Effect Of Crosslinking Research Articles

Synergistic crosslinking effect of hydroxyethyl cellulose and montmorillonite on the improvement of mechanical and electrochemical properties of polyvinyl alcohol hydrogel

Flexible solid-state zinc-ion battery is promising energy technology with low cost, excellent performance, and safety. However, the mechanical properties of flexible electrolytes are severely limited. Here, hydroxyethyl cellulose (HEC) and montmorillonite (MMT) were introduced into a polyvinyl alcohol (PVA) matrix to prepare a novel composite hydrogel using a repeated freeze-thaw method. Both organic HEC and inorganic MMT could form hydrogen bonds with PVA molecular chains, acting as crosslinkers to construct a well-networked hydrogel structure. The synergistic effect of these two crosslinkers significantly enhanced the mechanical properties of the composite hydrogel. The composite hydrogel prepared with 3 wt% HEC and 2 wt% MMT (denoted as P–H3%-M2%) exhibited a 242.6% increase in tensile strength, 78.6% increase in elongation at break, and 970.1% increase in compressive strength compared to pure PVA hydrogel. P–H3%-M2% hydrogel also demonstrated a high electrolyte uptake rate (199.15%) and ion conductivity (24.6 mS cm−1). When assembled in a Zn symmetric battery, it maintained stable operation for 3000 h with a low polarization voltage of approximately 70 mV. Furthermore, P–H3%-M2% hydrogel assembled in a Zn//MnO2 battery exhibited a discharge specific capacity of 218 mAh g−1 at a current density of 0.15 A g−1, with 91% capacity retention after 450 cycles. At a higher current density of 1.5 A g−1, it showed a discharge specific capacity of 108 mAh g−1, which is 4.5 times higher than that of the PVA hydrogel battery, demonstrating excellent rate performance.

Structural Effect of Cyclic Olefin Cross-Linkers on Long-Wave Infrared-Transmitting Sulfur Polymers

Structural Effect of Cyclic Olefin Cross-Linkers on Long-Wave Infrared-Transmitting Sulfur Polymers

Ultrarapid Gelation of Porous Ti3C2Tx MXene Monoliths Induced by Ionic Liquids.

Gelation is a promising method to assemble 3D macroscopic structures from MXene sheets for various applications. However, the fine control and scalable manufacturing of 3D MXene monoliths remains a great challenge. Herein, the controllable gelation of Ti3C2Tx MXene initiated by various ionic liquids (ILs) is first proposed, where the IL serve as linkers to bond the nanosheets together through electrostatic and hydrogen bonding interactions, forming 3D monoliths with well-adjustable structure. Furthermore, density functional theory calculations and experiments further reveal the cross-linking effect of different ILs. Typically, 3D porous structure with high specific surface area, suitable pore size, and improved electrolyte affinity is designed through the cross-linking of Ti3C2Tx with 1-vinyl-3-ethylimidazole bromide ([C2VIm]Br-Ti3C2Tx). Due to the strong coupling, the as-synthesized monolith possesses excellent rate performance and high energy density. The methodology is quite flexible, controllable, and universal that provides a new perspective for promoting innovative applications of 2D materials.

Coarse-grained molecular dynamics simulation of the effect of cross-linking on the wear mechanism of polymer brush

Abstract The effects of a cross-linking layer on the wear resistance of polymer brush were investigated by using molecular dynamics-based sliding simulations. We found that a cross-linking layer improved wear resistance. The cross-linking layer suppressed the interpenetration of polymer chains on the counter surface and thus lowered the frictional force and wear. The degrees of interpenetration decreased as the cross-linking layer closed to the tip of the chain. A cross-linking layer in the tip of the polymer chains was thus found to improve wear resistance most effectively.

Corneal Collagen Crosslinking for Ectasia After Refractive Surgery: A Systematic Review and Meta-Analysis.

