Dynamic Crosslinking Research Articles

Internal catalysis significantly promotes the bond exchange of covalent adaptable polyurethane networks

Self-healing covalent adaptable networks (CANs) are not only of fundamental interest but also of practical importance for achieving carbon neutrality and sustainable development. However, there is a trade-off between the mobility and cross-linking structure of CANs, making it challenging to develop CANs with excellent mechanical properties and high self-healing efficiency. Here, we report the utilization of a highly dynamic four-arm cross-linking unit with an internally catalyzed oxime-urethane group to obtain CAN-based ionogel with both high self-healing efficiency (>92.1%) at room temperature and superior mechanical properties (tensile strength 4.55 MPa and toughness 13.49 MJ m-3). This work demonstrates the significant potential of utilizing the synergistic electronic, spatial, and topological effects as a design strategy for developing high-performance materials.

Fabrication of dual dynamic crosslinking polyurethane networks towards self-healing, resist fatigue, and highly stretchable ionic skins

The limited anti-fatigue performance of self-healing polyurethane elastomers under high-strain conditions restricts their application in high-performance ionic skins. Herein, a polyurethane network (PU-DDN) synergistically reversibly crosslinked by dynamic thiourethane bonds and hydrogen bonds was synthesized successfully. This dual reversibly crosslinking strategy not only endowed the polyurethane network with an excellent fatigue resistance (showing a residual strain of only 63 % after 10 uninterrupted cyclic tensile tests at 400 % strains), but also imparted it with a high strength (6.12 MPa) and stretchability (611.42 %). Owing to the thermo-reversibility of dual dynamic networks, the damaged PU-DDN heated at 100 °C for 3h could fully restore its initial mechanical properties. Subsequently, transparent stretchable ionic skins were fabricated by mixing the PU-DDN with ionic liquids. A resulting highly-sensitive ionic skin (GF1 = 1.25, GF2 = 2.01) named PU-DDN/IL20 demonstrated exceptional durability, which could produce repeatable electrical signals even after 2000 cycles of stretching to an extensive deformation of 400 %. Meanwhile, it can also monitor human motions, showcasing its promising potential in the realm of intelligent wearable applications.

Supramolecular oligo-thymine/melamine nanobridge-driven macroscopic engineering: reprogrammable hydrogels for multi-stimuli responsive architectures

The arbitrary, modular, and reprogrammable engineering of macroscopic objects by DNA interactions remains a challenge, despite the well-established use of DNA to drive constructs at nano/micro-scale. Moreover, achieving adaptive responsiveness in assembled architectures under dynamic environmental triggers has yet to be realized. In this study, we introduce the association of oligo-thymine strands (polyT) and melamine (MA), as a low-molecular-weight cofactor, into a supramolecular DNA duplex, termed polyT-MA nanobridge. This unique nanostructure exhibits responsiveness to five external stimuli, including temperature, DNA strand, small molecule, acidic pH, and alkaline pH. The polyT-MA nanobridge is developed as the dynamic crosslinking elements for constructing multi-stimuli responsive DNA hydrogels, which exhibit physiochemical properties changes (e.g., rigidity, thermal stability) and hydrogel-to-liquid phase transitions in response to the five external triggers. Notably, the assembly of macroscopic hydrogel blocks at millimeter scale (cubes in 5 × 5 × 5 mm dimensions) into diverse architectures, e.g., linear type, cross, P-shape, T-shape, or heteromorphy, is achieved by using the non-canonical supramolecular polyT-MA nanobridges. Sequential, dynamic, and selective disassembly of polyT-MA bridged hydrogel constructs is triggered by multiple external stimuli and the rearrangement of these separated individual cubes into other architectures in LEGO styles is presented. This study provides insights into the development of advanced materials and devices with reconfigurable architectures and functionalities for intelligent nanoengineering applications.

