开更多
基金supported by the National Natural Science Foundation of China(No.21873021).
文摘Multi-component polymer systems exhibit exceptional versatility and structural diversity,making them indispensable in the polymer industry as well as in advanced and high performance applications.However,constructing accurate phase diagrams for these systems remains challenging due to inhomogeneous structures arising from the introduction of block copolymer components.Here,we present a unified and model-agnostic framework for computing phase equilibria in multi-component polymeric systems based on the concept of“effective chemical potential”.This approach directly connects key thermodynamic variables in the canonical ensemble to other ensembles,unifying phase coexistence determination without requiring the reformulation of self-consistent field theory(SCFT)calculations across different ensembles.By decoupling phase equilibrium determination from specific ensemble formulations,our approach enables the reuse of existing SCFT solvers.Moreover,it provides a useful framework to develop highly efficient phase equilibrium solvers for multi-component polymer systems.
基金financially supported by the National Natural Science Foundation of China (Nos. 92372126,52373203)the Excellent Young Scientists Fund Program
文摘Advancing the integration of artificial intelligence and polymer science requires high-quality,open-source,and large-scale datasets.However,existing polymer databases often suffer from data sparsity,lack of polymer-property labels,and limited accessibility,hindering system-atic modeling across property prediction tasks.Here,we present OpenPoly,a curated experimental polymer database derived from extensive lit-erature mining and manual validation,comprising 3985 unique polymer-property data points spanning 26 key properties.We further develop a multi-task benchmarking framework that evaluates property prediction using four encoding methods and eight representative models.Our re-sults highlight that the optimized degree-of-polymerization encoding coupled with Morgan fingerprints achieves an optimal trade-off between computational cost and accuracy.In data-scarce condition,XGBoost outperforms deep learning models on key properties such as dielectric con-stant,glass transition temperature,melting point,and mechanical strength,achieving R2 scores of 0.65-0.87.To further showcase the practical utility of the database,we propose potential polymers for two energy-relevant applications:high temperature polymer dielectrics and fuel cell membranes.By offering a consistent and accessible benchmark and database,OpenPoly paves the way for more accurate polymer-property modeling and fosters data-driven advances in polymer genome engineering.
基金supported by the National Natural Science Foundation of China(Nos.223B2119,U23A2083,52373014,52203129).
文摘The facile synthesis of high-valued polymers from waste molecules or low-cost common chemicals presents a significant challenge.Here,we develop a series of degradable poly(thiocarbonate)s from the new step-growth polymerization of diols,carbonyl sulfide(CoS,or carbon disulfide,CS_(2)),and dichlorides.Diols and dichlorides are common chemicals,and CoS(CS_(2))is released as industrial waste.In addition to abun-dant feedstocks,the method is efficient and performed under mild conditions,using common organic bases as catalysts,and affording unprece-dented polymers.When cos,diols,and dihalides were used as monomers,optimized conditions could completely suppress the oxygen-sulfur exchange reaction,enabling the efficient synthesis of well-defined poly(monothiocarbonate)s with melting points ranging from 48°C to 101°C.These polymers,which have a structure similar to polyethylene with low-density in-chain polar groups,exhibit remarkable toughness and ductili-ty that rival those of high-density polyethylene(melting point:90°C,tensile strength:21.6±0.7 MPa,and elongation at break:576%).Moreover,the obtained poly(monothiocarbonate)s can be chemically degraded by alcoholysis to yield small-molecule diols and dithiols.When CS_(2)was used in place of cos,a pronounced oxygen-sulfur exchange reaction occurred.By optimizing reaction condition,it was found that polymers with-S(C=O)S-and-S(C=S)S-as the main repeating units exhibited high thermal stability and crystallinity.Thus,a new approach for regulat-ing the structure of polythiocarbonates via the oxygen-sulfur exchange reaction is developed.Overall,the polymers hold great potential for green materials due to their facile synthesis,readily available feedstocks,excellent performance,and chemical degradability.