Corneal ectasia leads to progressive irregular corneal curvature and reduced visual acuity. To assess the safety and effectiveness of corneal collagen cross-linking (CXL) for managing corneal ectasia resulting from refractive laser surgery (RSL). A systematic review and meta-analysis were realized according to PRISMA guidelines. We searched PubMed, EMBASE, Cochrane, and Web of Science databases for studies on CXL in patients with ectasia after RLS. The outcomes of interest included visual acuity, refractive outcomes, topographic parameters (Kmax, index surface variance (ISV), index of Vertical Asymmetry (IVA), keratoconus index (KI), central keratoconus index (CKI), index of height asymmetry (IHA), index of height decentration (IHD) and Rmin (minimum sagittal curvature)), central corneal thickness, endothelial cell count, and possible adverse events. Statistical analysis was performed using the R software (version 4.2.3, R Foundation for Statistical Computing, Vienna, Austria). 15 studies encompassing 421 patients (512 eyes) were included. The mean age was 32.03 ± 4.4 years. The pooled results showed a stable uncorrected visual acuity post-CXL, with a significant improvement in corrected distance visual acuity (SMD = 0.09; 95% CI: -0.07 to 0.26). The spherical equivalent decreased significantly (SMD = -0.09; 95% CI: -0.35, -0.02). The topographic parameter Kmax decreased significantly (SMD = 0.15; 95% CI:0.01 to 0.28); however, the other parameters, ISV, IVA, KI, CKI, IHA, IHD, and Rmin, did not change significantly. Central corneal thickness decreased significantly (SMD = 0.24; 95% CI:0.07 to 0.41), and the endothelial cell count remained stable The complications were rare. CXL is a safe and effective technique for managing corneal ectasia after RLS.

Effect on thermal, mechanical, and biodegradable properties of plasma‐treated fish scale powder/linear low‐density polyethylene polymer composite films

AbstractIn the present work, we report the effect of low‐temperature plasma treatment on thermal, mechanical, and biodegradable properties of polymer composite blown films prepared from carp fish scale powder (CFSP) and linear low‐density polyethylene (LLDPE). The CFSP was melt compounded with LLDPE using a filament extruder to prepare 1, 2, and 3 wt.% of CFSP in LLDPE polymer composite filaments. These filaments were further pelletized and extruded into blown films. The blown films extruded with 1, 2, and 3 wt.% of CFSP in LLDPE were tested for thermal and mechanical properties. It was observed that the tensile strength decreased with the increased loading content of CFSP, and 1% CFSP/LLDPE exhibited the highest tensile strength. To study the effect of low‐temperature plasma treatment, 1% CFSP/LLDP polymer composite with high tensile strength was plasma treated with O2 and SF6 gas before blow film extrusion. The 1% CFSP/LLDPE/SF6‐extruded blown films showed increased thermal decomposition, crystallinity, tensile strength, and modulus. This may be due to the effect of crosslinking by the plasma treatment. The maximum thermal decomposition rate, crystallinity %, tensile strength, and modulus obtained for 1% CFSP/LLDPE/SF6 film were 500.02°C, 35.79, 6.32 MPa, and 0.023 GPa, respectively. Furthermore, the biodegradability study on CFSP/LLDPE films buried in natural soil for 90 days was analyzed using x‐ray fluorescence. The study showed an increase in phosphorus and calcium mass percent in the soil. This is due to the decomposition of the hydroxyapatite present in the CFSP/LLDPE biocomposite.

Fabrication of Highly Efficient and Ambient Stable Planar MAPbI3 Perovskite Solar Cells via Defect Passivation through Crosslinking Strategy

Iodine‐based hybrid planar perovskite solar cells’ (PSCs) overall performance is still very limited. In this work, a highly functionalized iodine‐based hybrid perovskite layer is fabricated by incorporating trimethylolpropane ethoxylated triacrylate (TET) within the perovskite precursor, which can crosslink with the grain boundaries to improve the crystallinity as well as the grain size and passivate the defect states of the perovskite material. The MAPbI3‐based thin films with TET exhibited large grain sizes from 195.73 to 587.49 nm with 8 mg mL−1 of TET concentration. The X‐ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), energy dispersive X‐ray (EDX) elemental mapping, photoluminescence (PL), and time resolved photoluminescence (TRPL) characterization results suggest the strong crosslinking effect between TET and MAPbI3, which improves the crystallinity and reduces the charge trap density. Planar PSCs is fabricated with the device architecture fluorine‐doped tin oxide (FTO)/c‐TiO2/MAPbI3:TET/Spiro‐MeOTAD/Au and achieved a power conversion efficiency (PCE) of 14.75% under 1.5 AM light illumination. The fabricated PSCs shows excellent ambient stability which retains 80% of their PCE after being exposed to the ambient environment of relative humidity (RH) ≈60%, room temperature (RT) ≈27 °C without any encapsulation.