Facile supramolecular processing of recyclable adaptive polymer composites for highly reproducible sensory materials

Dynamic polymer networks (DPNs), when cross-linked, can display chemical and physical adaptiveness due to their dynamic connections and associated phase transitions. However, the reliable preparation of these conductive composites and achieving consistent performance through recycling remain challenging, primarily due to a lack of systematic approaches. Herein, we describe synergistic association of supramolecular gel and high density dynamic crosslinking using vinylogous urethane (VU) bond that enable highly reliable sensitivity and reproducibility after recycling to high performance adaptive dynamic polymer networks containing conductive fillers. We introduce a straightforward method to create DPNs-single-walled carbon nanotube (SWCNT) composites. This involves facile grinding a random copolymer in a supramolecular eutectic liquid, resulting in a supramolecular gel. Subsequently, dynamic cross-linking is applied. The resulting dynamic polymer-SWCNT (DPC) composites, incorporating a supramolecular gel, demonstrate adjustable electrical conductivity and high sensitivities to various mechanical motions and irradiations, including specific light and heat. Significantly, the DPC exhibits excellent recyclability, along with enhanced reproducibility and sensitivity as a strain sensor compared to other recyclable sensors. Furthermore, we establish a strong correlation between the sensitivity and stiffness of the DPC composite with dynamic cross-linking density. These findings highlight the promising potential of adaptive gel-based processing of DPNs for highly sensitive, recyclable sensory materials with excellent reproducibility.

Accelerated, injectable, self-healing, scarless wound dressings using rGO reinforced dextran/chitosan hydrogels incorporated with PDA-loaded asiaticoside

The process of wound healing is intricate and complex, necessitating the intricate coordination of various cell types and bioactive molecules. Despite significant advances, challenges persist in achieving accelerated healing and minimizing scar formation. Herein, a multifunctional hydrogel engineered via dynamic Schiff base crosslinking between oxidized dextran and quaternized chitosan, reinforced with reduced graphene oxide (rGO) is reported. The resulting OQG hydrogels demonstrated injectability to aid in conforming to irregular wound geometries, rapid self-healing to maintain structural integrity and adhesion for intimate integration with wound beds. Moreover, the developed hydrogels possessed antioxidant and antibacterial activities, mitigating inflammation and preventing infection. The incorporation of conductive rGO further facilitated the transmission of endogenous electrical signals, stimulating cell migration and tissue regeneration. In addition, the polydopamine-encapsulated asiaticoside (AC@PDA) nanoparticles were encapsulated in OQG hydrogels to reduce scar formation during in vivo evaluations. In vitro results confirmed the histocompatibility of the hydrogels to promote cell migration. The recovery of the full-thickness rat wounds revealed that these designed OQG hydrogels with the incorporation of AC@PDA nanoparticles could accelerate wound healing, reduce inflammation, facilitate angiogenesis, and minimize scarring when implemented. This multifunctional hydrogel system offers a promising strategy for enhanced wound management and scarless tissue regeneration, addressing the multifaceted challenges in wound care.

On-demand bactericidal and self-adaptive antifouling hydrogels for self-healing and lubricant coatings of catheters

Catheter-related infections are one of the most common nosocomial infections with increasing morbidity and mortality, and robust antibacterial or antifouling catheter coatings remain great challenges for long-term implantation. Herein, multifunctional hydrogel coatings were developed to provide persistent and self-adaptive antifouling and antibacterial effects with self-healing and lubricant capabilities. Polyvinyl alcohol (PVA) with β-cyclodextrin (β-CD) grafts (PVA-Cd) and 4-arm polyethylene glycol (PEG) with adamantane and quaternary ammonium compound (QAC) terminals (QA-PEG-Ad) were crosslinked through host-guest recognitions between adamantane and β-CD moieties to acquire PVEQ coatings. In response to bacterial infections, QACs exhibit reversible transformation between zwitterions (pH 7.4) and cationic lactones (pH 5.5) to generate on-demand bactericidal effect. Highly hydrophilic PEG/PVA backbones and zwitterionic QACs build a lubricate surface and decrease the friction coefficient 10 times compared with that of bare catheters. The antifouling hydrated layer significantly inhibits blood protein adsorption and platelet activation and reveals negligible hemolysis and cytotoxicity. The dynamic host-guest crosslinking achieves full self-healing of cracks in PVEQ hydrogels, and the mechanical profiles were recovered to over 90 % after rejuvenating the broken hydrogels, exhibiting a long-term stability after mechanical stretching, twisting, knotting and compression. After subcutaneous implantation and local bacterial infection, the retrieved PVEQ-coated catheters display no tissue adhesion and 3 log folds lower bacterial number than that of bare catheters. PVEQ coatings effectively prevent the repeated bacterial infections and there are few inflammatory reactions in the surrounding tissue, while substantial lymphoid infiltration and inflammatory cell aggregation occur in muscle tissues around the bare catheter. Thus, this study demonstrates a catheter coating strategy by on-demand bactericidal, self-adaptive antifouling, self-healing and lubricant hydrogels to address medical devices-related infections. Statement of significanceIt is estimated over two billion peripheral intravenous catheters are annually used in hospitals around the world, and catheter-associated infection has become a great clinical challenge with rapidly rising morbidity and mortality. Surface coating is considered a promising approach, but substantial challenges remain in the development of coatings that simultaneously satisfy both anti-fouling and antibacterial attributes. Even more, few attempts have been made to design mechanically robust coatings and reversible antibacterial or antifouling capabilities, which are critical for long-term medical implants. To address these challenges, we propose a concise strategy to develop hydrogel coatings from commercially available poly(ethylene glycol) and polyvinyl alcohol. In addition to self-healing and lubricant capabilities, the reversible conversion between zwitterionic and cationic lactones of quaternary ammonium compounds enables on-demand bactericidal and self-adaptive antifouling effects.