基金funded by the National Natural Science Foundation of China,grant Nos.52373275 and 52303290,received by Peng-Fei Cao and Jiayao Chen,respectively。
文摘In recent years,ultrathin polymer-based electrolytes(UPEs)have emerged as a promising strategy to enhance the energy density of rechargeable batteries for wearable devices by minimizing electrolyte volume,demonstrating higher ionic conductance and lower internal resistance,and more compact battery stacking compared to conventional thick polymer-based electrolyte.This mini review systematically summarizes recent advances in ultrathin solid-state and gel-state electrolytes,focusing on their preparation strategies,advantages,and disadvantages,where the energy density,interfacial stability,mechanical properties,and ion-transport mechanisms are also analyzed for understanding the UPE application.Moreover,the challenges such as dendrite penetration and instability(thermal,chemical and interface),along with their solutions are also introduced through interfacial engineering,polymer matrix design,and fillers incorporation.Furthermore,for practical application,the demands of working current density,operating temperature and scale-up production are also illustrated.This mini review is hoped to spark insights into improving the energy density of batteries and ultimately bring us a step closer to realizing superior rechargeable batteries.
文摘Given the increasing demand for distributed electricity,there is a burning desire to harvest electricity from renewable sources using environmentally friendly methods.Thermoelectric (TE) materials can meet this requirement not only because of their ability to convert heat directly into electricity,enabling energy harvesting from waste heat and natural heat resources,but also because more than 60%of the energy is lost as waste heat [1].The discovery of the TE effect dates back to the 1820s when T.M.Seebeck observed electricity generation at the junction of two conductors with different temperatures.Additionally,when a voltage is applied to TE materials,they can create a temperature difference to enable solid-state cooling (known as the Peltier effect).Therefore,the TE effect promises both sustainable energy solutions and temperature control technologies.Over the past two decades,the urgent demand for powering ubiquitous Internet of Things devices has sparked significant interest in flexible thermoelectrics(F-TEs),which raises an intriguing question:Is the intrinsically flexible polymer an important candidate for state-of-the-art F-TEs applications?
基金funded by the National Natural Science Foundation of China(No.82400370)the Interdisciplinary Innovation Team Incubation Project of Children’s Hospital of Fudan University(No.EKYX202416).
文摘Owing to their excellent biocompatibility and potential for durability enhancement,polymeric heart valves(PHVs)are emerging as a promising alternative to traditional prostheses.Unlike conventional materials,PHVs can be manufactured under precise design criteria,enabling targeted performance improvements.This study introduces a geometric optimization strategy for enhancing the durability of PHVs.The finite element method(FEM)is combined with a dip-molding technique to develop a novel polymeric aortic valve with improved mechanical properties.The tri-leaflet geometry is parameterized using B-spline curves,and the maximum stress in the valve is reduced from 2.4802 to 1.7773 MPa using a multiobjective optimization algorithm NSGA-II(non-dominated sorting genetic algorithm II).Pre-optimized and optimized valve prototypes were fabricated via dip-molding and evaluated during pulsatile-flow tests and accelerated wear tests.The optimized design meets the ISO 5840 standards,with an effective orifice area of 2.019 cm^(2),a regurgitant fraction of 5.693%,and a transvalvular pressure gradient of 7.576 mmHg.Moreover,the optimized valve maintained its structural integrity and functionality over 14 million cycles of the accelerated wear test,whereas the unoptimized valve failed after two million cycles.These findings confirm that the FEM-based geometric optimization method enhances both the mechanical performance and durability of PHVs.