Strong and tough poly(vinyl alcohol)/xanthan gum-based ionic conducting hydrogel enabled through the synergistic effect of ion cross-linking and salting out

The mechanical properties of ionic conductive hydrogels (ICHs) are generally inadequate, leading to their susceptibility to breakage under external forces and consequently resulting in the failure of flexible electronic devices. In this work, a simple and convenient strategy was proposed based on the synergistic effect of ion cross-linking and salting out, in which the hydrogels consisting of polyvinyl alcohol (PVA) and xanthan gum (XG) were immersed in zinc sulfate (ZnSO4) solution to obtain ICHs with exceptional mechanical properties. The salt-out effects between PVA chains and SO42− ions along with the cross-linked network of XG chains and Zn2+ ions contribute to the desirable mechanical properties of ICHs. Notably, the mechanical properties of ICHs can be adjusted by changing the concentration of ZnSO4 solution. Consequently, the optimum fracture stress and the fracture energy can reach 3.38 MPa and 12.13 KJ m−2, respectively. Moreover, the ICHs demonstrated a favorable sensitivity (up to 2.05) when utilized as a strain sensor, exhibiting an accurate detection of human body movements across various amplitudes.

Effect of carbonyl-amino condensation, non-covalent cross-linking and conformational changes induced by ultrasound-assisted Maillard reaction on lysinoalanine formation in silkworm pupa protein

The inhibition of cross-linked lysinoalanine (LAL) formation in silkworm pupa protein isolates (SPPI) by Maillard reaction (using varying xylose concentration) and ultrasound treatment was studied. Results showed that sonicated SPPI was effectively grafted with high concentration of xylose (5 %), resulting in the lowest LAL content, which was 48.75 % and 30.64 % lower than the control and ultrasound-treated samples, respectively. Chemical bond analysis showed that the combined treatment destroyed the ionic bonds, intrachain (g-g-t), and interchain (g-g-g) disulfide bonds, but stimulated the polymerization of hydrogen and hydrophobic bonds between SPPI and xylose, and as well enhanced the net negative charge between SPPI/Xylose complexes. The particles of the complexes were more loose, dispersed and rough, and had a stronger hydrophilic microenvironment, accompanied by alterations in microscopic, secondary and tertiary structures. Ultrasound treatment induced the breakdown of the oxidative cross-linking in SPPI, and promoted the sulfhydryl group-dehydroalanine binding and the carbonyl-amino condensation of the protein and xylose, and thus inhibited the formation of cross-linked LAL. Furthermore, the physicochemical and structural parameters were highly interrelated with cross-linked LAL content (|r| > 0.9). The outcomes provided a novel avenue and theoretical basis for minimizing LAL formation in SPPI and improving the nutrition and safety of SPPI.

Investigating the influence of collagen cross-linking on mechanical properties of thoracic aortic tissue.

Vascular diseases, such as abdominal aortic aneurysms, are associated with tissue degeneration of the aortic wall, resulting in variations in mechanical properties, such as tissue ultimate stress and a high slope. Variations in the mechanical properties of tissues may be associated with an increase in the number of collagen cross-links. Understanding the effect of collagen cross-linking on tissue mechanical properties can significantly aid in predicting diseased aortic tissue rupture and improve the clarity of decisions regarding surgical procedures. Therefore, this study focused on increasing the density of the aortic tissue through cross-linking and investigating the mechanical properties of the thoracic aortic tissue in relation to density. Uniaxial tensile tests were conducted on the porcine thoracic aorta in four test regions (anterior, posterior, distal, and proximal), two loading directions (circumferential and longitudinal), and density increase rates (0%-12%). As a result, the PPC (Posterior/Proximal/Circumferential) group experienced a higher ultimate stress than the PDC (Posterior/Distal/Circumferential) group. However, this relationship reversed when the specimen density exceeded 3%. In addition, the ultimate stress of the ADC (Anterior/Distal/Circumferential) and PPC group was greater than that of the APC (Anterior/Proximal/Circumferential) group, while these findings were reversed when the specimen density exceeded 6% and 9%, respectively. Finally, the high slope of the PDL (Posterior/Distal/Longitudinal) group was lower than that of the ADL (Anterior/Distal/Longitudinal) group, but the high slope of the PDL group appeared larger due to the stabilization treatment. This highlights the potential impact of density variations on the mechanical properties of specific specimen groups.

