Stable Adhesion Research Articles

Enzyme initiated in situ gelation as an oxygen-tolerant, high adhesive, and versatile strategy for hydrogel coating preparation

Hydrogel coatings have great potential for applications in antifouling, biomedical, and electronic fields, but the lack of preparation strategies with mild gel-forming conditions, high adhesion, and versatility hinders their widespread use. Herein, a method called glucose oxidase (GOD)-initiated in situ gelation (GOD-IIG) is developed for preparing hydrogel coatings. The procedure includes immobilizing Fe[Gly]2 and GOD on the surface of the substrates by forming an intermediate layer using epoxy resin, and then immersing the pre-treated substrates into a monomer solution to initiate polymerization. In situ gelation on the surface of the substrates is triggered by free radicals generated through the redox reaction between ferrous glycine (Fe[Gly]2) and hydrogen peroxide (H2O2) produced by the GOD-catalyzed glucose oxidation process, which can be carried out in open-air environments. Using the GOD-IIG method, hydrogel coatings constructed from common low-adhesive polymers displayed an adhesive strength of up to 686 kPa and stable underwater adhesion for at least 7 days. Moreover, this method shows controllable hydrogel thickness and recyclable monomer solution for at least 25 times at room temperature. It is also applicable to a variety of hydrogel structures and substrates, such as plastic, metal, and glass, regardless of flatness or geometry. In order to demonstrate the applications of hydrogel coatings prepared by GOD-IIG method, the lubrication and antifouling abilities of the coatings were assessed, and the results indicated that the coatings had good hydration lubrication as well as oil and biofouling resistance. This method holds promise for advancing the preparation of hydrogel coatings and has potential applications in the fields of electrical, biological, and environmental engineering.

Analysis of nonlinear bending behavior of nano-switches considering surface effects

Nano-switch structures are important control elements in nanoelectromechanical systems and have potential applications in future nanodevices. This paper analyzes the effects of surface effects, geometric nonlinearity, electrostatic forces, and intermolecular forces on the nonlinear bending behavior and adhesion stability of nano-switches. Based on the Von Karman geometric nonlinearity theory, four types of boundary conditions for the nano-switch structure were specifically calculated. The results show that surface effects have a significant impact on the nonlinear bending and adhesion stability of nano-switches. Surface effects increase the adhesion voltage of the nano-switch and decrease its adhesion displacement, and as the size of the nano-switch structure increases, the impact of surface effects decreases. A comparative analysis of the linear theory and the nonlinear theory results shows that the adhesion voltage predicted by the linear theory is smaller than that predicted by the nonlinear theory. The effect of geometric nonlinearity increases as the size of the nano-switch structure increases, as the distance between the electrodes increases, and as the aspect ratio of the nano-switch structure increases. These findings provide theoretical support and reference for the design and use of future nanodevices and nanoelectromechanical systems.

Abstract A019: TRIM29 enhances the invasion of bladder cancer cells by modulating the intermediate filament network and focal adhesions

Abstract Background: Bladder cancer patient treatment and outcomes are determined by the tumor’s ability to invade and metastasize. Our previous work has shown that TRIM29, also known as ATDC, is regulated by TP63 in basal bladder cancers, where it promotes cancer invasion and metastasis. We also observe that TRIM29 predominately localizes to intermediate filaments in invasive bladder cancer cells. Hypothesis: TRIM29 promotes the invasive progression of bladder cancer by regulating K14-containing intermediate filaments and focal adhesions. Methods: To test this hypothesis, we utilized cell culture models of bladder cancer, live cell imaging and 2D and 3D invasion assays to examine the role of TRIM29 in the regulation of K14, focal adhesions and the migration and invasion and bladder cancer cells. Results: We observed a physical interaction between TRIM29 and K14 filamentous structures in bladder cancer cells. We also found that TRIM29 and K14 regulate focal adhesion stability during bladder cancer invasion. Finally, we found that both K14 and the focal adhesion protein, zyxin (ZYX), are essential for bladder cancer migration and invasion, acting downstream of TRIM29. Conclusions: Our findings highlight a novel role for TRIM29 in regulating the cytoskeleton and focal adhesion dynamics during tumor cell invasion and suggest a potential therapeutic pathway for treating bladder cancer. Citation Format: Yin Wang, Nicole A. Jerome, Allan Kelleher, Marian L. Henderson, Mark Day, Pierre A. Coulombe, Phillip L. Palmbos. TRIM29 enhances the invasion of bladder cancer cells by modulating the intermediate filament network and focal adhesions [abstract]. In: Proceedings of the AACR Special Conference on Bladder Cancer: Transforming the Field; 2024 May 17-20; Charlotte, NC. Philadelphia (PA): AACR; Clin Cancer Res 2024;30(10_Suppl):Abstract nr A019.