Water Molecule as a Dynamic Cross-Linker for Creating Multifunctional Poly(ionic liquid) Porous Membranes

Water Molecule as a Dynamic Cross-Linker for Creating Multifunctional Poly(ionic liquid) Porous Membranes

Naturally derived double-network hydrogels with application as flexible adhesive sensors

Hydrogels have been widely used in the biomedical field, including wearable sensors and biological adhesives. However, achieving a balance between various functionalities, such as wet adhesion, stable conductivity, and biocompatibility, in one customized hydrogel has been a challenging issue. In this study, we developed a multifunctional hydrogel comprising recombinant human collagen (RHC) and aldehyde-modified sodium alginate (Ald-alginate), which was primarily crosslinked through a Schiff-base reaction and metal chelation. Due to the combination of a dynamic covalent crosslinking network (imine linkage between RHC and Ald-alginate) and a dynamic ionic crosslinking network (ionic bonding between Ca2+ and Ald-alginate), the hydrogel exhibited excellent self-healing and injectable behaviors. Benefiting from the high Ca2+ content, the hydrogel also attained antifreezing and conductivity properties. In addition to its excellent conductivity and biocompatibility, the hydrogel exhibited strong wet tissue adhesion ability and could adhere rapidly and strongly to the surfaces of various objects or biological tissues, forming a good sealing environment. Moreover, the hydrogel could be directly adhered to a tissue surface as a flexible sensor to accurately detect physiological signals. The versatility of this multifunctional hydrogel will open new avenues for biomedical applications, such as bioadhesives and biosensing.

Dynamic Metal-Coordinated Adhesive and Self-Healable Antifreezing Hydrogels for Strain Sensing, Flexible Supercapacitors, and EMI Shielding Applications.

Dynamic metal-coordinated adhesive and self-healable hydrogel materials have garnered significant attention in recent years due to their potential applications in various fields. These hydrogels can form reversible metal-ligand bonds, resulting in a network structure that can be easily broken and reformed, leading to self-healing capabilities. In addition, these hydrogels possess excellent mechanical strength and flexibility, making them suitable for strain-sensing applications. In this work, we have developed a mechanically robust, highly stretchable, self-healing, and adhesive hydrogel by incorporating Ca2+-dicarboxylate dynamic metal-ligand cross-links in combination with low density chemical cross-links into a poly(acrylamide-co-maleic acid) copolymer structure. Utilizing the reversible nature of the Ca2+-dicarboxylate bond, the hydrogel exhibited a tensile strength of up to ∼250 kPa and was able to stretch to 15-16 times its original length. The hydrogel exhibited a high fracture energy of ∼1500 J m-2, similar to that of cartilage. Furthermore, the hydrogel showed good recovery, fatigue resistance, and fast self-healing properties due to the reversible Ca2+-dicarboxylate cross-links. The presence of Ca2+ resulted in a highly conductive hydrogel, which was utilized to design a flexible resistive strain sensor. This hydrogel can strongly adhere to different substrates, making it advantageous for applications in flexible electronic devices. When adhered to human body parts, the hydrogel can efficiently detect limb movements. The hydrogel also exhibited excellent performance as a solid electrolyte for flexible supercapacitors, with a capacitance of ∼260 F/g at 0.5 A/g current density. Due to its antifreezing and antidehydration properties, this hydrogel retains its flexibility at subzero temperatures for an extended period. Additionally, the porous network and high water content of the hydrogel impart remarkable electromagnetic attenuation properties, with a value of ∼38 dB in the 14.5-20.5 GHz frequency range, which is higher than any other hydrogel without conducting fillers. Overall, the hydrogel reported in this study exhibits diverse applications as a strain sensor, solid electrolyte for flexible supercapacitors, and efficient material for electromagnetic attenuation. Its multifunctional properties make it a promising candidate for use in various fields as a state-of-the-art material.

