In this work,we report a fabrication of recyclable iron oxide decorated MoS_(2)nanosheets via a facile liq-uid exfoliation approach and solvothermal reaction for visible-light photodegradation of tetracycline.The prep...In this work,we report a fabrication of recyclable iron oxide decorated MoS_(2)nanosheets via a facile liq-uid exfoliation approach and solvothermal reaction for visible-light photodegradation of tetracycline.The prepared Fe_(3)O_(4)-MoS_(2)was characterized by X-ray diffraction,transmission electron microscopy,X-ray photoelectron spectros-copy,Raman spectroscopy,magnetic hysteresis,and nitrogen adsorption-desorption isotherms.Experimental results indicate that,successful attachment of Fe_(3)O_(4)nanoparticles to MoS_(2)sheets has been achieved.The enhanced surface area of Fe_(3)O_(4)-MoS_(2)induced high rates of adsorption and the adsorbed tetracycline was degraded to 90%after 150 min of visible exposure,which is better than that from pure MoS_(2).The introduction of Fe_(3)O_(4)not only enhances the photo-catalytic performance of Fe_(3)O_(4)-MoS_(2),but also enables its convenient recovery from water by an external magnetic field.Furthermore,both the photocatalytic activity and composite phase of Fe_(3)O_(4)-MoS_(2)were well-retained over cy-cles.Owing to its efficient photocatalytic activity,good stability and magnetic recyclability,the Fe_(3)O_(4)-MoS_(2)nano-composite is considered to be a promising photocatalyst for wastewater treatment.展开更多
The advancement of functional adhesives featuring recyclable and repairable properties is of great significance in interfacial science and engineering.Herein,a series of high-strength,recyclable fluorine-containing ad...The advancement of functional adhesives featuring recyclable and repairable properties is of great significance in interfacial science and engineering.Herein,a series of high-strength,recyclable fluorine-containing adhesives(ESOx-FPF)were designed and synthesized by crosslinking two prepolymers,FPF-B(derived from side-chain fluorinated diol,isocyanate,and aminoboric acid)and ESO-B(synthesized from biobased epoxy soybean oil and aminoboric acid),through dynamic boro-oxygen bonds.The resulting adhesive exhibited an optimal tensile strength of 42 MPa and the shear strength on steel plates reached as high as 3.89 MPa.More importantly,benefiting from the dynamic reversibility of the boron-oxygen bonds along with the hydrogen bonds interaction,ESOx-FPF can be welded with the assistance of solvents and recycled for multiple cycles.The outstanding healing efficiency and excellent reprocessability of these functional adhesives were confirmed by mechanical testing.Moreover,the as-prepared adhesives demonstrated universal and remarkable adhesion to various substrates,such as aromatic polyamide,aluminum plates and polycarbonate,meanwhile,they could be easily disassembled and recycled using ethanol without damaging the substrates surface.This study not only provides a simple strategy for the synthesis of eco-friendly adhesives with weldable and recyclable properties,but also sheds light on the development of other functional materials utilizing dynamic covalent chemistry.展开更多
Polyurethane is widely used for its versatility in design and range of performance.Self-healing and recyclable dynamic polyurethane networks have attracted extensive attention due to their potential to extend service ...Polyurethane is widely used for its versatility in design and range of performance.Self-healing and recyclable dynamic polyurethane networks have attracted extensive attention due to their potential to extend service life and ensure safety in use,as well as to promote sustainable use of resources.Developing green and environment-friendly methods to obtain this material is an interesting and challenging task,as the majority of current dynamic polyurethane networks utilize the solution polymerization method.The use of solvents makes the processes complicated,harmful to environment,and increase the cost.Poly(oxime-urethanes)(POUs)are emerging dynamic polyurethanes and show great potential in diverse fields,such as biomaterials,hot melt adhesives,and flexible electronics.In this study,we utilized the solubility properties of dimethylglyoxime in raw material poly(ethylene glycol)to prepare POUs through bulk polymerization for the first time.This method is simple,convenient and cost-efficient.Simultaneously,copper ion coordination improves POUs strength and dynamic properties,with mechanical strength up from 0.54 MPa to 1.03 MPa and self-healing recovery rate up from 85.5%to 91.8%,and activation energy down from 119.6 k J/mol to 95.4 k J/mol.To demonstrate the application of this technology,self-healing and stretchable circuits are constructed from this dynamic polyurethane network.展开更多
The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of society.Since the existence of dynamic chemical bonds in vitrimers often reduces both the ther...The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of society.Since the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine solution.This study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.展开更多
Earth abundant metals are much less expensive,promising,valuable metals and could be served as catalysts for the borrowing hydrogen reaction,dehydrogenation and heterocycles synthesis,instead of noble metals.The unifo...Earth abundant metals are much less expensive,promising,valuable metals and could be served as catalysts for the borrowing hydrogen reaction,dehydrogenation and heterocycles synthesis,instead of noble metals.The uniformly dispersed zinc composites were designed,synthesized and carefully characterized by means of XPS,EDS,TEM and XRD.The resulting zinc composite showed good catalytic activity for the N-alkylation of amines with amines,ketones with alcohols in water under base-free conditions,while unsaturated carbonyl compounds could also be synthesized by tuning the reaction conditions.Importantly,it was the first time to realize the synthesis of 2-aryl-1H-benzo[d]imidazole derivatives by using this zinc composite under green conditions.Meanwhile,this zinc catalyst could be easily recovered and reused for at least five times.展开更多