Sea urchin-like nanocarrier for enhancing pesticide retention and rain fastness on hydrophobic and hydrophilic crop foliage

Foliar washoff by rainfall is a major factor inducing the inefficient utilization of pesticides. Enhancing the adhesion and retention of pesticide on plant foliage has long been of interest. The presence of waxy platelets on most plant foliage surfaces renders them rough and hydrophobic. This reduces the area of contact between pesticide particle and plant foliage, which decreases the adhesion. In this study, we developed a pesticide nanocarrier (PANI/HACC) with sea urchin-like surface morphology based on polyaniline (PANI) doped with biodegradable 2-hydroxypropyltrimethyl ammonium chloride chitosan (HACC). Then, azoxystrobin (AZOX) loaded nanoparticles (AZOX@PANI/HACC) was synthesized by physical adsorption. It exhibited retention rates of 61.4% on rice leaves and 64.6% on cucumber leaves, which were higher than that of commercially available azoxystrobin water dispersible granules (AZOX-WDG, 42.1% and 24.5%, respectively) and suspension concentrates (AZOX-SC, 23.1% and 58.8%, respectively). Additionally, pot experiments demonstrated that the control efficacy of AZOX@PANI/HACC on rice against Rhizoctonia solani was 1.64-fold and 3.0-fold of that of AZOX-WDG and AZOX-SC, respectively. The higher retention performance of AZOX@PANI/HACC was attributed to the stable adhesion by fitting nanometer-sized spikes into the spaces between the waxy platelets. Overall, the pesticide nanocarrier with spiky surface morphology provides an effective strategy for improving pesticide retention and reducing pesticide loss in agricultural production.

Bioprinting of Stable Bionic Interfaces Using Piezoresistive Hydrogel Organoelectronics.

Bionic tissues offer an exciting frontier in biomedical research by integrating biological cells with artificial electronics, such as sensors. One critical hurdle is the development of artificial electronics that can mechanically harmonize with biological tissues, ensuring a robust interface for effective strain transfer and local deformation sensing. In this study, a highly tissue-integrative, soft mechanical sensor fabricated from a composite piezoresistive hydrogel. The composite not only exhibits exceptional mechanical properties, with elongation at the point of fracture reaching up to 680%, but also maintains excellent biocompatibility across multiple cell types. Furthermore, the material exhibits bioadhesive qualities, facilitating stable cell adhesion to its surface. A unique advantage of the formulation is the compatibility with 3D bioprinting, an essential technique for fabricating stable interfaces. A multimaterial sensorized 3D bionic construct is successfully bioprinted, and it is compared to structures produced via hydrogel casting. In contrast to cast constructs, the bioprinted ones display a high (87%) cell viability, preserve differentiation ability, and structural integrity of the sensor-tissue interface throughout the tissue development duration of 10 d. With easy fabrication and effective soft tissue integration, this composite holds significant promise for various biomedical applications, including implantable electronics and organ-on-a-chip technologies.

Combining the Tunnel Orbicularis Oculi Muscle Flap Technique With Skin Grafting for Enhanced Adhesion in Burn-Induced Ectropion Repair.

Scar contracture of the eyelid following facial burns often has adverse consequences. Total cicatricial contracture often makes adjustment flap translation challenging to implement. Previously used upper and lower eyelid adhesion methods are ineffective for patients with severe cicatricial contracture, and ectropion can easily recur. This study aimed to retrospectively examine upper and lower eyelid adhesions using an orbicularis oculi muscle flap and verify its stability. In patients with ectropion caused by severe scar contracture following head and face burns, we employed a tunnel orbicularis oculi muscle flap technique, which involved creating a tunnel between the skin and the tarsal plate of the eyelid, mobilizing the orbicularis oculi muscle, and rotating it into this tunnel to provide stable adhesion of the upper and lower eyelids. Full-thickness skin grafting was then performed. The eyelids were examined postoperatively to determine whether reoperation was necessary and to monitor for any potential complications. This study included 26 patients and 46 eyes. No accidental disconnection occurred after eyelid adhesion, which lasted for an average of 21.87 ± 10.08 months before the eyelid adhesion was cut open. No complications or adverse reactions occurred, and the adhesions did not break unexpectedly. Repairing eyelid ectropion with the tunnel orbicularis oculi muscle flap is a simple procedure that immediately creates tension against upper and lower eyelid contractures, providing long-term stable adhesion. This method avoids structural disorders, such as eyelid margin scarring, minimally influences surrounding tissues, and has few postoperative complications. It holds great value for repairing eyelid tissue defects and warrants further study.

