Quadruple Bond Research Articles

Antibacterial and antioxidant supramolecular nanocomposite hydrogel dressings with angiogenesis and photo-thermal effect for multidrug‐resistant bacterial infected wound healing

Antioxidant, antibacterial and removable supramolecular nanocomposite hydrogel dressings with self-healing and tissue adhesiveness is highly anticipated for bacterial infected skin wound healing. A series of supramolecular nanocomposite hydrogels via quadruple hydrogen bond and coordination bonds (catechol-Cu) was developed based on ureidopyrimidinone-modified poly(glycerol sebacate)–co-poly(ethylene glycol)-g-catechol (PEGSDU) and mesoporous copper sulfide nanoparticle (CuS NPs) as antioxidative, antibacterial, removable and tissue-adhesive dressing to treat the MRSA-infected wound. The hydrogels exhibited good self-healing, free radical scavenging, photothermal sterilization performance, adhesiveness, and temperature-sensitive removability. In addition, the Cu2+ was able to be slowly released from the hydrogel, which can promote the proliferation and migration of fibroblasts. Hydrogels containing CuS NPs showed better wound repair efficiency than commercial TegadermTM films and hydrogels without CuS NPs in MRSA-infected skin wound, which was attributed to the good antibacterial property, improved collagen deposition, reduced inflammatory response, and improved new vessels formation, thereby significantly promoting the repair of wounds. In summary, this antioxidative and antibacterial supramolecular nanocomposite hydrogel dressing provide a new type of multi-functional dressing for the treatment of infected skin wounds.

Ultratough Supramolecular Polyurethane Featuring an Interwoven Network with Recyclability, Ideal Self-Healing and Editable Shape Memory Properties.

Developing multifunctional polymers with excellent mechanical properties, outstanding shape memory characteristics, and good self-healing properties is a formidable challenge. Inspired by the woven cross-linking strategy, a series of supramolecular polyurethane (PU) with an interwoven network structure composed of covalent and supramolecular cross-linking nodes have been successfully synthesized by introducing the ureido-pyrimidinone (UPy) motifs into the PU skeleton. The best-performing sample exhibited ultrahigh strength (∼77.2 MPa) and toughness (∼312.7 MJ m-3), along with an ideal self-healing efficiency (up to 90.8% for 6 h) and satisfactory temperature-responsive shape memory effect (shape recovery rates up to 96.9%). Furthermore, it ensured recyclability. These favorable properties are mainly ascribed to the effective dissipation of strain energy due to the disassembly and reconfiguration of supramolecular nodes (i.e., quadruple hydrogen bonds (H-bonds) between UPy units), as well as the covalent cross-linking nodes that maintain the integrity of the polymer network structure. Thus, our work provides a universal strategy that breaks through the traditional contradictions and paves the way for the commercialization of high-performance multifunctional PU elastomers.

Measuring the Magnetic Anisotropy of Metal-Metal Multiple Bonds: The Importance of Correcting for Ligand Effects.

We describe the synthesis and characterization of the quadruply-bonded dimer Mo2(CH2NMe2BH3)4 in which each molybdenum(II) center is bound to two chelating boranatodimethylaminomethyl (BDAM) ligands. The BDAM anions bind to the metal at one end by a metal-carbon σ bond and at the other by a three-center M-H-B interaction. Each BDAM ligand chelates to a single Mo atom so that the metal-metal bond is unbridged; the Mo-Mo distance is 2.114(2) Å. Structural and solution NMR data, analyzed via McConnell's equation and supported by DFT calculations, show that the magnetic anisotropies associated with highly polarizable and π-bonding ligands (such as chloride groups and aryl rings) can greatly affect the NMR chemical shifts of reporter groups, so that ignoring their contributions leads to significant overestimates of the anisotropy due just to the metal-metal bond. We propose a method to quantify and correct for the magnetic anisotropy effects arising from the ligands. Application of this method to Mo2(BDAM)4 indicates that the magnetic anisotropy of the Mo-Mo quadruple bond in this molecule is about -800 × 10-36 m3 molecule-1. Anisotropies significantly higher than this value (as sometimes reported in the prior literature) are most likely incorrect.

