Three-dimensional Cross-linked Network Research Articles

Three-dimensional cross-linked network deep eutectic gel polymer electrolyte with the self-healing ability enable by hydrogen bonds and dynamic disulfide bonds

Solid polymer electrolytes (SPEs) are effective solutions for the development of high-performance and flexible lithium metal batteries (LMBs). However, the key problems of SPEs including low ionic conductivity and inability to repair damage have hindered their industrialization process. In this work, a three-dimensional (3D) cross-linked network gel polymer electrolyte (CNGPE) is designed. The addition of deep eutectic solvent (DES) improves the ionic conductivity of CNGPE. The hydrogen bonds and dynamic disulfide bonds in the 3D cross-linked network endow CNGPE rapid self-healing ability at ambient temperature. In addition, the addition of lithium difluoro(oxalato)borate (LiDFOB) and lithium nitrate (LiNO3) helps to form a stable solid electrolyte interface (SEI). Due to the ingenious design, the Li/CNGPE/Li symmetrical cell exhibits excellent interface stability and no short circuit occurs for more than 800 h. The assembled LiFePO4/CNGPE/Li cell exhibits a discharge specific capacity of 126 mAh g−1 after 960 cycles at 0.5C. This work has shown that the self-healing gel polymer electrolyte containing DES provides an effective and feasible method for the development of high-performance LMBs.

Three-Dimensional Cross-Linking Network Coating for the Flame Retardant of Bio-Based Polyamide 56 Fabric by Weak Bonds.

Weak bonds usually make macromolecules stronger; therefore, they are often used to enhance the mechanical strength of polymers. Not enough studies have been reported on the use of weak bonds in flame retardants. A water-soluble polyelectrolyte complex composed of polyethyleneimine (PEI), sodium tripolyphosphate (STPP) and melamine (MEL) was designed and utilized to treat bio-based polyamide 56 (PA56) by a simple three-step process. It was found that weak bonds cross-linked the three compounds to a 3D network structure with MEL on the surface of the coating under mild conditions. The thermal stability and flame retardancy of PA56 fabrics were improved by the controlled coating without losing their mechanical properties. After washing 50 times, PA56 still kept good flame retardancy. The cross-linking network structure of the flame retardant enhanced both the thermal stability and durability of the fabric. STPP acted as a catalyst for the breakage of the PA56 molecular chain, PEI facilitated the char formation and MEL released non-combustible gases. The synergistic effect of all compounds was exploited by using weak bonds. This simple method of developing structures with 3D cross-linking using weak bonds provides a new strategy for the preparation of low-cost and environmentally friendly flame retardants.

Advancements in Noble Metal-Decorated Porous Carbon Nanoarchitectures: Key Catalysts for Direct Liquid Fuel Cells.

Noble-metal nanocrystals have emerged as essential electrode materials for catalytic oxidation of organic small molecule fuels in direct liquid fuel cells (DLFCs). However, for large-scale commercialization of DLFCs, adopting cost-effective techniques and optimizing their structures using advanced matrices are crucial. Notably, noble metal-decorated porous carbon nanoarchitectures exhibit exceptional electrocatalytic performances owing to their three-dimensional cross-linked porous networks, large accessible surface areas, homogeneous dispersion (of noble metals), reliable structural stability, and outstanding electrical conductivity. Consequently, they can be utilized to develop next-generation anode catalysts for DLFCs. Considering the recent expeditious advancements in this field, this comprehensive review provides an overview of the current progress in noble metal-decorated porous carbon nanoarchitectures. This paper meticulously outlines the associated synthetic strategies, precise microstructure regulation techniques, and their application in electrooxidation of small organic molecules. Furthermore, the review highlights the research challenges and future opportunities in this prospective research field, offering valuable insights for both researchers and industry experts.

Geometry-based cross-linking algorithm for modeling resorcinol resins through united-atom molecular dynamics simulations