With the increasing consumption of non renewable resources such as oil,the traditional polymer manufacturing industry that relies on fossil resources is facing unprecedented challenges.The design,synthesis,and recycli...With the increasing consumption of non renewable resources such as oil,the traditional polymer manufacturing industry that relies on fossil resources is facing unprecedented challenges.The design,synthesis,and recycling of renewable and environmentally friendly bio-based polymers as alternatives to petroleum based polymers have become hot topics in research and industrial fields.Biomass has been used as a raw material to design and synthesize closed-loop recyclable polymers,which is of great significance in addressing the waste of resources and negative impact on the environment in the traditional polymer preparation process.This review summarized recent advances in the design,synthesis,and properties of closed-loop recyclable bio-based polymers,focusing on the sustainability and recyclability of bio-based materials,followed by a brief discussion of the potential applications of closed-loop recyclable bio-based polymers in emerging applications such as 3D printing and friction electric nanogenerators.In addition,perspectives and recommendations for future research on closedloop recyclable bio-based polymers were presented.展开更多
The development of degradable and chemically recyclable polymers is a promising strategy to address pressing environmental and resource-related challenges.Despite significant progress,there is a need for continuous de...The development of degradable and chemically recyclable polymers is a promising strategy to address pressing environmental and resource-related challenges.Despite significant progress,there is a need for continuous development of such recyclable polymers.Herein,PPDOPLLA-PU copolymers were synthesized from poly(p-dioxanone)-diol(PPDO-diol)and poly(L-lactide)-diol(PLLA-diol)by chain extension reaction.The chemical structures and microphase structures of PPDO-PLLA-PU were characterized,and their crystalline properties,mechanical properties,and degradation behaviors were further investigated.Significantly,the distribution of PLLA phase in the copolymer matrix showed a rod-like microstructure with a slight orientation,despite the thermodynamic incompatibility of PPDO and PLLA segments.Moreover,on the basis of this microphase separation,PPDO spherulites can crystallize using the interface of the two phases as nucleation sites.Accordingly,the combined effect of above two contributes to the enhanced mechanical properties.In addition,PPDO-PLLA-PU copolymers have good processability and recyclability,making them valuable for a wide range of applications.展开更多
Chemically recyclable polythioesters are of particular interest owing to their unique properties and desired sustainability.By the exploit of a benzo-fusion strategy toε-thiocaprolactone,we successfully improved the ...Chemically recyclable polythioesters are of particular interest owing to their unique properties and desired sustainability.By the exploit of a benzo-fusion strategy toε-thiocaprolactone,we successfully improved the chemical recyclability and regulated the thermal and mechanical properties of the resulting polythioesters.The efficient ring-opening polymerization(ROP)of benzo-fused thiolactone monomers(M)containing different substituents gave rise to high-molecular-weight semi-aromatic polythioesters P(M)s.The resulting P(M)s showcased tunable physical and mechanical properties.The debenzylation of P(M3)was able to generate P(M3-OH)with free hydroxyl sidechains.Notably,chemical recycling of the resulting P(M)s back to their corresponding monomers via bulk thermal depolymerization achieved high efficiency(>95%yield,99%purity),establishing a closed-loop lifecycle.展开更多
The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel ap...The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel approach involving the development of iron-based ionic liquids as photocatalysts has been pursued for the first time,with the goal of simultaneously facilitating the LMCT process and addressing the issue of photocatalyst recovery.Remarkably,the iron-based ionic liquid 1-butyl-3-methylimidazolium tetrachloroferrate(C_(4)mim-Fe Cl_(4))demonstrates exceptional recyclability and stability for the photocatalytic hydroacylation of olefins.This study will pave the way for new approaches to photocatalytic organic synthesis using ionic liquids as recyclable photocatalysts.展开更多
Elastomers are widely used in various fields owing to their excellent tensile properties.Recyclable and self-healing properties are key to extending the service life of elastomers.Accumulating evidence indicates that ...Elastomers are widely used in various fields owing to their excellent tensile properties.Recyclable and self-healing properties are key to extending the service life of elastomers.Accumulating evidence indicates that dynamic covalent chemistry has emerged as a powerful tool for constructing recyclable and self-healing materials.In this work,we demonstrate the preparation of a recyclable and self-healable polydimethylsiloxane(PDMS)elastomer based on the Knoevenagel condensation(KC)reaction.This PDMS elastomer was prepared by the KC reaction catalyzed by 4-dimethylaminopyridine(DMAP).The obtained PDMS elastomer exhibited an elongation at break of 266%,a tensile strength of 0.57 MPa,and a good thermal stability(Td=357℃).In addition,because of the presence of dynamic C=C bonds formed by the KC reaction and low glass transition temperature(Tg=-117℃).This PDMS exhibited good self-healing and recycling properties at room temperature and could be reprocessed by hot pressing.In addition,the PDMS elastomer exhibits good application prospects in the fields of adhesives and flexible electronic devices.展开更多
Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains...Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.展开更多