基金supported by the National Natural Science Foundation of China(Grant No.62205103)the Natural Science Foundation of Hunan Province(Grant No.2023JJ40216)the Elite Youth Program by the Department of Education of Hunan Province(Grant No.24B0663)。
文摘Although the certified power conversion efficiency(PCE)of single-junction perovskite solar cells(PSCs)has achieved a high level of 27%,approaching the single-crystalline silicon solar cells,the device stability remains an urgent issue to be resolved for the commercialization.Defect passivation emerged as a viable approach to enhance the operational stability of the solar devices.Herein,phenylthiourea(PhTu)derivatives are selected as effective passivation agents to enhance the optoelectronic properties of printed methylammonium lead iodide(MAPbI_(3))films.It is demonstrated that incorporating a small amount of 1-(4-carboxyphenyl)-2-thiourea(PhTu-COOH)significantly reduces the trap-state density and leads to longer carrier lifetime of the perovskite films.As a result,the inverted solar device made of Ph Tu-COOH-modified MAPbI_(3) perovskite film shows remarkably improved efficiency(from 17.29%to 20.22%)and obviously increased open-circuit voltage(V_(OC))(from 1.043 to 1.143 V),as compared with the pristine device.Moreover,the Ph Tu-COOH-modified PSCs exhibit enhanced operational stability due to the significantly reduced trap-state density.Finally,the optimized solar module fabricated with an active area of 11.28 cm^(2) delivers a high PCE of 17.07%with negligible V_(OC)loss,demonstrating the feasibility of the blade-coating method for large-area perovskite film deposition.
基金financially supported by the Science and Technology Project of PetroChina Company Limited,China(No.2022DJ6314)the National Natural Science Foundation of China(No.52173056)。
文摘Dynamic melt modification of polyethylene via the direct grafting of peroxide fragments shows promise for the development of processable functionalized materials.In this study,four linear low-density polyethylenes(LLDPEs)with comparable molecular weights but different short-chain branch(SCB)contents(ranging of 5-66 per 1000 carbon atoms)were modified via dynamic melt mixing using 2 wt% benzoyl peroxide at 145℃ and 50 r/min for 30 min.The influence of SCB content on the processability and structure of the resulting products was systematically investigated.All modified products exhibited good melt processability with melt flow rates(MFR)ranging from 0.46 g/10min to 1.07 g/10min.Products derived from low-SCB LLDPEs showed a lower MFR,higher cross-linking content,a larger number of long-chain branches,and a higher degree of benzoyl grafting.In contrast,those produced from high-SCB LLDPEs exhibited improved processability,reduced cross-linking,fewer long-chain branches,and lower benzoyl grafting levels.A detailed structural investigation of the soluble and insoluble fractions,which were separated using trichlorobenzene fractionation,was conducted to analyze the structural features of various modified products and demonstrate that the SCB content(i.e.,tertiary carbon density)significantly influences radical coupling during dynamic modification.Elevated tertiary carbon density,by introducing greater steric hindrance,suppresses radical coupling during dynamic modification,thereby reducing the efficiency of both crosslinking and peroxide fragment grafting.These findings provide new insights into the structure-reactivity relationships in peroxide-induced polyethylene modification and lay the foundation for tailoring material properties via dynamic processing.
基金financially supported by the National Natural Science Foundation of China(Nos.32471396,82230071,82172098,82201716,and 61973206)the National Key R&D Program of China(No.2023YFC2411303)+4 种基金the Integrated Project of Major Research Plan of the National Natural Science Foundation of China(No.92249303)the Shanghai Committee of Science and Technology(No.23141900600,Laboratory Animal Research Project)the Shanghai Clinical Research Plan of SHDC2023CRT01the Young Elite Scientist Sponsorship Program by the China Association for Science and Technology(No.YESS20230049)the Baoshan District Health Commission Talents(Excellent Academic Leaders)Program(No.BSWSYX-2024-05)。
文摘With the rapid advancements in biomedical engineering,bioprinting has emerged as a pivotal solution to address the shortage of organ transplants and advance disease model research.The evolution of bioprinting has progressed from the fabrication of simple models(1.0)to the fabrication of permanent implants(2.0),tissue engineering scaffolds(3.0),and complex biostructures utilizing living cells(4.0).Nevertheless,significant challenges remain,particularly in accurately replicating the structure and function of host tissues,selecting appropriate materials,and optimizing printing parameters.The integration of artificial intelligence(AI),especially machine learning,provides promising novel opportunities in bioprinting(5.0).This review systematically summarizes the current applications of AI in bioprinting,discussing both construction strategies and application scenarios.It also explores the potential of AI to improve bioprinting in the preparation of complex functional tissues and in situ tissue repair.Overall,the synergy between AI and bioprinting is poised to drive the development of personalized medicine,facilitate high-throughput preparation of in vitro models,and provide robust tools for regenerative medicine and precision healthcare.