The addition-condensation polymerization (ACP) of resorcinol with formaldehyde and the electrochemical polymerization (ECP) of resorcinol were desirable to improve the performances of resins. To achieve computational design, a new geometry-based cross-linking modeling algorithm for three-dimensional (3D) cross-linked network structures of resorcinol resins was developed for molecular dynamics (MD) simulations using a united-atom model. The ACP and ECP of resorcinol were successfully modeled using one algorithm by changing the parameters of the reaction rate constants of methylene, ether, and biphenyl bond formations. Furthermore, reaction judgment was performed under a reaction probability function comprising the Gaussian functions based on the interatomic distance of the reaction candidate atom pairs and interior angles regarding the spatial arrangement of two resorcinol rings. This geometry-based cross-linking algorithm successfully generated strainless 3D cross-linked network structures of the ACP and ECP resorcinol resins without the formation of highly bent unstable structures, such as U-shaped biphenyls. The MD simulation results indicated that the cross-linking of the ACP resin comprising methylene linkages proceeded with a network structure formation mechanism similar to that of phenolic resins, where the cross-linked network structure was determined at the gel point and the reactions after the gel point were to fix and freeze the network structure. For the ECP resins comprising ether and biphenyl linkages, the molar ratio of ether to biphenyl bonds affected the elastic property of the resins, and the incorporation of rigid biphenyl structures into ether-linkage networks increased the elastic modulus. Moreover, an increase in rigidity was observed as a decrease in the Poisson's ratio.

Integrating with a tough framework and efficient self-healing behavior based on a flexible polymer skeleton for Si anode binders in lithium-ion cells

As a prospective and efficient strategy to address the volume expansion of the Si nanoparticles, the binder plays an increasingly significant role in the Si anode of lithium-ion batteries. Based on the inspiration of natural physics and cross-linked networks, a functional (named polyacrylic acid-citric acid-polyethyleneimine) binder that is similar to a flexible polymer skeleton integrated with a tough framework and efficient self-healing behavior is designed to achieve long cycling stability for Si anodes. The cross-linked network can be stabilized by the amide bonds, formed by polyethyleneimine (PEI) and polyacrylic acid (PAA). Based on this, citric acid (CA) can be added to form multiple hydrogen bonds, whose carboxyl groups can also establish a more reversible cross-linked network with Si particles. Then, PEI and CA molecules can connect with PAA to form a “rigid and flexible” structure. The expansion stress of Si nanoparticles is relieved by the protective buffer layer built by the addition of PEI and CA molecules. In addition, PAA, PEI, and CA work together to solve the problem that the action of CA and PAA alone cannot perform well under large currents. Hence, this water-based binder with a three-dimensional cross-linked network structure with self-healing ability has better performance during cycling: at a current density of 0.2C, it still has a capacity of 2017.4 mAh·g−1 after 200 cycles, with a capacity retention rate of 80.7 % (1745.3 mAh·g−1, 300 cycles, a capacity retention of 74.9 %).

Developments in Emerging Topical Drug Delivery Systems for Ocular Disorders.

According to the current information, using nano gels in the eye has therapeutic benefits. Industry growth in the pharmaceutical and healthcare sectors has been fueled by nanotechnology. Traditional ocular preparations have a short retention duration and restricted drug bioavailability because of the eye's architectural and physiological barriers, a big issue for physicians, patients, and chemists. In contrast, nano gels can encapsulate drugs within threedimensional cross-linked polymeric networks. Because of their distinctive structural designs and preparation methods, they can deliver loaded medications in a controlled and sustained manner, enhancing patient compliance and therapeutic efficacy. Due to their excellent drugloading capacity and biocompatibility, nano-gels outperform other nano-carriers. This study focuses on using nano gels to treat eye diseases and provides a brief overview of their creation and response to stimuli. Our understanding of topical drug administration will be advanced using nano gel developments to treat common ocular diseases such as glaucoma, cataracts, dry eye syndrome, bacterial keratitis, and linked medication-loaded contact lenses and natural active ingredients.

Properties of wheat gluten based wood adhesives enhanced by transglutaminase and epichlorohydrin

Bio-based eco-friendly products are well-received globally due to increasingly scarce petroleum resources and growing public concern about human health risks and environmental concerns. In this study, wheat gluten (WG) as the raw material modified with transglutaminase (TGase) and epichlorohydrin (ECH) was used to develop an eco-friendly bio-based adhesive. Effects of TGase and ECH on the properties of the adhesive were emphatically discussed. The dry and wet shear strengths of the combined modified adhesive achieved at 3.21 MPa and 0.81 MPa, which was higher than the Chinese National Standard Ⅱ plywood requirements (0.7 MPa). Meanwhile, the solid content and the protein surface hydrophobicity H0 were increased to 28.27 % and 636.54, respectively. These improvements were mainly because, during the modification, the structure of WG became more stretched after ethanol treatment. Then the TGase promoted the cross-linking of the protein molecules and enhanced the cohesion strength of the adhesive system. Finally the ECH further cross-linked and aggregated with exposed active groups to varying degrees, and formed a compact three-dimensional cross-linked network structure, which allowed the WG-based adhesive to form a smoother and more uniform microscopic surface and better water resistance. The obtained adhesives might be utilized to substitute petroleum-derived adhesives in the plywood sector, providing ideas and references for future eco-friendly adhesive research and increasing the high value usage of wheat starch processing by-products.