Chitosan-Based Hierarchical Scaffolds Crosslinked with Genipin

Osteochondral defects present significant challenges for effective tissue regeneration due to the complex composition of bone and cartilage. To address this challenge, this study presents the fabrication of hierarchical scaffolds combining chitosan/β-tricalcium phosphate (β-TCP) to simulate a bone-like layer, interconnected with a silk fibroin layer to mimic cartilage, thus replicating the cartilage-like layer to mimic the native osteochondral tissue architecture. The scaffolds were produced by freeze-drying and then crosslinking with genipin. They have a crosslinking degree of up to 24%, which promotes a structural rearrangement and improved connection between the different layers. Micro-CT analysis demonstrated that the structures have distinct porosity values on their top layer (up to 84%), interface (up to 65%), and bottom layer (up to 77%) and are dependent on the concentration of β-tricalcium phosphate used. Both layers were confirmed to be clearly defined by the distribution of the components throughout the constructs, showing adequate mechanical properties for biomedical use. The scaffolds exhibited lower weight loss (up to 7%, 15 days) after enzymatic degradation due to the combined effects of genipin crosslinking and β-TCP incorporation. In vitro studies showed that the constructs supported ATDC5 chondrocyte-like cells and MC3T3 osteoblast-like cells in duo culture conditions, providing a suitable environment for cell adhesion and proliferation for up to 14 days. Overall, the physicochemical properties and biological results of the developed chitosan/β-tricalcium phosphate/silk fibroin bilayered scaffolds suggest that they may be potential candidates for osteochondral tissue strategies.

Evolution of the structure and tribological behavior of the organic coatings under gamma-ray irradiation

More reliable and long-term irradiation stability is essential for lubrication protection materials that served in nuclear energy equipment. In this paper, three typical commercially organic bonded solid lubricating coatings were chosen to investigate the influence of gamma (γ)-ray irradiation on microstructure and tribological behaviors. The evolution of microstructure and the changes of tribological properties for these coatings after irradiation were comparatively studied in detail. The results revealed that the crystallinity of the molybdenum disulfide (MoS2) lubricating phase was improved and were partial oxidized in the coatings after γ-ray irradiation, resulting in the surface roughness of the coating with MoS2 as the solid lubricating phase decreased significantly. The polytetrafluoroethylene (PTFE) lubricating phase was degraded from the long chains structure to smaller molecules after γ-ray irradiation. The results of tribological properties of the three coatings after γ-ray irradiation indicated that, for polyamide-imide-based lubricating coatings, the friction coefficient is decreased and the wear rate is increased after irradiation. For phenolic epoxy-based lubricating coating, the cross-linking effect of γ-ray irradiation predominated to improve the wear resistance and prolong the wear life of the coating. But overall, the influence of irradiation on tribological properties of three polymer-based coatings could almost be neglected duo to the changes of the microstructure in nanoscale. This work provides path and direction for design and preparation of the lubricating coatings that served in a nuclear reactor.

Using bacterial cellulose to bridge covalent and physical crosslinks in hydrogels for fabricating multimodal sensors

Network optimization is vital for the polysaccharide based hydrogels with multiple crosslinks. In this study, we developed a ‘two-step’ strategy to activate synergistic effect of chemical and physical crosslinks using a poly (vinyl alcohol) (PVA)/bacterial cellulose (BC) hydrogel as a template. The BC nanofibers, on the one hand, acted as nucleating agents, participating in the crystallization of PVA, and on the other hand, were also involved in the formation of boronic ester bond, anchored with the PVA chains via chemical bonding. Therefore, the existence of BC nanofibers, as ‘bridge’, linked the crystalline regions and amorphous parts of PVA together, associating the two characteristic crosslinks, which was conducive to load transfer. The mechanical properties of resultant hydrogels, including the tensile elongation and strength, as well as fracture toughness, were significantly improved. Moreover, the dually cross-linked hydrogels possessed ionic conductivity, which was sensitive to the tensile deformation and environmental temperature. This study clarifies a unique role of BC nanofibers in hydrogels, and proposes an effective approach to construct multiple networks in the nanocellulose reinforced PVA hydrogels.

Open-system force-elongation relationship of collagen in chemo-mechanical equilibrium with water

A significant deformation mechanism of collagen at low loads is molecular uncoiling and rearrangement. Although the effect of hydration and cross-linking has been investigated at larger loads when collagen undergoes molecular sliding, their effects on collagen molecular reorganization remain unclear. Here we develop two thermodynamic models that use the notion of open-system elasticity to elucidate the effect of swelling due to water uptake during deformation of collagen networks under low and high cross-linking conditions. With low crosslinking, entropic contributions dominate resulting in rejection of solvent from the polymer network leading to reduced collagen stiffness with increased loads. Contrarily, high cross-linking inhibits initial coiling and structural kinking and the mechanical behavior is dominated by elastic energy. In this configuration, the solvent content depends on the sign of the applied load resulting in a non-linear open-system stress-strain relationship. The models provide insight on the parameters that impact the stress-strain relationships of hydrated collagen and can inform the way collagenous matrices are treated both in medical and laboratory settings.