Metallization of polypropylene substrates through surface functionalization and physical vapor deposition of chromium coatings

Physical vapor deposition (PVD) of chromium coatings represents an interesting alternative to electroplating to obtain metallized plastic parts for a variety of manufacturing sectors. This process is however hampered by the limited adhesion of the metallic layer on the underlying polymeric substrates. Within this context, PVD metallization of polypropylene substrates has so far been particularly challenging given the low surface energy and poor wettability of this commodity plastics. To address this issue, a comprehensive approach is proposed here to enable the production of PVD-metallized PP substrates with excellent and stable interlayer adhesion. The adhesive properties of the PP substrate are modified by a selective UV-induced photografting process in which vinyl-, glycidyl- or 2-hydroxyethyl methacrylate species are covalently attached to the PP surface, as confirmed by Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy and surface wettability measurements. Based on the chemistry of the photografted functionality, different resin systems are selected and investigated for use as primers to enable subsequent chromium deposition, including acrylic, epoxy and polyurethane systems. The effect of the photografting process on the adhesion between PP and the primers is systematically assessed by means of pull-off tests, highlighting a significant improvement of the adhesion force after surface functionalization with appropriate grafting agents. Finally, functionalized PP substrates are chromated through PVD, obtaining homogeneous and crack-free chromium surfaces upon judicious selection of suitable primer-grafting agent combinations. This also led to outstanding interlayer adhesion and micromechanical performance. This work provides the first demonstration of chromium-metallization of PP substrates via PVD for metallized plastic components with excellent surface characteristics, and paves the path for the design of mechanically durable and aesthetically-compliant PVD-metallized PP components.

A multiscale study of the influence of aggregate type on adhesion at the asphalt–aggregate interface

In order to examine the influence of aggregate type on the asphalt–aggregate interface, the adhesion performance between asphalt and aggregate was investigated at three scales. The pull-out test was conducted on asphalt and three kinds of aggregates at the macroscale to directly estimate the adhesion performance between them. At the microscale, the surface energies between asphalt and limestone, basalt, and andesite were examined through a surface energy experiment, and then the adhesion and debonding work were assessed. At the nanoscale, the interfacial behavior between six mineral compositions (SiO2, CaO, MgO, Al2O3, Fe2O3, and Na2O) of these aggregates and asphalt was determined using molecular dynamics simulation. The correlation of adhesion work at the microscale and nanoscale was further explored to unveil the bonding mechanisms between asphalt and aggregate. The macroscale results indicate that the adhesion force of andesite is slightly greater than that of limestone, probably because andesite has a greater surface roughness than limestone. The microscale results show the best adhesion and water stability between asphalt and limestone. The finding further explains that alkaline aggregates exhibit superior interfacial adhesion to asphalt. The nanoscale results show that the adhesion work of alkaline oxides with asphalt is more significant than that of acidic oxides with asphalt. Limestone and basalt have better adhesion to asphalt due to higher alkaline oxide content, while andesite has poorer adhesion to asphalt due to lower alkaline oxide and higher SiO2 content. The interfacial adhesion work increases from the microscale to the nanoscale by a factor of 2.91–4.75.

3D concrete printing for tunnel linings: Opportunities and challenges

The use of shotcrete for hard rock tunnel linings has drawbacks such as irregular surfaces and rebounds. By contrast, extrusion-based 3D concrete printing presents a promising solution with precise deposition and reduced rebound. This study discusses the potential of 3D printing for tunnel linings, focusing on mitigating shear failure and addressing interfacial detachment. Achieving high strength early for stable adhesion to rock surfaces is paramount for countering shear failure. A twin-pipe pumping system was introduced utilizing a helical static mixer to blend concrete involving chemical triggers, effectively managing the stiffness and fluidity during pumping. In addition, the adhesion to the substrate must be addressed. Based on the above discussion, this study offers insights into the fundamental challenges, paving the way for advancing extrusion-based 3D concrete printing for tunnel linings.