Tailoring Three-Dimensional Cross-Linked Networks Based on Water-Soluble Polymeric Materials for Stable Silicon Anode.

For stable battery operation of silicon (Si)-based anodes, utilizing cross-linked three-dimensional (3D) network binders has emerged as an effective strategy to mitigate significant volume fluctuations of Si particles. In the design of cross-linked network binders, careful selection of appropriate cross-linking agents is crucial to maintaining a balance between the robustness and functionality of the network. Herein, we strategically design and optimize a 3D cross-linked network binder through a comprehensive analysis of cross-linking agents. The proposed network is composed of poly(vinyl alcohol) grafted poly(acrylic acid) (PVA-g-PAA, PVgA) and aromatic diamines. PVgA is chosen as the polymer backbone owing to its high flexibility and facile synthesis using an ecofriendly water solvent. Subsequently, an aromatic diamine is employed as a cross-linker to construct a robust amide network that features a resonance-stabilized high modulus and enhanced adhesion. Comparative investigations of three cross-linkers, 2,2'-bis(trifluoromethyl)benzidine, 3,3'-oxidianiline, and 4,4'-oxybis[3-(trifluoromethyl)aniline] (TFODA), highlight the roles of the trifluoromethyl group (-CF3) and the ether linkage. Consequently, PVgA cross-linked with TFODA (PVgA-TFODA), featuring both -CF3 and -O-, establishes a well-balanced 3D network characterized by heightened elasticity and improved binding forces. The optimized Si and SiOx/graphite composite electrodes with the PVgA-TFODA binder demonstrate impressive structural stability and stable cycling. This study offers a novel perspective on designing cross-linked network binders, showcasing the benefits of a multidimensional approach considering chemical and physical interactions.

PH dependent biocompatible room temperature covalent organic polymers for selective chemotherapeutic drug delivery

Covalent organic polymers (COP) are a special class of two-dimensional and three-dimensional cross-linked polymeric networks with repeating organic units. They are ideally suited for drug delivery applications because of their large surface area, porous nature, and tunable properties. Furan-2,5-dicarbohydrazide and 1,3,5-triformylbenzene were used to synthesize pH-responsive hydrazone-linked furan-based spherical COP(FRT-COP) at room temperature. The formulated FRT-COP were later stabilized using hyaluronic acid (HA) and then encapsulated anticancer drug doxorubicin (DOX), utilizing the porous structure of the synthesized COP. The newly developed FRT-COP have a pore size of 10 nm, and FRT-COP-DOX-HA exhibit drug loading capacity of 34.4 % and an encapsulation efficiency of 52.32 %. The 80 % viability of NIH 3T3 cells and 82.1 % viability of the CT2A cells, even at a higher concentration of 100 μg/mL of the carrier system, proves the outstanding biocompatibility of the carrier system for chemotherapeutic drug delivery administration. The FRT-COP-DOX-HA-treated NIH-3T3 normal cell line exhibits a viability of 80.59 % at a material concentration of 25 μg/mL. Furthermore, CT2A cancer cell lines show a viability of 33.1 % at a material concentration of 25 μg/mL. The in vivo results obtained from the experiments performed on male BALB/c nude mice also unequivocally demonstrated the exceptional suitability of the proposed drug delivery carrier system for antitumor chemotherapeutic drug administration.

Electronically modified hierarchical porous carbon by N, P heteroatoms for zinc ion hybrid capacitor

Due to the low cost and steady physicochemical properties of carbon materials, zinc-ion hybrid capacitors (ZICs) composed of carbon cathode and Zn anode have aroused considerable attracts in recent years. However, the unsatisfactory capacity and electrochemical kinetics of carbonaceous cathode hinder its application in ZICs. Herein, a facile self-template thermal treatment method was proposed to prepare N, P co-doped hierarchical porous carbons (NP-HPCs). The electronically modified NP-HPC3 has an ultrahigh ratio of active N species and abundant micropores, which is favorable for zinc ions adsorption. In addition, the three-dimensional cross-linked network with abundant mesoporous cavities synchronously boosts electrons/ions transfer kinetics. Ex-situ characterization shows that the introduction of N, P heteroatoms is helpful to improve the adsorption of zinc ions. Thanks to these favorable structural characteristics, the NP-HPC3 displays an exceptional specific capacitance (275.0 F g−1 at 0.1 A g−1) and rate capability (182.0 F g−1 at 20 A g−1). More significantly, the NP-HPC3-based ZIC delivers a prominent energy density of 107.8 Wh kg−1 at a power density of 90.7 W kg−1, a long cycle life (96.9 % capacitance retention after 10,000 cycles) together with an outstanding anti-self-discharge performance (0.001145 V h−1@200 h). This study not only affords a feasible and environmental route to construct advanced heteroatom doped carbonaceous materials, but also explores the interrelation between zinc ions storage behavior and structural characteristics of carbon materials.