Chitosan silver nanoparticle inspired seaweed (Gracilaria crassa) biodegradable films for seafood packaging

As an alternative to conventional plastic packaging, the concept of developing blend films with bio-based materials seems to be an environmentally friendly approach. In the present study, blend films were prepared using ethanolic extract of Gracilaria crassa (GCE) with chitosan (CS) and silver nanoparticles (AgNPs). The developed films were evaluated based on the physical, mechanical, structural, barrier and antioxidant indices. The films were slightly yellowish in color (b* ranges 39.69–53.08) and smooth textured. The FTIR spectra confirmed the intermolecular interaction between film components and the combination of CS and GCE occurred by means of -OH groups and hydrophobic interaction due to the cross-linking effect of the plasticizer (glycerol). The antioxidant properties of the films were investigated via DPPH assay and total phenolic contents showed significant improvement (p < 0.05) upon incorporation of GCE. Similar observations were made for tensile parameter (37.29 ± 1.22–38.39 ± 1.09) compared to the control (29.71 ± 1.66). The thermal pattern of blended films showed greater stability with Tg of 112.6 °C. The formulated films significantly extended the shelf-life of shrimp nuggets in refrigerated storage (4 °C) up to 9 days. The study reveals that the incorporation of GCE/AgNPs with chitosan films can be an active packaging system in the field of sustainable food packaging technology.

Transglutaminase-induced Cornea Collagen Crosslinking Effect on Central Corneal Thickness and Keratocyte Cell Density

Abstract&#x0D; Introduction &amp; Objectives : This research is aimed to evaluate the effect of transglutaminase-induced corneal collagen crosslinking (CXL) on central corneal thickness (CCT) and keratocyte cell density in vivo.&#x0D; Methods : Twenty-eight white New Zealand rabbits were divided into four groups: the transglutaminase- induced CXL group, the epithelial-off CXL group, the transepithelial CXL group, and the control group. The ocular surface was treated with a 1 U/mL microbial transglutaminase solution, and both the epithelial-off and transepithelial groups were exposed to clinical ultraviolet A-riboflavin (UVA/RF). The efficacy of each group was evaluated on the 14th day after the procedures. Central corneal thickness was evaluated with Corneal Visualization Scheimpflug Technology (Corvis ST) and keratocyte cell density wad evaluated with histopathology examination.&#x0D; Results : Transglutaminase-induced CXL group exhibited the highest mean biomechanical CCT (370.14 ± 38.85) in comparison to the UVA/RF epithelial-off group (368.00 ± 25.48), the UVA/RF transepithelial group (369.86 ± 23.43), and the control group (365.14 ± 28.74). Still, there was no significant differences in both biomechanical CCT (p=0.990). Transglutaminase-induced CXL group had the highest mean of keratocyte cell density (43.26 ± 10.65) compared to UVA/RF epithelial-off (29.99 ± 4.79), UVA/RF transepithelial group (42.03 ± 6.55), and control group (34.36 ± 6.76). There was a significant difference between the group, with a p-value of 0.008.&#x0D; Conclusion : Transglutaminase shown that it produces favorable results for CCT and keratocyte density after CXL, which are two factors contributing to corneal rigidity. The outcomes are equivalent to riboflavin used as a conventional element in CXL.

Effects of synthesis temperature on structures and properties of epoxidized soybean oil oligomers and starch‐based bioplastics

AbstractThe work investigated the synthesis of the oligomers with citric acid (CA) and epoxidized soybean oils (ESO) at various temperatures and the effects of the oligomers on the structures and properties of starch‐based bioplastics. CA was bonded effectively onto ESO via ring‐opening polymerization at 90°C as confirmed by the results of Fourier‐transform infrared spectroscopy, thermogravimetric analysis, and carboxylic group contents of CA‐ESO oligomers (CESO). The oligomers exhibited higher thermal stability than ESO. Regarding starch‐based bioplastics, CESO disrupted the hydrogen bonding interaction within starch molecules and formed the esterification reaction with starch. The bioplastics containing CESO exhibited remarkably higher structural homogeneity and opacity as the synthesis temperatures of CESO increased. However, the thermal properties of the bioplastics with various CESO reduced, which might be due to the decomposition of starch by CESO. The films containing CESO also exhibited lower tensile strength than the film with ESO, which might be related to the decomposition, crosslinking, and plasticization effects of CESO on starch. The bioplastics with CESO exhibited lower degradation due to a more intense interaction of CESO and starch. The study demonstrated the potential of CA as an interfacial linker of starch/ESO‐based bioplastics by adjusting the synthetic temperatures of CESO.