PH-responsive bioadhesive with robust and stable wet adhesion for gastric ulcer healing

Development of bioadhesives that can be facilely delivered by endoscope and exhibit instant and robust adhesion with gastric tissues to promote gastric ulcer healing remains challenging. In this study, an advanced bioadhesive is prepared through free radical polymerization of ionized N-acryloyl phenylalanine (iAPA) and N-[tris (hydroxymethyl) methyl] acrylamide (THMA). The precursory polymer solution exhibits low viscosity with the capability for endoscope delivery, and the hydrophilic-hydrophobic transition of iAPA upon exposure to gastric acid can trigger gelation through phenyl groups assisted multiple hydrogen bonds formation and repel water molecules on tissue surface to establish favorable environment for interfacial interactions between THMA and functional groups on tissues. The in-situ formed hydrogel features excellent stability in acid environment (14 days) and exhibits firm wet adhesion to gastric tissue (33.4 kPa), which can efficiently protect the wound from the stimulation of gastric acid and pepsin. In vivo studies reveal that the bioadhesive can accelerate the healing of ulcers by inhibiting inflammation and promoting capillary formation in the acetic acid-induced gastric ulcer model in rats. Our work may provide an effective solution for the treatment of gastric ulcers clinically.

Multiscale Synergistic Gecko-Inspired Adhesive for Stable Adhesion under Varying Preload and Surface Roughness.

Inspired by geckos, fibrillar microstructures hold great promise as controllable and reversible adhesives in the engineering field. However, enhancing the adhesion strength and stability of gecko-inspired adhesives (GIAs) under complex real-world contact conditions, such as rough surfaces and varying force fields, is crucial for its commercialization, yet further research is lacking. Here, we propose a hierarchically designed GIA, which features a silicone foam (SF) backing layer and a film-terminated fibrillar microstructure under a subtle multiscale design. This structure has been proven to have a "multiscale synergistic effect", allowing the material to maintain strong and stable adhesion to surfaces with changing normal pressures and roughness. Specifically, under a high load, the adhesive strength is 2 times more than that of conventional GIA, and it is 1.5 times stronger on rough surfaces compared to conventional GIA. Under high pressure and high surface roughness simultaneously, the adhesive strength is 3.3 times higher compared to conventional GIA. Our research demonstrates that the synergistic effect of multiscale biomimetic adhesion structures is highly effective in enhancing the adhesive strength of GIA under some harsh contact conditions.

Shape-adaptive underwater adhesive based on supramolecular assembly for robustly integrated underwater wireless sensing/communication and bioelectronic adhesion

Developing multifunctional supramolecular adhesives, capable of instant underwater adhesion and multi-responsive sensing, is crucial for marine exploitation. However, producing underwater conductive adhesives that can effectively bind and conform to the complex contours of substrate surfaces is challenging. Herein, drawing inspiration from traditional gourmet “gluten” processing, we devised an “one-pot kneading-washing” supramolecular assembly strategy to engineer a shape-adaptive multifunctional underwater electroactive adhesive (e-PT/GS) for underwater sensing/communication and leakage sealing. Utilizing multiple non-covalent interactions, e-PT/GS demonstrated excellent electrical conductivity, underwater self-healing capability, anti-swelling properties, and the ability to achieve rapid, stable, and long-lasting underwater adhesion to a wide range of substrates in various harsh environments (e.g., acids, alkalis, seawater, and salt solutions). E-PT/GS exhibited anticipative shape-adaptability, repelling interfacial water and filling irregularities on the substrate surface, thereby establishing tight and unprecedentedly adaptable underwater contact with the substrates. In combination with the multi-dimensional sensing origins, e-PT/GS was utilized for underwater sealing and in-situ real-time monitoring of signals from the sealing points. Additionally, it was applied in body motion perception, wireless and underwater communications and enabled the collection of steady and authentic ECG signals. The proposed novel strategy is expected to significantly advance the design and applications of the next-generation conductive underwater adhesives.