Dynamic Cross-Linking, Self-Healing, Antibacterial Hydrogel for Regenerating Irregular Cranial Bone Defects.

Given the widespread clinical demand, addressing irregular cranial bone defects poses a significant challenge following surgical procedures and traumatic events. In situ-formed injectable hydrogels are attractive for irregular bone defects due to their ease of administration and the ability to incorporate ceramics, ions, and proteins into the hydrogel. In this study, a multifunctional hydrogel composed of oxidized sodium alginate (OSA)-grafted dopamine (DO), carboxymethyl chitosan (CMCS), calcium ions (Ca2+), nanohydroxyapatite (nHA), and magnesium oxide (MgO) (DOCMCHM) was prepared to address irregular cranial bone defects via dynamic Schiff base and chelation reactions. DOCMCHM hydrogel exhibits strong adhesion to wet tissues, self-healing properties, and antibacterial characteristics. Biological evaluations indicate that DOCMCHM hydrogel has good biocompatibility, in vivo degradability, and the ability to promote cell proliferation. Importantly, DOCMCHM hydrogel, containing MgO, promotes the expression of osteogenic protein markers COL-1, OCN, and RUNX2, and stimulates the formation of new blood vessels by upregulating CD31. This study could provide meaningful insights into ion therapy for the repair of cranial bone defects.

Glucose-responsive, self-healing, wet adhesive and multi-biofunctional hydrogels for diabetic wound healing

Diabetic wounds are serious clinical complications which manifest wet condition due to the mass exudate, along with disturbed regulation of inflammation, severe oxidative stress and repetitive bacterial infection. Existing treatments for diabetic wounds remain unsatisfactory due to the lack of ideal dressings that encompass mechanical performance, adherence to moist tissue surfaces, quick repair, and diverse therapeutic benefits. Herein, we fabricated a wet adhesive, self-healing, glucose-responsive drug releasing hydrogel with efficient antimicrobial and pro-healing properties for diabetic wound treatment. PAE hydrogel was constructed with poly(acrylic acid-co-acrylamide) (AA-Am) integrated with a dynamic E-F crosslinker, which consisted of epigallocatechin gallate (EGCG) and 4-(2-acrylamidoethylcarbamoyl)-3-fluorophenylboronic acid (AFPBA). Due to the dynamic crosslinking nature of boronate esters, abundant catechol groups and hydrogen bonding, PAE hydrogel demonstrated excellent mechanical properties with about 1000 % elongation, robust adhesion to moist tissues, fast self-healing, and absorption of biofluids of 10 times of its own weight. Importantly, PAE hydrogel exhibited sustained and glucose-responsive release of EGCG. Together, the bioactive PAE hydrogel had effective antibacterial, antioxidative, and anti-inflammatory properties in vitro, and accelerated diabetic wound healing in rats via reducing tissue-inflammatory response, enhancing angiogenesis, and reprogramming of macrophages. Overall, this versatile hydrogel provides a straightforward solution for the treatment of diabetic wound, and shows potential for other wound-related application scenarios.

NH2-MXene/OXG nanocomposite hydrogel with efficient photothermal antibacterial activity for potentially removing biofilms

The adhesion of bacteria to the surface leads to formation of biofilms causing numerous infection problems in implanting medical devices or interventional therapy. Traditional treatment for such problems is generally to administrate patients with antibiotics or antifungal agent. Alternatively, devices are taken out of the body to mechanically destroy the biofilm and re-used by surgery. In this study, a straightforward method was developed to remove biofilms using a MXene-based photothermal hydrogel. The hydrogel consists of dynamic crosslinking network formed by Schiff-base reaction between aldehyde-containing xyloglucan (OXG) and amine-containing MXene (NH2-MXene), which showed efficient killing of both gram-positive Staphylococcus aureus (S. aureus) and gram-negative Escherichia coli (E. coli) bacteria upon near-infrared (NIR) laser irradiation. The NH2-MXene/OXG nanocomposite hydrogel showed a high photothermal antibacterial efficiency and stable photothermal conversion, demonstrated by efficient removal of biofilms ex vivo.