Synthesis of a new three-dimensional cross-linked network dust suppressant and its mechanism of coal-dust inhibition

A new dust suppressant was proposed and studied by numerical calculations and experiments to control dust. The synthesis of suppressant required three steps. First, Polyvinyl alcohol starch was synthesized by the dehydration condensation of carboxymethyl starch and polyvinyl alcohol under the initiation of ammonium persulfate, requiring 288.8 kJ/mol energy. Second, polyvinyl alcohol caprolactam starch was synthesized by the dehydration condensation of caprolactam and polyvinyl alcohol starch under the initiation of ammonium persulfate, requiring 172.8 kJ/mol of energy. Third, the suppressant had the optimum wetting and bonding effects by 30 g/L polyvinyl alcohol caprolactam starch and 20 g/L sodium dodecylbenzene sulfonate. The suppressant–lignite system exhibited increased hydrogen bonds which were formed between the –OH and –COOH groups of the suppressant and the –OH, –COOH, and –NH2 groups on the coal surface. The solidified layer formed on the coal dust surface did not raise dust at wind speed of 10 m/s.

Furan-derived Schiff base covalent adaptable thermosets with recyclability and anti-flammability

Conventional thermosetting polymers, mostly derived from nonrenewable petroleum resources, are not reprocessable and recyclable due to their highly cross-linked three-dimensional networks and face the disadvantage of high flammability. To solve these issues, in this study, we synthesized a novel Schiff base covalent adaptable thermoset from a furan-derived tri-aldehyde monomer (TMFP) and a furan-derived di-amine monomer (DFDA). The as-prepared TMFP-DFDA-Vitrimer exhibited superior anti-flammability with a high limiting oxygen index (LOI) of 35.0% and a UL-94 V-0 rating, which was attributed to the excellent charring ability. Additionally, TMFP-DFDA-Vitrimer could also be conveniently recycled by chemical decomposition under a mixed hydrochloric acid/tetrahydrofuran (HCl/THF) solution. After recycling for 5 times, the thermal, mechanical, and flame retardant properties of the recycled TMFP-DFDA-Vitrimer retained almost unchanged compared to the original one. This work provides a prime instance to develop advanced thermosetting polymers from abundant furan-based compounds.

A metal-organic framework-based electrocatalytic membrane boosts redox kinetics of lithium‑sulfur batteries

The shuttle behavior and sluggish conversion kinetics of polysulfides significantly impede the commercialization of lithium‑sulfur (LiS) batteries. Herein, we report a membrane-based electrocatalytic interlayer that consists of metal-organic framework (MOF) Co-ZIF-9 sheets and carbon nanotubes (CNT) for these issues, which is facilely weaved by vacuum filtration. The fully exposed active sites of ZIF-9 sheets endow this interlayer an efficient anchoring ability towards polysulfides, therefore efficaciously suppressing the polysulfides shuttle, and, more importantly, a strong electrocatalytic effect to accelerate the redox kinetics. Meanwhile, the three-dimensional cross-linked network structured by the conductive CNT and MOF material favours a rapid ion and electron transport, and the full utilization of adsorption and catalytic sites. As a consequence, this interlayer exhibits an excellent rate performance (a capacity up to 817 mAh g−1 under 5 C), an exceptional cyclic stability (a tiny decay of 0.019% for 1000 cycles at 1 C) and a distinctive high‑sulfur loading performance (7.2 mg cm−2) under a reduced electrolyte content. This study provides inspirations for the rational design of MOF-based nanostructures that can validly anchor polysulfides and catalyze their conversion for high-powered LiS batteries.