Adhesion Stability According to Adhesion Area of Traditional Tile Gluing Method

In this study, verification was conducted through experiments to identify problems caused by traditional attachment methods in order to highlight the need for a suitable attachment method for new tile types according to changes in materials, production technology, and demand. The stability of adhesion strength was evaluated by subdividing the size of the adhesion area and adhesion strength measurement method for the country-type attachment method. The adhesion area on the back of the tile was divided into 60% and 80%, and the test specimens used in the experiment were tested for partial adhesion strength (Ta-1), overall adhesion strength (Ta-2), and adhesion strength after splitting (Ta-3), and the results were derived. As a result of conducting the adhesion test presented in the current national building standard tile specification (KCS 41 48 01) for 80% of the backfill area, the average adhesive strength was 0.85 N/mm2, and the standard strength was 0.39 N/mm2. However, as a result of the arithmetic average test of the adhesive strength of all tiles or cutting of the entire tile, rather than the partial adhesion test method of the mortar-attached part, it was confirmed that the adhesive strength was about −20% less than the current KCS 0.39 N/mm2.

Non-swelling polyelectrolyte complex hydrogels with tissue-matchable mechanical properties for versatile wet wound closure

The stable adhesion of hydrogel-based bioadhesives with tissue-matchable mechanical properties in biological environments remains a significant challenge. In this work, we propose a polyethyleneimine-polyacrylic acid (PEI-PAA, PEA) double-network polyelectrolyte hydrogel with swelling resistant capacity and tunable mechanical properties via one-step UV-initiated polymerization. Driven by electrostatic interactions and polymer-chain entanglement, this PEA hydrogel displays a distinctive microphase separation behavior, which facilitates a wide tunability in mechanical properties. Specifically, the modulus varies from 0.4 MPa to 106 MPa, and the toughness ranges from 1479 kJ/m3 to 7641 kJ/m3, respectively. Besides, the microphase separation endows PEA hydrogel with notable anti-swelling properties in saline, TBS buffer, and blood, leading to consistent adhesion to diverse moist tissues. We further demonstrate that our PEA hydrogels provide matchable mechanical properties and long-lasting adhesion to rat skin and arteries, which promote skin injury healing and effectively halt artery rupture bleeding in vivo. This work presents a straightforward method to generate non-swelling hydrogels and offers novel insight into the development of bioadhesives to meet diverse mechanical requirements.

Connecting Interfacial Mechanical Adhesion, Efficiency, and Operational Stability in High Performance Inverted Perovskite Solar Cells

Connecting Interfacial Mechanical Adhesion, Efficiency, and Operational Stability in High Performance Inverted Perovskite Solar Cells

Modification of Petroleum Bitumen with Secondary Polyethylene in the Presence of Vermiculite

This article presents studies on the modification of petroleum bitumen with polymer waste in the presence of vermiculite. An increase in temperature leads to an increase in the interaction of components, partial breakage of polyethylene and bitumen macromolecules, and the formation of radical-free valences. As a result, fragments of polyethylene and bitumen molecules react with each other, and the formation of qualitatively new structural formations occurs via the strong connection of polar and amorphous bitumen with nonpolar structurally viscous polyethylene. Domestically produced Kulantau vermiculite was used to ensure stable adhesion over a wide temperature range and increase the specific surface area, which acquired additional energy, resulting in an increase in the degree of adhesion to bitumen and increased durability of the binder with improved rheological characteristics. Because of the increased service life of road asphalt pavements, the use of the latter results in a considerable decrease in the cost of polymer-bitumen binders. Based on improved binder formulations, asphalt concrete exhibits excellent water resistance and strength at 50 °C (4.7 to 5.0 MPa). In summary, the modification of bitumen with polymer waste and vermiculite offers a promising avenue for improving the performance and longevity of asphalt pavements.

Tyrosinase-Modified UHMW SELP Polymers as Wet and Underwater Adhesives to Achieve Multi-interface Adhesion.

The presence of a hydration layer in humid and underwater environments challenges adhesive-substrate interactions and prevents effective bonding, which has become a significant obstacle to the development of adhesives in the industrial and biomedical fields. In this study, ultrahigh-molecular-weight (UHMW) silk-elastin-like proteins (SELP) with 3,4-dihydroxyphenylalanine (DOPA) converted from tyrosine residues by tyrosinase exhibited excellent adhesive properties on different interfaces, such as glass, aluminum, wood, polypropylene sheets, and pigskin, under both dry and wet conditions. Additionally, by incorporating trace amounts of cross-linking agents like Fe3+, NaIO4, and tris(hydroxymethyl) phosphine (THP), the mussel-inspired adhesives maintained a stable and excellent adhesion, broadening the conditions of application. Notably, the UHMW SELP adhesive exhibited remarkable underwater adhesion properties with a shear strength of 0.83 ± 0.17 MPa on glass. It also demonstrated good adhesion to biological tissues including the kidney, liver, heart, and lungs. In vitro cytocompatibility testing using L929 cells showed minimal toxicity, highlighting its potential application in the biomedical field. The sustainable, cytocompatible, cost-effective, and highly efficient adhesive provides valuable insights for the design and development of a new protein-based underwater adhesive for medical application.