Highly stretchable dynamic hydrogels for soft multilayer electronics.

Recent progress in the development of synthetic polymer networks has enabled the next generation of hydrogel-based machines and devices. The ability to mimic the mechanical and electrical properties of human tissue gives great potential toward the fields of bioelectronics and soft robotics. However, fabricating hydrogel devices that display high ionic conductivity while maintaining high stretchability and softness remains unmet. Here, we synthesize supramolecular poly(ionic) networks, which display high stretchability (>1500%), compressibility (>90%), and rapid self-recovery (<30 s), while achieving ionic conductivities of up to 0.1 S cm -1. Dynamic cross-links give rise to inter-layer adhesion and a stable interface is formed on account of ultrahigh binding affinities (>1013 M-2). Superior adherence between layers enabled the fabrication of an intrinsically stretchable hydrogel power source, paving the way for the next generation of multi-layer tissue mimetic devices.

Catalyst-Free Dynamic Covalent C=C/C=N Metathesis Reaction for Associative Covalent Adaptable Networks.

Covalent adaptable networks (CANs), leveraging the dynamic exchange of covalent bonds, emerge as a promising material to address the challenge of irreversible cross-linking in thermosetting polymers. In this work, we explore the introduction of a catalyst-free and associative C=C/C=N metathesis reaction into thermosetting polyurethanes, creating CANs with superior stability, solvent resistance, and thermal/mechanical properties. By incorporating this dynamic exchange reaction, stress-relaxation is significantly accelerated compared to imine-bond-only networks, with the rate adjustable by modifying substituents in the ortho position of the dynamic double bonds. The obtained plasticity enables recycle without altering the chemical structure or mechanical properties, and is also found to be vital for achieving shape memory functions with complex spatial structures. This metathesis reaction as a new dynamic crosslinker of polymer networks has the potential to accelerate the ongoing exploration of malleable and functional thermoset polymers.

Catalyst‐Free Dynamic Covalent C=C/C=N Metathesis Reaction for Associative Covalent Adaptable Networks

AbstractCovalent adaptable networks (CANs), leveraging the dynamic exchange of covalent bonds, emerge as a promising material to address the challenge of irreversible cross‐linking in thermosetting polymers. In this work, we explore the introduction of a catalyst‐free and associative C=C/C=N metathesis reaction into thermosetting polyurethanes, creating CANs with superior stability, solvent resistance, and thermal/mechanical properties. By incorporating this dynamic exchange reaction, stress‐relaxation is significantly accelerated compared to imine‐bond‐only networks, with the rate adjustable by modifying substituents in the ortho position of the dynamic double bonds. The obtained plasticity enables recycle without altering the chemical structure or mechanical properties, and is also found to be vital for achieving shape memory functions with complex spatial structures. This metathesis reaction as a new dynamic crosslinker of polymer networks has the potential to accelerate the ongoing exploration of malleable and functional thermoset polymers.

Constructing Dynamic Cross-Linking Networks as Durable Bifunctional Coating for Highly Stable Zinc Anodes.

The serious dendrite growth and H2O-induced side reactions on the Zn electrode lead to a significant fading in the cycling performance, hindering the development of commercial applications of aqueous Zn-ion batteries (AZIBs). Herein, a novel bifunctional network coating of dynamically cross-linking sodium alginate with trehalose has been rationally constructed on the Zn anode (Zn@AT). Firstly, the AT coating possesses abundant zinophilic oxygen-containing functional groups, which are able to induce uniform Zn2+ ion flux. Secondly, the AT coating as a solid barrier can effectively inhibit H2O-induced side reactions by lowering the activity of H2O molecules. More specially, based on the dynamic cross-linking, AT network coating is endowed with self-healing capacity during cycling for durable battery operation. Consequentially, Zn@AT anodes in symmetric cells can cycle stably for 2787 h at 2 mA cm-2/2 mAh cm-2, and even achieve a significantly long cycle performance of 1087 h at large charge/discharge depths of 10 mA cm-2/10 mAh cm-2. Moreover, the Zn@AT//MnO2 full cell shows excellent specific capacity of 175 mAh g-1 after 400 cycles. This study lights an effective strategy to enhance the durability of Zn electrodes in AZIBs.