Flexible phase change materials(PCMs)have become increasingly critical to address the demand for thermal management in electronic technologies and energy conversion.However,their application remains challenging becaus...Flexible phase change materials(PCMs)have become increasingly critical to address the demand for thermal management in electronic technologies and energy conversion.However,their application remains challenging because of their rigidity,liquid leakage,and insufficient thermal conductivity.Herein,flexible glutamic acid@natural rubber/paraffin wax(PW)/carbon nanotubes-graphene nanoplatelets(GNR/PW/CGNP)phase change composites with high thermal conductivity,excellent shape stability,and recyclability were reported.Zn^(2+)-based dynamic crosslinking was constructed through the reaction of zinc acetate and carboxyl groups on glutamic acid@natural rubber(GNR),which was used as a flexible matrix to physically blend with paraffin wax/carbon nanotubes/graphene nanoplatelets(PW/CGNP)to achieve uniform dispersion of PW/CGNP,continuous thermal conductivity networks,and good encapsulation of PW.The GNR/PW/CGNP composites showed excellent mechanical strength,flexibility,and recycling ability,and effective encapsulation prevented the outflow of melted PW during the phase transition.Also,the phase change enthalpy could attain 111.1 J/g with a higher thermal conductivity of 1.055 W/m K,428%higher than that of pure PW owing to the formation of efficient thermal conductive pathways,which exhibited outstanding thermal management performance and superior temperature control behavior in electronic devices.The developed flexible composite PCMs may open new possibilities for next-generation flexible thermal management electronics.展开更多
Polymers that exhibit both biodegradability and chemical recyclability offer a promising solution to environmental pollution and resource scarcity. Poly(glycolic acid)(PGA) is a promising chemically recyclable polymer...Polymers that exhibit both biodegradability and chemical recyclability offer a promising solution to environmental pollution and resource scarcity. Poly(glycolic acid)(PGA) is a promising chemically recyclable polymer, characterized by its seawater degradability and high mechanical strength. In this study, aliphatic polycarbonates were synthesized through melt polycondensation and subsequently copolymerized with glycolide(GL) to produce chemically recyclable PGA based triblock copolymers with well-defined structures. The properties of these copolymers, including their thermal properties, crystallization behavior, and mechanical performance, can be effectively adjusted by modifying the structure and content of the middle block. Furthermore, an in-depth investigation reveals that the pyrolysis process involves ester exchange, radical, and back-biting reactions. In addition, the high-efficiency "Monomer↔Copolymer" chemical recycling loop has been established, achieving a remarkable yield exceeding 88% along with a purity greater than 99%.展开更多
Most commercial plastics cannot easily degrade,which raises a number of sustainability issues.To address the current problem of plastic pollution,the research and development of easily degradable and recyclable polyme...Most commercial plastics cannot easily degrade,which raises a number of sustainability issues.To address the current problem of plastic pollution,the research and development of easily degradable and recyclable polymers has become an attractive subject.Herein,a new monomer of thiosalicylic methyl glycolide(TSMG)was synthesized using one-pot method and high molecular weight poly(thiosalicylic methyl glycolide)(PTSMG,M_(n) up to 300 kDa)can be obtained via the ring-opening polymerization(ROP)of TSMG.PTSMG exhibits good closed-loop recyclability and hydrolytic degradability,where PTSMG can generate pristine monomers through sublimation thermal depolymerization conditions due to the presence of thiophenol ester bond in the polymer chains,and can be degraded rapidly in aqueous solution,which provides a potential solution to the current plastic pollution problem.展开更多
Despite their high-energy conversion efficiency that has earned them the label of next-generation energy utilization devices,protonic ceramic fuel cells(PCFCs)have not yet fully fulfilled their potential in terms of l...Despite their high-energy conversion efficiency that has earned them the label of next-generation energy utilization devices,protonic ceramic fuel cells(PCFCs)have not yet fully fulfilled their potential in terms of low-cost integration and environmentally friendly application,which remain significant concerns that heavily influence their progress towards commercial viability.A pragmatic way of cell recycling is extremely helpful for addressing these concerns.Herein,we unveil a novel concept of reusable PCFCs,and propose a comprehensive recycling scheme for discarded PCFCs.In this research,a recycled cell with a recycled single perovskite cathode exhibited a peak power density(PPD)of 1.10 W cm^(-2)at 700℃,comparable to a pristine cell of 1.05 W cm^(-2).Metal ion rearrangement and phase evolution during the recycling processes were investigated,which were demonstrated to be in high relevance to the performance of recycled cells.This research constitutes a pioneering exploration of the mechanisms underlying recycling efforts and offers valuable insights into the material recycling of solid-state functional devices used for energy conversion and storage.展开更多
The“2025 China New-Formulation Detergent Products Development Conference & 2025 China Daily Chemicals Biodegradable,Recyclable,Renewable Technology Innovation Summit”,cohosted by the China Research Institute of ...The“2025 China New-Formulation Detergent Products Development Conference & 2025 China Daily Chemicals Biodegradable,Recyclable,Renewable Technology Innovation Summit”,cohosted by the China Research Institute of Daily Chemical(RIDCI),was held in Yangzhou,Jiangsu Province.The event brought together over 230 representatives from government agencies,industry associations,and leading enterprises to contribute insights for the high-quality development of China's daily chemical industry.展开更多
Nickel-catalyzed borylation of aryl nonaflates with B2pin2 could be realized,which proceeded effectively by means of C—O bond functionalization to afford a wide variety of valuable arylboronates in moderate to excell...Nickel-catalyzed borylation of aryl nonaflates with B2pin2 could be realized,which proceeded effectively by means of C—O bond functionalization to afford a wide variety of valuable arylboronates in moderate to excellent yields with good functionality compatibility.In addition,the gram-scale synthesis and the application of the approach in the late-stage elaboration of aryl nonaflate derived from pterostilbene could also be achieved.展开更多