基金supported by National Program for Thousand Young Talents of China,the National Natural Science Foundation of China(Nos.51773041,21544001,21603038)Shanghai Committee of Science and Technology in China(No.18ZR1404900)Fudan University
文摘Self-healing materials have been developed over the past decade with the recovery ability after damage.However,most researches focused on the self-healing process at three-dimension.Herein,we prepare monolayer self-healing hydrogen-bond-based supramolecular polymer film and explore the self-healing process at the two-dimensional limit.The healing process,which can be reversibly repeated for at least three times,is influenced by the temperature,the molecule-substrate interaction and the substrate roughness.In the application,the monolayer self-healing polymer film can be used to modify the SiO2 dielectric for copper phthalocyanine field effect transistor with improved mobility.This work will be valuable for developing two-dimensional functional self-healing materials in the future.
基金Project supported by the National Key R&D Program of China(2017YFA0205100)。
文摘Lateral flow immunoassays(LFIAs)provide a powerful tool for rapid real-time assay of cancer biomarkers,which is vital for cancer detection and treatment follow-up.Lanthanide-based LFIAs is one of the most widely used methods,especially Eu(Ⅲ)chelates,which possess distinctive and attractive characteristics,such as time-resolved fluorescence and large Stokes shift.Herein,we adopted a new onestep mini-emulsion polymerization method to synthesize carboxyl-modified fluorescent microsphere(OS-EuCM),which shows good stability,resistance to non-specific adhesion and uniform particle size distribution compared with traditional microspheres synthesized through the swelling method.Benefiting from the above advantages,OS-EuCM was successfully used in LFIAs to detect tumor marker Alpha-fetoprotein with high sensitivity and selectivity in concentration as high as 320 ng/mL,as well as a detection limit of 0.683 ng/mL This lanthanide-based microsphere holds great potential for rapid pointof-care screening and clinical application.
基金financially supported by Chinese Ministry of Science and Technology(973 programs Nos.2009CB930000 and 2011CB606203)NSF of China(Nos.21034002,91127028 and 51273046)
文摘A facile technique is herein reported to fabricate three-dimensional （3D） polymeric porous scaffolds with interior surfaces of a topographic microstructure favorable for cell adhesion. As demonstration, a well-known biodegradable polymer poly（lactide-co-glycolide） （PLGA） was employed as matrix. Under the porogen-leaching strategy, the large and soft porogens of paraffin were modified by colliding with small and hard salt particles, which generated micropits on the surfaces of paraffin spheres. The eventual PLGA scaffolds after leaching the modified porogens had thus interior surfaces of microscale roughness imprinted by those micropits. The microrough scaffolds were confirmed to benefit adhesion of bone marrow stromal cells （BMSCs） of rats and meanwhile not to hamper the proliferation and osteogenic differentiation of the cells. The insight and technique might be helpful for biomaterial designing in tissue engineering and regenerative medicine.