By Introducing Multiple Hydrogen Bonds Endows MOF Electrodes with an Enhanced Structural Stability.

Recently, metal-organic frameworks (MOFs) have attracted great interest in energy storage areas. However, the poor structural stability of MOFs derived from weak coordination bonds limits their applications. Here, quadruple hydrogen bonds (H-bonds) were introduced onto the MOFs to enhance their structural stability. Cross-linked networks could be formed between molecules owing to multiple H-bonds, strengthening the framework stability. Moreover, the dynamic reversibility of H-bonds could endow MOFs with self-healing ability. Furthermore, due to lower binding energy compared to coordination bonds, H-bonds break preferentially when subjected to internal stress, thus protecting the MOFs. Consequently, the as-prepared self-healing hybrid (SHH-Cu-MOF@Ti3C2TX) exhibited high capacitance retention (89.4%) after 5000 cycles at 1 A g-1, while that hybrid without dynamic H-bonds (H-Cu-MOF@Ti3C2TX) presented a 79.9% retention, delivering an enhancement in cycling stability. Moreover, an asymmetric supercapacitor (ASC) was fabricated by employing SHH-Cu-MOF@Ti3C2TX and activated carbon (AC) as the electrodes. The ASC delivered a specific capacitance (47.4 F g-1 at 1 A g-1), an energy density (16.9 Wh kg-1), and a power density (800 W kg-1) as well as good rate ability (retains 81% of its initial capacitance from 0.2 A g-1 to 5 A g-1).

Degradable, self-healing, humidity-driven poly(urethane-urea) film

Humidity-driven materials are widely used in actuators, soft robots, sensors, and other fields. The extensive use of these materials increases the demand for degradable, highly durable, and self-healing materials. However, the preparation of such ideal materials still faces serious challenges. Herein, a novel poly(urethane-urea) film material (PUU-DHA-Cu4) with synergetic quadruple dynamic bonds (acylhydrazone bonds, boron-oxygen bonds, coordination bonds, and hydrogen bonds) is developed. The prepared PUU-DHA-Cu4 film material exhibited a tensile strength of 23.2 MPa, an elongation at break of 1142 %, and a healing efficiency of 90.1 % after 48 h of self-healing at room temperature. Meanwhile, the reversibility of the boron-oxygen bond imparts degradability to the material. Finally, a humidity-driven poly(urethane-urea) material that not only has self-healing ability but can also be degraded easily was successfully developed. This work will make a valuable addition to the field of environment-friendly humidity-driven materials.

Quadruple bonds in MoC: Accurate calculations and precise measurement of the dissociation energy of low-lying states of MoC.

In the present work, the electronic structure and chemical bonding of the MoC X3Σ- ground state and the six lowest excited states, A3Δ, a1Γ, b5Σ-, c1Δ, d1Σ+, and e5Π, have been investigated in detail using multireference configuration interaction methods and basis sets, including relativistic effective core potentials. In addition, scalar relativistic effects have been considered in the second order Douglas-Kroll-Hess approximation, while spin-orbit coupling has also been calculated. Five of the investigated states, X3Σ-, A3Δ, a1Γ, c1Δ, and d1Σ+, present quadruple σ2σ2π2π2 bonds. Experimentally, the predissociation threshold of MoC was measured using resonant two-photon ionization spectroscopy, allowing for a precise measurement of the dissociation energy of the ground state. Theoretically, the complete basis set limit of the calculated dissociation energy with respect to the atomic ground state products, including corrections for scalar relativistic effects, De(D0), is computed as 5.13(5.06) eV, in excellent agreement with our measured value of D0(MoC) of 5.136(5) eV. Furthermore, the calculated dissociation energies of the states having quadruple bonds with respect to their adiabatic atomic products range from 6.22 to 7.23eV. The excited electronic states A3Δ2 and c1Δ2 are calculated to lie at 3899 and 8057 cm-1, also in excellent agreement with the experimental values of DaBell et al., 4002.5 and 7834 cm-1, respectively.