To address the longstanding challenge in traditional carborane methodology of rapidly and efficiently constructing carboranyl-based polycyclic frameworks,Pd-catalyzed one-pot reactions between pyridyl-substituted nido...To address the longstanding challenge in traditional carborane methodology of rapidly and efficiently constructing carboranyl-based polycyclic frameworks,Pd-catalyzed one-pot reactions between pyridyl-substituted nidocarboranes and alkynes directly afford two distinct types of 2D-3D fused carboranyl polycyclic compounds:3a-3f,4a-4d.The structures of this series of compounds were characterized by nuclear magnetic resonance spectroscopy,single-crystal X-ray diffraction,and high-resolution mass spectrometry,and a plausible reaction mechanism was proposed.Crystal structures reveal that the multiple rings in such 2D-3D fused carboranyl polycyclic compounds exhibit a certain degree of coplanarity.Furthermore,these compounds exhibited properties distinct from those of conventional 2D polycyclic systems.CCDC:2481988,3c,2481990,3f,2481986,4d.展开更多
A multi-stimuli-responsive hydrogel,P(VI-co-MAAC-NE),was successfully constructed by covalently integrating the aggregation-induced emission(AIE)moiety(Z)-N-(4-(1-cyano-2-(4-(diethylamino)phenyl)vinyl)-phenyl)methacry...A multi-stimuli-responsive hydrogel,P(VI-co-MAAC-NE),was successfully constructed by covalently integrating the aggregation-induced emission(AIE)moiety(Z)-N-(4-(1-cyano-2-(4-(diethylamino)phenyl)vinyl)-phenyl)methacrylamide(NE)into a dynamic hydrogen-bonding network composed of 1-vinylimidazole(VI)and methacrylic acid(MAAC)groups.The dense hydrogen-bonding network not only provides enhanced mechanical robustness,but also significantly enhances the AIE effect of NE by restricting its molecular motion.Under various external stimuli,the hydrogen bonds within the hydrogel network undergo reversible dissociation and reformation,thus enabling synergistic modulation of the hydrogel’s mechanical properties and luminescence behavior.Specifically,organic solvents disrupt the hydrogen-bonding network and the aggregation of the AIE moiety NE,resulting in macroscopic swelling and fluorescence quenching of the hydrogel.In strongly acidic conditions,protonation of NE molecules suppresses the intramolecular charge transfer(ICT)process,yielding a blue-shifted emission band accompanied by intense blue fluorescence;in highly alkaline environments,deprotonation of carboxyl groups induces hydrogel swelling and disperses NE aggregates,leading to pronounced fluorescence quenching.Moreover,the system exhibits thermally activated shape-memory behavior:heating above the glass transition temperature(T_(g):ca.62℃)softens the hydrogel to allow programmable reshaping,and subsequent hydrogen bond reformation at ambient conditions locks in the resultant geometries without sacrificing the hydrogel’s fluorescence performance.By capitalizing on these multi-stimuli-responsive characteristics and shape-memory behavior,the potential of hydrogel P(VI-co-MAAC-NE)for advanced information encryption and anti-counterfeiting applications is demonstrated.This work not only provides a versatile material platform for sensing and information storage,but also offers new insights into the design of intelligent soft materials integrating AIE features with dynamically regulated supramolecular network structures.展开更多
The global energy landscape is undergoing a profound transformation,with wind energy,especially wind power,gaining increasing prominence due to its clean,renewable nature.However,as the installed capacity of wind powe...The global energy landscape is undergoing a profound transformation,with wind energy,especially wind power,gaining increasing prominence due to its clean,renewable nature.However,as the installed capacity of wind power continues to expand,the disposal of waste wind turbine blades(WWTB)has emerged as a significant challenge.These blades are predominantly composed of epoxy resin(EP)polymers,carbon fibers(CFs),and glass fibers(GFs).Improper disposal not only exacerbates environmental concerns but also leads to the loss of valuable resources,particularly carbon-based materials.Pyrolysis technology,a versatile and environmentally sustainable method for resource recovery,has garnered considerable attention in the context of WWTB disposal.This work presents a comprehensive review of the pyrolytic recycling of WWTB,focusing on the principles and classifications of pyrolysis technology,key factors influencing the pyrolysis process,as well as the pyrolysis methods,equipment,products,and their applications.Through an in-depth analysis of the current research on the pyrolytic recycling of WWTB,this review identifies critical unresolved issues in the field and provides a forward-looking perspective on emerging research trends.展开更多
文摘In this work,we report a fabrication of recyclable iron oxide decorated MoS_(2)nanosheets via a facile liq-uid exfoliation approach and solvothermal reaction for visible-light photodegradation of tetracycline.The prepared Fe_(3)O_(4)-MoS_(2)was characterized by X-ray diffraction,transmission electron microscopy,X-ray photoelectron spectros-copy,Raman spectroscopy,magnetic hysteresis,and nitrogen adsorption-desorption isotherms.Experimental results indicate that,successful attachment of Fe_(3)O_(4)nanoparticles to MoS_(2)sheets has been achieved.The enhanced surface area of Fe_(3)O_(4)-MoS_(2)induced high rates of adsorption and the adsorbed tetracycline was degraded to 90%after 150 min of visible exposure,which is better than that from pure MoS_(2).The introduction of Fe_(3)O_(4)not only enhances the photo-catalytic performance of Fe_(3)O_(4)-MoS_(2),but also enables its convenient recovery from water by an external magnetic field.Furthermore,both the photocatalytic activity and composite phase of Fe_(3)O_(4)-MoS_(2)were well-retained over cy-cles.Owing to its efficient photocatalytic activity,good stability and magnetic recyclability,the Fe_(3)O_(4)-MoS_(2)nano-composite is considered to be a promising photocatalyst for wastewater treatment.