基金supported by The Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning(No.TP2015002)the National Natural Science Foundation of China(No.51403099)
文摘Three-dimensional graphene/conducting polymer（3DGCP） composites have received significant attention in recent years due to their unique structures and promising applications in energy storage.With the structural diversity of graphene and π-functional conducting polymers via rich chemical routes,a number of 3DGCP composites with novel structures and attractive performance have been developed.Particularly,the hierarchical porosity,the interactions between graphene and conducting polymers as well as the their synergetic effects within 3DGCP composites can be well combined and elaborated by various synthetic methods,which made 3DGCP composites show unique electrochemical properties and significantly improved performance in energy storage fields compared to other graphenebased composites.In this short review,we present recent advances in 3DGCP composites in developing effective strategies to prepare 3DGCP composites and exploring them as a unique platform for supercapacitors with unprecedented performance.The challenges and future opportunities are also discussed for promotion of further study.
基金supported by National Program for Thousand Young Talents of Chinathe National Natural Science Foundation of China(Nos.51773041,21544001,21603038)+1 种基金Shanghai Committee of Science and Technology in China(No.18ZR1404900)Fudan University。
文摘Recent development of self-healing material has attracted tremendous attention,owing to its biomimetic ability to restore structure and functionality when encountering damages.Here,we develop a threedimensional(3D)printable self-healing composite conductive polymer by mixing hydrogen-bond-based supramolecular polymer with low-cost carbon black.It has a room-temperature self-healing capability in both conductivity and mechanical property,while its shear-thinning behavior enables fabrication of a self-healable circuit by 3D printing technology.As an application,the circuit shows an excellent temperature-dependent behavior of the resistance,indicating its great potential fo r practical application in the artificial intelligence field.
基金Supported by FONDECYT(Project no.1150510)PIA(Anillo ACT-130)+4 种基金7FP-MC Actions Grant,REDOC(MINEDUC Project UCO1202 at U.de Concepción)CHILTURPOL2(PIRSES-GA-2009 Project,Grant No.269153)the Marie Curie Program(n°269153)FONDECYT Grant No.11140324CIPA(No.20301.934.15),Chile
文摘Modifying polypropylene membranes with interpenetrating polymer networks(IPNs) through the incorporation of poly(glycidyl methacrylate-N-methyl-D-glucamine)(P(GMA-NMG)) was performed by in situ synthesis via radical polymerization. The surface of the polypropylene membrane was activated by hydrophilic grafted polyelectrolyte, and then, pressure injection was used for the impregnation of the reactive solution in the membrane.Two types of pore-filled membranes were synthesized, chelating interpenetrating homopolymer networks of P(GMA-NMG), and chelating-ion exchange interpenetrating polymer networks(e.g., P(GMA-NMG)/P(AA),P(GMA-NMG)/P(AMPSA), and P(GMA-NMG)/P(Cl VBTA)). After their synthesis, the modified polypropylene membranes were characterized using techniques such as the electrokinetic potential, SEM, FT-IR, and Donnan dialysis to corroborate the chromium ion transport. The P(GMA-NMG) and complex network membranes exhibited a hydrophilic character with a water-uptake capacity between 20% and 35% and a percentage of modification between 4.0% and 7.0% in comparison with the behavior of the unmodified polypropylene membrane.Hexavalent chromium ions were efficiently transported from the food chamber at p H 9.0 when the 65.2%MTA1 P(Cl VBTA) homopolymer IPN membrane and 48.5% MTAG P(GMA-NMG)/P(Cl VBTA) IPN membrane were used. Similarly, hexavalent chromium ions were removed from the food chamber at pH 3.0 when MTAG(63.30%) and MTA1(35.68%) were used in 1 mol·L^(-1)Na Cl solution as the extraction reagent.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.21704016 and 21971044).