PH Sensitive Hydrogel: A Review

Hydrogels are three-dimensional cross-linked networks of polymer chains that can absorb and hold lots of water in the interstitial spaces between chains. Improving the safety efficacy ratio of existing drugs is a current challenge to be addressed rather than the development of novel drugs which involves much expense and time. The efficacy of drugs is affected by several factors such as their low aqueous solubility, unequal absorption along the gastrointestinal (GI) tract, risk of degradation in the acidic milieu of the stomach, low permeation of the drugs in the upper GI tract, systematic side effects, etc. This review aims to enlighten readers on the role of pH-sensitive hydrogels in drug delivery, their mechanism of action, swelling, and drug release as a function of pH change along the GI tract. The basis for the selection of materials, their structural features, physical and chemical properties, the presence of ionic pendant groups, and the influence of their pKavalues on the ionization, consequent swelling, and targeted drug release are also highlighted.

Unraveling the New Perspectives on Antimicrobial Hydrogels: State-of-the-Art and Translational Applications.

The growing impact of infections and the rapid emergence of antibiotic resistance represent a public health concern worldwide. The exponential development in the field of biomaterials and its multiple applications can offer a solution to the problems that derive from these situations. In this sense, antimicrobial hydrogels represent a promising opportunity with multiple translational expectations in the medical management of infectious diseases due to their unique physicochemical and biological properties as well as for drug delivery in specific areas. Hydrogels are three-dimensional cross-linked networks of hydrophilic polymers that can absorb and retain large amounts of water or biological fluids. Moreover, antimicrobial hydrogels (AMH) present good biocompatibility, low toxicity, availability, viscoelasticity, biodegradability, and antimicrobial properties. In the present review, we collect and discuss the most promising strategies in the development of AMH, which are divided into hydrogels with inherent antimicrobial activity and antimicrobial agent-loaded hydrogels based on their composition. Then, we present an overview of the main translational applications: wound healing, tissue engineering and regeneration, drug delivery systems, contact lenses, 3D printing, biosensing, and water purification.

Fungal Ligninolytic Enzymes and Their Application in Biomass Lignin Pretreatment.

Lignocellulosic biomass is a significant source of sustainable fuel and high-value chemical production. However, due to the complex cross-linked three-dimensional network structure, lignin is highly rigid to degradation. In natural environments, the degradation is performed by wood-rotting fungi. The process is slow, and thus, the use of lignin degradation by fungi has not been regarded as a feasible technology in the industrial lignocellulose treatment. Fungi produce a wide variety of ligninolytic enzymes that can be directly introduced in industrial processing of lignocellulose. Within this study, screening of ligninolytic enzyme production using decolorization of ABTS and Azure B dyes was performed for 10 fungal strains with potentially high enzyme production abilities. In addition to standard screening methods, media containing lignin and hay biomass as carbon sources were used to determine the change in enzyme production depending on the substrate. All selected fungi demonstrated the ability to adapt to a carbon source limitation; however, four strains indicated the ability to secrete ligninolytic enzymes in all experimental conditions-Irpex lacteus, Pleurotus dryinus, Bjerkandera adusta, and Trametes versicolor-respectively displayed a 100%, 82.7%, 82.7%, and 55% oxidation of ABTS on lignin-containing media and 100%, 87.9%, 78%, and 70% oxidation of ABTS on hay-containing media after 168 h of incubation. As a result, the most potent strains of fungi were selected to produce lignocellulose-degrading enzymes and to demonstrate their potential application in biological lignocellulose pretreatment.

Controlled Preparation of Cross-Linked SnO2 Hollow Nanotube Networks for Electrocatalytic CO2 Reduction

The electrochemical system based on water, CO2, and electricity is the key technology to realize the coexistence and combination of renewable energy and fossil energy, which can convert CO2 molecules into high-value-added products under mild and controlled conditions, thus achieving carbon neutrality. Designing efficient electrocatalysts to realize highly active, selective, and stable CO2RR has become one of the vital issues. Particularly, the nanostructure design and interface adjustment of electrocatalysts have been regarded as the key points for improving their catalytic performance. Herein, a tin dioxide hollow nanotube (SnO2 HNT) catalyst with a three-dimensional cross-linked network structure has been fabricated by electrospinning and rapid-heating calcination. The morphology and component structure of SnO2 HNTs were analyzed by a series of characterizations. The performance in electrocatalytic carbon dioxide reduction reaction (eCO2RR) was further tested. Owing to the hollow nanostructure, the catalyst possessed a large specific surface area and abundant active sites, which greatly accelerated mass transport and electron mobility. During eCO2RR, SnO2 HNTs achieved a peak faraday efficiency value of 87.4% for C1 products at −1.1 V vs RHE, which significantly suppressed the occurrence of hydrogen evolution side reactions. In addition, compared with the commercial SnO2 nanoparticles or partially reduced Sn/SnO2, the catalytic activity and selectivity of CO2-to-formate conversion significantly increased under the same potential, indicating that the optimization of electronic/geometric structure for high-yield metal oxides can effectively improve the comprehensive performance of eCO2RR.