Effect of aging on micromechanical behavior of asphalt surfaces using an atomic force microscope

The micro-mechanical properties of asphalt surfaces are significantly impacted by short-term aging during construction and long-term aging in service. This, in turn, affects macroscopic characteristics such as asphalt-aggregate adhesion and water stability of asphalt mixtures. The study investigated different aging processes had different impacts on the micromechanical properties of the asphalt on the surface. The short-term aging process had the most significant effects, while the subsequent long-term aging had similar but less important effects. The adhesion, surface energy, and Young's modulus of five different types of asphalt using atomic force microscopy (AFM) in their original state, after short-term aging through the Rolling Thin Film Oven Test (RTFOT), and after long-term aging through the RTFOT+Pressure Aging Vessel (PAV). The results showed that ZH and SK asphalts had a distinct "bee structure", and aging had varying effects on adhesion, surface energy, and Young's modulus in different areas (peak, valley, and other region). Before and after asphalt aging, the adhesion and surface energy approximately followed the order other region > peak > valley, while Young's modulus approximately followed the peak>valley> other region. This indicates that the bumpy "bee structure" does not always correspond to higher modulus or lower adhesion. It was also found that ZH asphalt and SK asphalt with a "bee structure" exhibited better aging resistance compared to KL asphalt without a "bee structure". The study also revealed that aging led to decreased adhesion and surface energy, while increasing Young's modulus. This finding indicates that as asphalt ages, adhesion decreases and asphalt elasticity increases. Additionally, it was observed that the modified asphalt showed less change in adhesion, surface energy, and Young's modulus after aging compared to the matrix asphalt, indicating that SBS modifiers contribute to improving the aging resistance of asphalt. These results will provide a good reference for understanding the microscopic changes in asphalt aging properties.

A smart band-aid with temperature and reactive oxygen species dual-responsiveness for synergistic mechanical and pharmacological therapy of chronic wounds

In this study, a dual-responsive multifunctional band-aid comprising a force-induced shrinkage layer and a drug-treated layer has been developed, characterized by its on-demand drug release. Evaluated through the pig skin the force-induced shrinkage layer facilitates active wound closure by forming stable adhesion to the skin. Afterward, the layer could provide mechanical force simulating the embryonic skin in response to temperature changes. Concomitantly, confronting the increased levels of reactive oxygen species (ROS) at the wound site, the drug-treated layer made of an ROS-responsive hydrogel, promptly releases zinc oxide (ZnO) and catalase (CAT) to exert antibacterial and anti-inflammatory stress effects, ultimately accelerating the healing process of chronic wounds. More important, this versatile hydrogel-based band-aid demonstrates remarkable efficacy in both bacteria-infected rat wounds and rat tooth extraction wounds. Overall, the versatility of this approach presents a comprehensive and convenient strategy for the treatment of clinical chronic wounds.

Solvent and low temperature resistant natural polyphenolic adhesives

The development of robust and bioinspired adhesives with excellent performances including fast gel time, low cost, good adhesion strength and stability, and excellent solvent and temperature resistance against harsh environment is urgent for practical applications. In this paper, kinds of natural polyphenolic adhesives have been successfully fabricated via the multiple polyphenol-diisocyanate cross-linking (PDC) reactions between natural polyphenols (extracts) and diisocyanate molecules. Under heating, as-prepared adhesives could effectively adhere onto a wide range of substrates (i.e. PTFE, PET, PMMA, Al, Cu, paper, glass, wood) through hierarchical interactions. Moreover, these adhesives exhibited great adhesion stability against complex solvents and low-temperature environments, whose adhesion strength could remain unchanged after soaking solvents after 30 days, which was conducive to their potential applications in industry and chemical fields, including petroleum, wood, metal, glass, plastics, and rubber adhesion. We believed that this work would provide new strategies towards the preparation of robust adhesives with excellent resistant against various solvents and low temperature for many fields by using naturally occurring building blocks.