Research on Toughening Polylactic Acid by an Epoxy Soybean Oil Curing Network Based on Dynamic Cross-Linking

Research on Toughening Polylactic Acid by an Epoxy Soybean Oil Curing Network Based on Dynamic Cross-Linking

Probing Viscoelastic Properties and Interfaces in High-Density Polyethylene Vitrimers at the Nanoscale Using Dynamic Mode Atomic Force Microscopy.

Vitrimers are a new class of heterogeneous polymers that combine the best features of thermosets with those of thermoplastics. The introduction of cross-links strongly changes the viscoelastic behavior of vitrimer materials. However, the characterization and understanding of the nanostructures and interfaces in vitrimers resulting from dynamic cross-linking formation remain a major challenge. Here, using dynamic modes of atomic force microscopy (AFM), namely intermodulation AFM (ImAFM) and AFM-based dynamic mechanical analysis (AFM-nDMA), local viscoelastic properties and interfaces at the nanoscale length of high-density polyethylene (HDPE) vitrimer materials are reported. ImAFM imaging in combination with the k-means clustering algorithm clearly reveals two distinct phases in the vitrimer system with highly different viscoelastic properties. AFM-nDMA further provides quantitative nanoviscoelastic properties at the nanoscale to confirm that there is a cross-linking-rich aggregation area forming a nanosize network structure in the cross-linking-poor matrix phase. The cross-linking-rich region shows a similar elastic modulus but much higher adhesion force measured by AFM compared to the cross-linking-poor HDPE matrix. Furthermore, the frequency influence on the local viscoelastic properties of HDPE vitrimer at the nanoscale was initially screened. The observed HDPE vitrimer nanostructures and viscoelastic properties at the nanoscale also provide explanations on the observed bulk HDPE vitrimer crystallinity decrease and dimensional stability increase compared to HDPE. Therefore, probing the viscoelastic properties and interfaces of HDPE vitrimer provides important insights into understanding of the correlations between the vitrimer nanostructure and the bulk mechanical and rheological behaviors.

Multibiofunctional Self-healing Adhesive Injectable Nanocomposite Polysaccharide Hydrogel.

Injectable hydrogels with good antimicrobial and antioxidant properties, self-healing characteristics, suitable mechanical properties, and therapeutic effects have great practical significance for developing treatments for pressing healthcare challenges. Herein, we have designed a novel, self-healing injectable hydrogel composite incorporating cross-linked biofunctional nanomaterials by mixing alginate aldehyde (Ox-Alg), quaternized chitosan (QCS), adipic acid dihydrazide (ADH), and copper oxide nanosheets surface functionalized with folic acid as the bioligand (F-CuO). Gelation was achieved under physiological conditions via the dynamic Schiff base cross-linking mechanism. The developed nanocomposite injectable hydrogel demonstrated the fast self-healing ability essential to bear deformation and outstanding antibacterial properties along with ROS scavenging ability. Furthermore, the optimized formulation of our F-CuO-embedded injectable hydrogel exhibited excellent cytocompatibility, blood compatibility, and in vitro wound healing performance. Taken together, the F-CuO nanosheet cross-linked injectable hydrogel composite presented herein offers a promising candidate biomaterial with multifunctional properties to develop solutions for addressing clinical challenges.

Fully Recycled Polyolefin Elastomer-Based Vitrimers with Ultra-High, Universal, Stable, and Switchable Adhesion.

Achieving both robust adhesion to arbitrary surfaces and thermal-switchable/recyclable properties has proven challenging, particularly for commodity polyolefins. Herein, a simple and effective route is reported to transform polyolefins elastomer (POE) into a fully recycled epoxy-functionalized POE vitrimers (E-POE vit) with ultra-high, universal, stable, and switchable adhesion via facile free radical grafting and dynamic cross-linking. The resultant E-POE vit exhibits increase in adhesion strength on glass exceeding three to ten times compared to those commonly used polymers, due to the synergy of dense hydrogen (H)-bonds and strong interfacial affinity. In addition, E-POE vit also displays strong adhesion on diverse surfaces ranging from inorganic to organic while maintaining good stability in various harsh environments. More importantly, temperature-sensitive H-bonds allow E-POE vit to switch between attachment-detachment at alternating temperatures, resulting in reversible adhesion without adhesion loss, even after 10 cycles. Moreover, E-POE vit is able to be fully recycled and reused more than ten times via thermo-activated transesterification reactions with negligible change in structure and performance. This work may unlock strategies to fabricate high-performance commercial polymer-based adhesives with adhesion and recyclable features for intelligent and sustainable applications.