文摘Photo-controlled reversible-deactivation radical polymerizati on(photo-RDRP)has been investigated as a"green"and spatiotem-porally controlling pathway for polymer synthesis.While the combination of photo-RDRP and flow chemistry has offered opportunities to increase light intensity and enable uniform light irradiation,problems associated with flow approaches still remain for photoflow-RDRP,which has hindered merging flow polymerization with other cutting-edge techniques.Herein,we summarize challenges and recent achievements in photoflow-RDRP including the development of(a)droplet/slug-flow to regulate reside nee time distribution,(b)mixing techniques to tailor polymer,(c)polymerization in duced self-assembly,and(d)computer-aided synthesis.We hope this work will provide in formative knowledge to people in related fields and stimulate novel ideas to promote polymer synthesis in both academia and industry.
基金the National Natural Science Foundation of China(Nos.21704017,21871056,and 91956122).
文摘The activation and deactivation of the chain-transfer agent were achieved by oxygen initiation and regulation with triethylborane under ambient temperature and atmosphere.The autoxidation of triethylborane overcame the oxygen inhilbition and produced initiating radicals that selectively activate the chain-transfer agent for the chain growth or deactivate the active chain-end of polymer in controlled radical polymerization.Both activation and deactivation were highly efficient with broad scope for various polymers with different chain-transfer agents in both organic and aqueous systems.Oxygen molecule was particularly used as an external regulator to initiate and achieve the temporal control of both activation and deactivation by simply feeding the air.
基金financially supported by the National Natural Science Foundation of China(Nos.21674022 and 51703034)
文摘Biological stimuli-responsive polymers have increasingly attracted attention in recent years because it can satisfy many requirements of applications related with human body while traditional systems do not meet.Due to the importance of this burgeoning field,great efforts have been devoted and,up to now,polymer chemists have made a remarkable success in this prospective research topic.In this review,we systematically generalize the present state of biological stimuli-responsive polymer systems.We highlight several representative examples to specify the current problems and look ahead a clear sense of direction in this area.
文摘Heterogeneous membranes were obtained by using styrene-acrylonitrile copolymer（SAN）blends with low content of ion-exchanger particles（5 wt.%）. The membranes obtained by phase inversion were used for the removal of copper ions from synthetic wastewater solutions by electrodialytic separation. The electrodialysis was conducted in a three cell unit, without electrolyte recirculation. The process, under potentiostatic or galvanostatic control, was followed by p H and conductivity measurements in the solution. The electrodialytic performance,evaluated in terms of extraction removal degree（rd） of copper ions, was better under potentiostatic control then by the galvanostatic one and the highest（over 70%） was attained at8 V. The membrane efficiency at small ion-exchanger load was explained by the migration of resin particles toward the pores surface during the phase inversion. The prepared membranes were characterized by various techniques i.e. optical microscopy, Fourier transform infrared spectroscopy, scanning electron microscopy, thermogravimetric analysis and differential thermal analysis and contact angle measurements.
文摘An optimized and high-performance Monte Carlo simulation is developed to take thorough account of four different cases of termination in styrene ATRP. According to the simulation results, the bimolecular termination rate constant sharply drops throughout the polymerization when either chain-length dependency of termination rate constant, gel effect, or both together is applied to the simulation. In addition, as expected, the initiator is quickly decomposed at the early stages of the polymerization. The concentration of the catalyst in lower oxidation state decreases at first and then plateaus at higher conversion; furthermore, the steady concentration of Ml^nY/L in the polymerization is the highest when the chain-lengthdependent diffusion-controlled termination rate constant is employed in the simulation. The rates of deactivation and chain end degradation reactions are also smaller in this case. Therefore, the fraction of dormant chains is higher throughout the reaction and consequently the portion of dead polymers decreases. Besides, molecular weight increases linearly with conversion; however, when neither gel effect nor chain-length dependency of termination rate constant is considered, the molecular weight deviates from linearity at the end of the reaction. The peak of chain length distribution shifts toward higher molecular weight too during the reaction. Finally, the molecular weight distribution broadens at higher conversion; however, the chain length distribution of polymers produced under conditions of applying chain-length-dependent diffusion-controlled termination rate constant is narrower.