Stretchable interconnected modular electrochromic devices enabled by self-healing, self-adhesive, and ion-conducting polymer electrolyte

Here, we propose a versatile terpolymer electrolyte material, UPy-PEGMA-VBMI, comprised of three monomers: ureidopyrimidinone methacrylate (UPyMA), poly(ethylene glycol) methacrylate (PEGMA), and vinyl benzyl-methylimidazolium (VBMI). The UPy-PEGMA-VBMI, supported by a combination of soft ethylene glycol chains, an ion-conducting imidazole unit, and self-complementary quadruple hydrogen bonds of UPy, exhibits exceptional properties such as high stretchability, rapid self-repair, solution processability, self-adhesion, and ion conduction. The UPy-PEGMA-VBMI was then applied to make ion gel composite films, demonstrating a notable ionic conductivity of 3.84 × 10−3 S cm−1 while maintaining robust stretching and adhesive characteristics. The electrochromic devices (ECDs) fabricated by this ion gel demonstrate outstanding performance, with fast switching times, long-term kinetic stability, and extraordinarily high coloration efficiency of 443.83 cm2 C−1. The stretchable ECDs are fabricated by utilizing the stretchable nature of UPy-PEGMA-VBMI, exhibiting a transmittance contrast of 42.7 % at an extension of 53 % and operational stability during stretching cycles. Moreover, self-healing and self-adhesive features enable the fabrication of interconnected modular ECDs, implementing area-scalable devices. These modular ECDs, each powered independently, provide arbitrary positioning and shifting of individual device patches, overcoming the performance limitations of conventional large-area devices. The unprecedented material and resulting devices open new possibilities for electrochromic applications, particularly in stretchable ECDs, pattern-switching devices, and scalable flexible ECDs.

Highly adhesive and impact‐strengthening supramolecular polyurethane derived from facile incorporation of UPy motifs toward energy dissipation binding applications

AbstractThe implementation of hot melt adhesives reaching structural adhesion with both impact resistance and detachability is of prospective industry value but still remains challenging. In this work, 2‐amino‐4‐hydroxy‐6‐methylpyrimidine serving as both chain extender and end‐capping reagent due to its isomerism, was developed to construct a supramolecular polyurethane‐derived hot melt structural adhesive. The as‐synthesized PUM elastomers occurs obvious decrease of molecular weight at 80°C compared to room temperature, revealing the existence of self‐complementary 2‐ureido‐4[1H]‐pyrimidinone (UPy) motifs at chain ends. This unique structure allows to chemically incorporate abundant hierarchical and quadruple hydrogen bonding moieties, which results in remarkable enhancement of shear strength, ranging from 6.4 to 16.6 MPa. More importantly, it also exhibits unique impact‐strengthening and reproducible adhering ability. The Hopkinson‐press‐bar and cyclic tensile tests manifest that quadruple hydrogen bonds play a pivotal role in buffering external forces and increasing energy dissipation when exposed to high velocity impacts. The true stress and strain synchronously increase as the strain rate augments while the shear strength can even roar up to ~18 MPa at high tensile speed. With regard to mild synthetic conditions, atomic economic use of reactants, it is promising that this material has industrial potential to be utilized in applications referred to energy‐absorption and reproducible structural adhesion.

Verification of the Self-Healing Ability of PP-co-HUPy Copolymers in Epoxy Systems.

This work concerns the verification of the self-healing ability of PP-co-HUPy copolymers dispersed in epoxy systems. PP is the acronym for the Poly-PEGMA polymer, and HUPy refers to the HEMA-UPy copolymers based on ureidopyrimidinone (UPy) moieties. In particular, this work aims to verify whether this elastomer characterized by an intrinsic self-healing ability can activate supramolecular interactions among polymer chains of an epoxy resin, as in the elastomer alone. The elastomer includes a class of polyethylene glycol monomethyl ether methacrylate-based copolymers, with different percentages of urea-N-2-amino-4-hydroxy-6-methyl pyrimidine-N'-(hexamethylene-n-carboxyethyl methacrylate) (HEMA-UPy) co-monomers. The self-healing capability of these copolymers based on possible quadruple hydrogen bond interactions between polymer chains has been verified. The formulated epoxy samples did not show self-healing efficiency. This can be attributed to the formation of phase segregation that originates during the curing process of the samples, although the PP-co-HUPy copolymers are completely soluble in the liquid epoxy matrix EP. The morphological investigation highlighted the presence of crystals of PP-co-HUPy copolymers, which are in greater quantity in the sample containing the highest weight percentage (7.8 wt%) of HUPy units. Furthermore, the crystals act as promotors for increasing the curing degree (DC) of the epoxy systems containing HUPy units. DC goes from 91.6% for EP to 96.1% and 95.4% for the samples containing weight percentages of 2.5 and 7.8 wt% of HUPy units, respectively. Dynamic mechanical analysis (DMA) shows storage modulus values for epoxy systems containing PP-co-HUPy units lower than that of the unfilled resin EP. The values of maximum in Tan δ (Tg), representing the temperature at which the glass transition occurs, are 220 for the unfilled resin EP, 228 for the sample containing 2.5 wt% of HEMA-UPy units, and 211 for the sample containing 7.8 wt% of HEMA-UPy units.