基金financially supported by the Natural Science Foundation of Shandong Province(No.ZR2022MB034)。
文摘The advancement of functional adhesives featuring recyclable and repairable properties is of great significance in interfacial science and engineering.Herein,a series of high-strength,recyclable fluorine-containing adhesives(ESOx-FPF)were designed and synthesized by crosslinking two prepolymers,FPF-B(derived from side-chain fluorinated diol,isocyanate,and aminoboric acid)and ESO-B(synthesized from biobased epoxy soybean oil and aminoboric acid),through dynamic boro-oxygen bonds.The resulting adhesive exhibited an optimal tensile strength of 42 MPa and the shear strength on steel plates reached as high as 3.89 MPa.More importantly,benefiting from the dynamic reversibility of the boron-oxygen bonds along with the hydrogen bonds interaction,ESOx-FPF can be welded with the assistance of solvents and recycled for multiple cycles.The outstanding healing efficiency and excellent reprocessability of these functional adhesives were confirmed by mechanical testing.Moreover,the as-prepared adhesives demonstrated universal and remarkable adhesion to various substrates,such as aromatic polyamide,aluminum plates and polycarbonate,meanwhile,they could be easily disassembled and recycled using ethanol without damaging the substrates surface.This study not only provides a simple strategy for the synthesis of eco-friendly adhesives with weldable and recyclable properties,but also sheds light on the development of other functional materials utilizing dynamic covalent chemistry.
基金the National Key Research and Development Program of China(No.2021YFC2101800)the National Natural Science Foundation of China(Nos.52173117 and 21991123)+3 种基金the Natural Science Foundation of Shanghai(No.20ZR1402500)Belt&Road Young Scientist Exchanges Project of Science and Technology Commission Foundation of Shanghai(No.20520741000)Ningbo 2025 Science and Technology Major Project(No.2019B10068)the Science and Technology Commission of Shanghai(No.20DZ2254900)。
文摘Polyurethane is widely used for its versatility in design and range of performance.Self-healing and recyclable dynamic polyurethane networks have attracted extensive attention due to their potential to extend service life and ensure safety in use,as well as to promote sustainable use of resources.Developing green and environment-friendly methods to obtain this material is an interesting and challenging task,as the majority of current dynamic polyurethane networks utilize the solution polymerization method.The use of solvents makes the processes complicated,harmful to environment,and increase the cost.Poly(oxime-urethanes)(POUs)are emerging dynamic polyurethanes and show great potential in diverse fields,such as biomaterials,hot melt adhesives,and flexible electronics.In this study,we utilized the solubility properties of dimethylglyoxime in raw material poly(ethylene glycol)to prepare POUs through bulk polymerization for the first time.This method is simple,convenient and cost-efficient.Simultaneously,copper ion coordination improves POUs strength and dynamic properties,with mechanical strength up from 0.54 MPa to 1.03 MPa and self-healing recovery rate up from 85.5%to 91.8%,and activation energy down from 119.6 k J/mol to 95.4 k J/mol.To demonstrate the application of this technology,self-healing and stretchable circuits are constructed from this dynamic polyurethane network.
基金financially supported by the National Natural Science Foundation of China (Nos.51973118, 22175121,52003160 and 22001175)Key-Area Research and Development Program of Guangdong Province (Nos.2019B010941001 and2019B010929002)+7 种基金the Natural Science Foundation of Guangdong Province (No.2020A1515010644)the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2019ZT08C642)Shenzhen Science and Technology Program (Nos.JCYJ20220818095810022, JSGGZD20220822095201003 and JCYJ20210324095412035)the start-up fund of Shenzhen University (No.000002110820)the Guangdong Natural Science Foundation (Nos.2022A1515011781 and2021A1515110086)Science and Technology Innovation Commission of Shenzhen,China (Nos.RCBS20200714114910141 and JCYJ20210324132816039)the Start-up Grant at Harbin Institute of Technology (Shenzhen),China (Nos.HA45001108 and HA11409049)Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application (No.ZDSYS20220527171407017)。
文摘The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of society.Since the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine solution.This study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.
基金financial support of this work by the National Natural Science Foundation of China(Nos.21776111,21861039)State Key Laboratory of Pulp and Paper Engineering(No.202001)Central Laboratory,School of Chemical and Material Engineering,Jiangnan University。
文摘Earth abundant metals are much less expensive,promising,valuable metals and could be served as catalysts for the borrowing hydrogen reaction,dehydrogenation and heterocycles synthesis,instead of noble metals.The uniformly dispersed zinc composites were designed,synthesized and carefully characterized by means of XPS,EDS,TEM and XRD.The resulting zinc composite showed good catalytic activity for the N-alkylation of amines with amines,ketones with alcohols in water under base-free conditions,while unsaturated carbonyl compounds could also be synthesized by tuning the reaction conditions.Importantly,it was the first time to realize the synthesis of 2-aryl-1H-benzo[d]imidazole derivatives by using this zinc composite under green conditions.Meanwhile,this zinc catalyst could be easily recovered and reused for at least five times.
基金Natural Science Foundation of China(Grant Nos.32471815 and 32401528)Natural Science Foundation of Jiangsu Province of China(Grant Nos.BK20241745 and BK20240294).