Effect of High Humidity Exposure to Wheat Starch Based High Conducting Flexible Polymer‐in‐Salt‐Electrolyte

AbstractPolymer‐in‐salt‐electrolytes (PISEs) are an important class of electrolytes as they carry the promise of faster and single ion transport. Unfortunately, due to unavailability of a suitable polymer host PISE has still not reached to commercial level. In the present work, using a novel synthesis protocol developed by the group, glutaraldehyde crosslinked wheat starch has been successfully modified with sodium iodide (NaI) to synthesize a flexible PISE membrane with desired electrochemical properties. Present paper reports the effect of crosslinker and exposure to high humidity ambience on electrochemical and morphological properties. It has been established that on exposure to higher humidity atmosphere starch‐based PISEs stabilize at lower resistance value, but with higher ion relaxation time, which indicates that effect of high humidity treatment is more on salt dissociation instead of assisting the ion transport. The studied materials have conductivity ≈0.01 S cm−1 range with ESW &gt;2.5 V, ensuring its usability in electrochemical devices. The developed synthesis protocol does not require any complicated synthesis route and/or sophisticated instrument hence the overall process is economical also, adding up to its potentiality for energy device fabrication.

Ultrastable, Superrobust, and Recyclable Supramolecular Polymer Networks

AbstractSupramolecular polymer networks (SPNs), crosslinked by noncovalent bonds, have emerged as reorganizable and recyclable polymeric materials with unique functionality. However, poor stability is an imperative challenge faced by SPNs, because SPNs are susceptible to heat, water, and/or solvents due to the dynamic and reversible nature of noncovalent bonds. Herein, the design of a noncovalent cooperative network (NCoN) to simultaneously stabilize and reinforce SPNs is reported, resulting in an ultrastable, superrobust, and recyclable SPN. The NCoN is constructed by multiplying the H‐bonding sites and tuning the conformation/geometry of the H‐bonding segment to optimize the multivalence cooperativity of H‐bonds. The rationally designed H‐bonding segment with high conformational compliance favors the formation of tightly packed H‐bond arrays comprising higher‐density and stronger H‐bonds. Consequently, the H‐bonded crosslinks in the NCoN display a covalent crosslinking effect but retain on‐demand dynamics and reversibility. The resultant ultrastable SPN not only displays remarkable resistance to heat up to 120 °C, water soaking, and a broad spectrum of solvents, but also possesses a superhigh true stress at break (1.1 GPa) and an ultrahigh toughness (406 MJ m−3). Despite the covalent‐network‐like stability, the SPN is recyclable through activating its reversibility in a high‐polarity solvent heated to a threshold temperature.

Ultrastable, Superrobust, and Recyclable Supramolecular Polymer Networks.

Supramolecular polymer networks (SPNs), crosslinked by noncovalent bonds, have emerged as reorganizable and recyclable polymeric materials with unique functionality. However, poor stability is an imperative challenge faced by SPNs, because SPNs are susceptible to heat, water, and/or solvents due to the dynamic and reversible nature of noncovalent bonds. Herein, the design of a noncovalent cooperative network (NCoN) to simultaneously stabilize and reinforce SPNs is reported, resulting in an ultrastable, superrobust, and recyclable SPN. The NCoN is constructed by multiplying the H-bonding sites and tuning the conformation/geometry of the H-bonding segment to optimize the multivalence cooperativity of H-bonds. The rationally designed H-bonding segment with high conformational compliance favors the formation of tightly packed H-bond arrays comprising higher-density and stronger H-bonds. Consequently, the H-bonded crosslinks in the NCoN display a covalent crosslinking effect but retain on-demand dynamics and reversibility. The resultant ultrastable SPN not only displays remarkable resistance to heat up to 120 °C, water soaking, and a broad spectrum of solvents, but also possesses a superhigh true stress at break (1.1 GPa) and an ultrahigh toughness (406 MJ m-3 ). Despite the covalent-network-like stability, the SPN is recyclable through activating its reversibility in a high-polarity solvent heated to a threshold temperature.