In situ crosslink polymerization induced long-lived multicolor supramolecular hydrogel based on modified β-cyclodextrin

The construction of hydrogels with good mechanical properties and phosphorescent properties is full of challenges. Herein, we report a supramolecular phosphorescent hydrogel with long lifetime, high tensile strength and self-healing property, which can be easily constructed through in-situ thermal-initiated polymerization of isocyanatoethyl acrylate-modified β-cyclodextrin (β-CD-DA) and acrylate-modified adamantane (Ad-DA), acrylic acid (AA), followed by the non-covalent association with carbon dots (CNDs). The lifetime of phosphorescent hydrogel can reach 1261 ms at room temperature, and the quantum yield is 11%. Importantly, through the efficient triplet to singlet Förster resonance energy transfer (TS-FRET), the phosphorescent hydrogel shows the good phosphorescence energy transfer property for organic dyes Rhodamine B and Eosin Y with the delayed fluorescence lifetime up to 730 ms and 585 ms as well as the energy transfer efficiency (ΦET) up to 99.9% and 99.3%, respectively. Moreover, owing to the host-guest interactions between β-CD-DA and Ad-DA, the three-dimensional cross-linked network phosphorescent hydrogel can be easily stretched to 18 times of its original length, and can achieve self-healing of the cut surfaces within 30 min. These results will expand the scope of phosphorescent materials and provide new ideas and opportunities for materials science.

Core-shell FeCo@carbon nanocages encapsulated in biomass-derived carbon aerogel: Architecture design and interface engineering of lightweight, anti-corrosion and superior microwave absorption

The development of multifunctional microwave absorbing materials for practical applications in complex environments is a challenging research hotspot. Herein, the core–shell structure FeCo@C nanocages were successfully anchored on the surface of biomass-derived carbon (BDC) from pleurotus eryngii (PE) via freeze-drying and electrostatic self-assembly process, achieving lightweight, anti-corrosive, and excellent absorption properties. The superior versatility benefits from the large specific surface area, high conductivity, three-dimensional cross-linked networks, and appropriate impedance matching characteristics. The as-prepared aerogel realizes a minimum reflection loss (RLmin) of −69.5 dB with a corresponding effective absorption bandwidth (EAB) of 8.6 GHz at 2.9 mm. Simultaneously, the computer simulation technique (CST) further proves that the multifunctional material can dissipate microwave energy in actual applications. More importantly, the special heterostructure of aerogel endows excellent resistance to acid, alkali, salt medium, allowing potential applications of the microwave absorbing materials under complex environmental conditions.

Rheological and Aging Properties of Vegetable Oil-Based Polyurethane (V-PU) Modified Asphalt.

To study the rheological and aging properties of vegetable oil-based polyurethane (V-PU) modified asphalt, V-PU terminated with an -NCO group was synthesized from renewable castor oil, and liquefied MDI-100LL and 10-40 wt% V-PU modified asphalts were prepared. Temperature classification, multiple stress creep recovery (MSCR), and linear amplitude scanning (LAS) tests were carried out. The results showed that the modulus, the creep recovery rate (R), and the yield stress and yield strain of the V-PU modified asphalts significantly increased in the order: 0 wt% < 10 wt% < 20 wt% < 40 wt% < 30 wt%, while the phase angle and the unrecoverable creep compliance (Jnr) changed in the opposite order, and the high temperature grade of 30 wt% V-PU modified asphalt was 4 grades higher than that of the base asphalt, which indicated that the addition of V-PU enhanced the fatigue, permanent deformation, and recovery deformation resistance. The 30 wt% sample exhibited phase inversion had the best performance. Comprehensive FTIR, GPC, and fluorescence microscopy analyses showed that the molecular weight significantly increased and the V-PU molecules agglomerated after aging. The excess -NCO groups of V-PU prepolymer react with water in the air and the active hydrogen in the asphalt system and finally form a cross-linked three-dimensional network structure with the asphalt to improve performance. The mechanism of intramolecular cementation reaction and the aging process of V-PU modified asphalt was creatively derived.