文摘With the increasing consumption of non renewable resources such as oil,the traditional polymer manufacturing industry that relies on fossil resources is facing unprecedented challenges.The design,synthesis,and recycling of renewable and environmentally friendly bio-based polymers as alternatives to petroleum based polymers have become hot topics in research and industrial fields.Biomass has been used as a raw material to design and synthesize closed-loop recyclable polymers,which is of great significance in addressing the waste of resources and negative impact on the environment in the traditional polymer preparation process.This review summarized recent advances in the design,synthesis,and properties of closed-loop recyclable bio-based polymers,focusing on the sustainability and recyclability of bio-based materials,followed by a brief discussion of the potential applications of closed-loop recyclable bio-based polymers in emerging applications such as 3D printing and friction electric nanogenerators.In addition,perspectives and recommendations for future research on closedloop recyclable bio-based polymers were presented.
基金financially supported by the National Key R&D Program of China(No.2021YFB3801901)the National Natural Science Foundation of China(Nos.52403138 and U19A2095)+1 种基金Institutional Research Fund from Sichuan University(No.2020SCUNL205)Fundamental Research Funds for the Central Universities,and 111 Project(No.B20001)。
文摘The development of degradable and chemically recyclable polymers is a promising strategy to address pressing environmental and resource-related challenges.Despite significant progress,there is a need for continuous development of such recyclable polymers.Herein,PPDOPLLA-PU copolymers were synthesized from poly(p-dioxanone)-diol(PPDO-diol)and poly(L-lactide)-diol(PLLA-diol)by chain extension reaction.The chemical structures and microphase structures of PPDO-PLLA-PU were characterized,and their crystalline properties,mechanical properties,and degradation behaviors were further investigated.Significantly,the distribution of PLLA phase in the copolymer matrix showed a rod-like microstructure with a slight orientation,despite the thermodynamic incompatibility of PPDO and PLLA segments.Moreover,on the basis of this microphase separation,PPDO spherulites can crystallize using the interface of the two phases as nucleation sites.Accordingly,the combined effect of above two contributes to the enhanced mechanical properties.In addition,PPDO-PLLA-PU copolymers have good processability and recyclability,making them valuable for a wide range of applications.
基金financially supported by the National Key R&D Program of China(No.2021YFA1501700)the National Natural Science Foundation of China(Nos.22371194 and 22301197)Fundamental Research Funds from Sichuan University(Nos.2023SCUNL103 and 2024SCUQJTX005)。
文摘Chemically recyclable polythioesters are of particular interest owing to their unique properties and desired sustainability.By the exploit of a benzo-fusion strategy toε-thiocaprolactone,we successfully improved the chemical recyclability and regulated the thermal and mechanical properties of the resulting polythioesters.The efficient ring-opening polymerization(ROP)of benzo-fused thiolactone monomers(M)containing different substituents gave rise to high-molecular-weight semi-aromatic polythioesters P(M)s.The resulting P(M)s showcased tunable physical and mechanical properties.The debenzylation of P(M3)was able to generate P(M3-OH)with free hydroxyl sidechains.Notably,chemical recycling of the resulting P(M)s back to their corresponding monomers via bulk thermal depolymerization achieved high efficiency(>95%yield,99%purity),establishing a closed-loop lifecycle.
基金financial support from the National Natural Science Foundation of China(Nos.22071222,22171249)the Natural Science Foundation of Henan Province(Nos.232300421363,242300420526)+2 种基金Key Research Projects of Universities in Henan Province(No.23A180010)Science&Technology Innovation Talents in Universities of Henan Province(No.23HASTIT003)Science and Technology Research and Development Plan Joint Fund of Henan Province(No.242301420006)。
文摘The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel approach involving the development of iron-based ionic liquids as photocatalysts has been pursued for the first time,with the goal of simultaneously facilitating the LMCT process and addressing the issue of photocatalyst recovery.Remarkably,the iron-based ionic liquid 1-butyl-3-methylimidazolium tetrachloroferrate(C_(4)mim-Fe Cl_(4))demonstrates exceptional recyclability and stability for the photocatalytic hydroacylation of olefins.This study will pave the way for new approaches to photocatalytic organic synthesis using ionic liquids as recyclable photocatalysts.
基金supported by the National Natural Science Foundation of China(Nos.51973025 and 52222307)Jilin Science and Technology Bureau(Nos.20220204107YY and 20230204086YY)+1 种基金Changchun Science and Technology Bureau(No.21ZGY06)Jilin Province Development and Reform Commission(No.2023C028-4).
文摘Elastomers are widely used in various fields owing to their excellent tensile properties.Recyclable and self-healing properties are key to extending the service life of elastomers.Accumulating evidence indicates that dynamic covalent chemistry has emerged as a powerful tool for constructing recyclable and self-healing materials.In this work,we demonstrate the preparation of a recyclable and self-healable polydimethylsiloxane(PDMS)elastomer based on the Knoevenagel condensation(KC)reaction.This PDMS elastomer was prepared by the KC reaction catalyzed by 4-dimethylaminopyridine(DMAP).The obtained PDMS elastomer exhibited an elongation at break of 266%,a tensile strength of 0.57 MPa,and a good thermal stability(Td=357℃).In addition,because of the presence of dynamic C=C bonds formed by the KC reaction and low glass transition temperature(Tg=-117℃).This PDMS exhibited good self-healing and recycling properties at room temperature and could be reprocessed by hot pressing.In addition,the PDMS elastomer exhibits good application prospects in the fields of adhesives and flexible electronic devices.
基金financially supported by the National Natural Science Foundation of China(Nos.22272118,22172111,and 22309134)the Science and Technology Commission of Shanghai Municipality,China(Nos.22ZR1464100,20ZR1460300,and 19DZ2271500)+2 种基金the China Postdoctoral Science Foundation(2022M712402),the Shanghai Rising-Star Program(23YF1449200)the Zhejiang Provincial Science and Technology Project(2022C01182)the Fundamental Research Funds for the Central Universities(2023-3-YB-07)。
文摘Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.
基金financially supported by the China Postdoctoral Science Foundation(No.2024M751205)。
文摘Flexible phase change materials(PCMs)have become increasingly critical to address the demand for thermal management in electronic technologies and energy conversion.However,their application remains challenging because of their rigidity,liquid leakage,and insufficient thermal conductivity.Herein,flexible glutamic acid@natural rubber/paraffin wax(PW)/carbon nanotubes-graphene nanoplatelets(GNR/PW/CGNP)phase change composites with high thermal conductivity,excellent shape stability,and recyclability were reported.Zn^(2+)-based dynamic crosslinking was constructed through the reaction of zinc acetate and carboxyl groups on glutamic acid@natural rubber(GNR),which was used as a flexible matrix to physically blend with paraffin wax/carbon nanotubes/graphene nanoplatelets(PW/CGNP)to achieve uniform dispersion of PW/CGNP,continuous thermal conductivity networks,and good encapsulation of PW.The GNR/PW/CGNP composites showed excellent mechanical strength,flexibility,and recycling ability,and effective encapsulation prevented the outflow of melted PW during the phase transition.Also,the phase change enthalpy could attain 111.1 J/g with a higher thermal conductivity of 1.055 W/m K,428%higher than that of pure PW owing to the formation of efficient thermal conductive pathways,which exhibited outstanding thermal management performance and superior temperature control behavior in electronic devices.The developed flexible composite PCMs may open new possibilities for next-generation flexible thermal management electronics.
基金financially supported by the National Key R&D Program of China(No.2021YFB3801901)the Institutional Research Fund from Sichuan University(No.2020SCUNL205)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Higher Education Discipline Innovation Project(No.B20001)。
文摘Polymers that exhibit both biodegradability and chemical recyclability offer a promising solution to environmental pollution and resource scarcity. Poly(glycolic acid)(PGA) is a promising chemically recyclable polymer, characterized by its seawater degradability and high mechanical strength. In this study, aliphatic polycarbonates were synthesized through melt polycondensation and subsequently copolymerized with glycolide(GL) to produce chemically recyclable PGA based triblock copolymers with well-defined structures. The properties of these copolymers, including their thermal properties, crystallization behavior, and mechanical performance, can be effectively adjusted by modifying the structure and content of the middle block. Furthermore, an in-depth investigation reveals that the pyrolysis process involves ester exchange, radical, and back-biting reactions. In addition, the high-efficiency "Monomer↔Copolymer" chemical recycling loop has been established, achieving a remarkable yield exceeding 88% along with a purity greater than 99%.
基金supported by the National Key R&D Program of China(No.2023YFA1506804)the National Natural Science Foundation of China(Nos.22471110,22171111,22131007 and 22071093)+1 种基金the Science Foundation of Gansu Province of China(No.22JR5RA406)the Fundamental Research Funds for the Central Universities(No.lzujbky-2023-15)。
文摘Most commercial plastics cannot easily degrade,which raises a number of sustainability issues.To address the current problem of plastic pollution,the research and development of easily degradable and recyclable polymers has become an attractive subject.Herein,a new monomer of thiosalicylic methyl glycolide(TSMG)was synthesized using one-pot method and high molecular weight poly(thiosalicylic methyl glycolide)(PTSMG,M_(n) up to 300 kDa)can be obtained via the ring-opening polymerization(ROP)of TSMG.PTSMG exhibits good closed-loop recyclability and hydrolytic degradability,where PTSMG can generate pristine monomers through sublimation thermal depolymerization conditions due to the presence of thiophenol ester bond in the polymer chains,and can be degraded rapidly in aqueous solution,which provides a potential solution to the current plastic pollution problem.
基金financially supported by the Research Startup Project for High-Level Talent Attraction in Inner Mongolia Agricultural University(No.NDYB2023-40)the Natural Science Research Fund for Colleges and Universities in Anhui Province(No.2022AH050309)+3 种基金The Scientific Research Foundation of Education Department of Anhui Province of China(No.KJ2021ZD0043)the University Synergy Innovation Program of Anhui Province of China(No.GXXT-2022-010)the High-Level Talent Project of Talent Development Fund of Inner Mongoliathe Start-Up Funding from Inner Mongolia University of Technology(No.YLXKZX-NGD-039)
文摘Despite their high-energy conversion efficiency that has earned them the label of next-generation energy utilization devices,protonic ceramic fuel cells(PCFCs)have not yet fully fulfilled their potential in terms of low-cost integration and environmentally friendly application,which remain significant concerns that heavily influence their progress towards commercial viability.A pragmatic way of cell recycling is extremely helpful for addressing these concerns.Herein,we unveil a novel concept of reusable PCFCs,and propose a comprehensive recycling scheme for discarded PCFCs.In this research,a recycled cell with a recycled single perovskite cathode exhibited a peak power density(PPD)of 1.10 W cm^(-2)at 700℃,comparable to a pristine cell of 1.05 W cm^(-2).Metal ion rearrangement and phase evolution during the recycling processes were investigated,which were demonstrated to be in high relevance to the performance of recycled cells.This research constitutes a pioneering exploration of the mechanisms underlying recycling efforts and offers valuable insights into the material recycling of solid-state functional devices used for energy conversion and storage.
文摘The“2025 China New-Formulation Detergent Products Development Conference & 2025 China Daily Chemicals Biodegradable,Recyclable,Renewable Technology Innovation Summit”,cohosted by the China Research Institute of Daily Chemical(RIDCI),was held in Yangzhou,Jiangsu Province.The event brought together over 230 representatives from government agencies,industry associations,and leading enterprises to contribute insights for the high-quality development of China's daily chemical industry.
文摘Nickel-catalyzed borylation of aryl nonaflates with B2pin2 could be realized,which proceeded effectively by means of C—O bond functionalization to afford a wide variety of valuable arylboronates in moderate to excellent yields with good functionality compatibility.In addition,the gram-scale synthesis and the application of the approach in the late-stage elaboration of aryl nonaflate derived from pterostilbene could also be achieved.
文摘To address the longstanding challenge in traditional carborane methodology of rapidly and efficiently constructing carboranyl-based polycyclic frameworks,Pd-catalyzed one-pot reactions between pyridyl-substituted nidocarboranes and alkynes directly afford two distinct types of 2D-3D fused carboranyl polycyclic compounds:3a-3f,4a-4d.The structures of this series of compounds were characterized by nuclear magnetic resonance spectroscopy,single-crystal X-ray diffraction,and high-resolution mass spectrometry,and a plausible reaction mechanism was proposed.Crystal structures reveal that the multiple rings in such 2D-3D fused carboranyl polycyclic compounds exhibit a certain degree of coplanarity.Furthermore,these compounds exhibited properties distinct from those of conventional 2D polycyclic systems.CCDC:2481988,3c,2481990,3f,2481986,4d.
文摘A multi-stimuli-responsive hydrogel,P(VI-co-MAAC-NE),was successfully constructed by covalently integrating the aggregation-induced emission(AIE)moiety(Z)-N-(4-(1-cyano-2-(4-(diethylamino)phenyl)vinyl)-phenyl)methacrylamide(NE)into a dynamic hydrogen-bonding network composed of 1-vinylimidazole(VI)and methacrylic acid(MAAC)groups.The dense hydrogen-bonding network not only provides enhanced mechanical robustness,but also significantly enhances the AIE effect of NE by restricting its molecular motion.Under various external stimuli,the hydrogen bonds within the hydrogel network undergo reversible dissociation and reformation,thus enabling synergistic modulation of the hydrogel’s mechanical properties and luminescence behavior.Specifically,organic solvents disrupt the hydrogen-bonding network and the aggregation of the AIE moiety NE,resulting in macroscopic swelling and fluorescence quenching of the hydrogel.In strongly acidic conditions,protonation of NE molecules suppresses the intramolecular charge transfer(ICT)process,yielding a blue-shifted emission band accompanied by intense blue fluorescence;in highly alkaline environments,deprotonation of carboxyl groups induces hydrogel swelling and disperses NE aggregates,leading to pronounced fluorescence quenching.Moreover,the system exhibits thermally activated shape-memory behavior:heating above the glass transition temperature(T_(g):ca.62℃)softens the hydrogel to allow programmable reshaping,and subsequent hydrogen bond reformation at ambient conditions locks in the resultant geometries without sacrificing the hydrogel’s fluorescence performance.By capitalizing on these multi-stimuli-responsive characteristics and shape-memory behavior,the potential of hydrogel P(VI-co-MAAC-NE)for advanced information encryption and anti-counterfeiting applications is demonstrated.This work not only provides a versatile material platform for sensing and information storage,but also offers new insights into the design of intelligent soft materials integrating AIE features with dynamically regulated supramolecular network structures.
基金Supported by the National Natural Science Foundation of China(22468035,22468036,22368038,22308048)the Natural Science Foundation of Inner Mongolia(2024QN02018,2025MS02030)+2 种基金First-class Discipline Research Special Project of Inner Mongolia(YLXKZX-NGD-045)Inner Mongolia Autonomous Region Postgraduate Research Innovation Project(KC2024047B)Research Foundation for Introducing High-level Talents in Inner Mongolia Autonomous Region。
文摘The global energy landscape is undergoing a profound transformation,with wind energy,especially wind power,gaining increasing prominence due to its clean,renewable nature.However,as the installed capacity of wind power continues to expand,the disposal of waste wind turbine blades(WWTB)has emerged as a significant challenge.These blades are predominantly composed of epoxy resin(EP)polymers,carbon fibers(CFs),and glass fibers(GFs).Improper disposal not only exacerbates environmental concerns but also leads to the loss of valuable resources,particularly carbon-based materials.Pyrolysis technology,a versatile and environmentally sustainable method for resource recovery,has garnered considerable attention in the context of WWTB disposal.This work presents a comprehensive review of the pyrolytic recycling of WWTB,focusing on the principles and classifications of pyrolysis technology,key factors influencing the pyrolysis process,as well as the pyrolysis methods,equipment,products,and their applications.Through an in-depth analysis of the current research on the pyrolytic recycling of WWTB,this review identifies critical unresolved issues in the field and provides a forward-looking perspective on emerging research trends.