BeM(CO)3- (M = Co, Rh, Ir) and BeM(CO)3 (M = Ni, Pd, Pt): Triply bonded terminal beryllium in zero oxidation state.

We perform detailed potential energy surface explorations of BeM(CO)3- (M = Co, Rh, Ir) and BeM(CO)3 (M = Ni, Pd, Pt) using both single-reference and multireference-based methods. The present results at the CASPT2(12,12)/def2-QZVPD//M06-D3/def2-TZVPPD level reveal that the global minimum of BeM(CO)3- (M = Co, Rh, Ir) and BePt(CO)3 is a C3v symmetric structure with an 1A1 electronic state, where Be is located in a terminal position bonded to M along the center axis. For other cases, the C3v symmetric structure is a low-lying local minimum. Although the present complexes are isoelectronic with the recently reported BFe(CO)3- complex having a B-Fe quadruple bond, radial orbital-energy slope (ROS) analysis reveals that the highest occupied molecular orbital (HOMO) in the title complexes is slightly antibonding in nature, which bars a quadruple bonding assignment. Similar weak antibonding nature of HOMO in the previously reported BeM(CO)4 (M = Ru, Os) complexes is also noted in ROS analysis. The bonding analysis through energy decomposition analysis in combination with the natural orbital for chemical valence shows that the bonding between Be and M(CO)3q (q = -1 for M = Co, Rh, Ir and q = 0 for M = Ni, Pd, Pt) can be best described as Be in the ground state (1S) interacting with M(CO)30/- via dative bonds. The Be(spσ) → M(CO)3q σ-donation and the complementary Be(spσ) ← M(CO)3q σ-back donation make the overall σ bond, which is accompanied by two weak Be(pπ) ← M(CO)3q π-bonds. These complexes represent triply bonded terminal beryllium in an unusual zero oxidation state.

Stability of Ti3C2-MXene/Waterborne polyurethane composite emulsion and investigation of visible light-driven film self-healing performance

Intrinsic self-healing waterborne polyurethane (WPU) is an environmentally friendly, economically viable, and practical novel intelligent material. However, the key to achieving practical applications lies in the remote activation of repair in self-healing materials and the excellent mechanical properties of the matrix. In this study, we introduce quadruple hydrogen bonding in the polyurethane backbone. We have incorporated a novel two-dimensional sheet-like material, MXene, to achieve visible light remote-driven self-healing of material hydrogen bonds while enhancing the material’s mechanical properties. By utilizing the MXene supernatant, this approach not only resolves the issues of poor stability and easy sedimentation of MXene nanosheets in water-based polymers but also helps to prevent resource wastage. Our research results demonstrate that the composite film exhibits a tensile strength of 6.55 MPa and a fracture elongation of 604%. Additionally, quadruple hydrogen bonds in the WPU chains enable rapid self-healing of microcracks under visible light irradiation at 300 mW/cm2, with complete disappearance within 80 min.

Ionic liquid-based self-healing gel electrolyte for high-performance lithium metal batteries

The gel electrolytes with self-healing function are being considered as promising replacement for traditional liquid electrolytes in lithium metal batteries due to their excellent battery safety, high energy density and minimum electrolyte damage. However, balancing self-healing, conductivity and mechanical properties remains a challenge for their practical application. Herein, a new ion liquid-based self-healing gel polymer electrolyte (IL-SHGPE) is introduced. The electrolyte was synthesized via UV-induced cross-linking of a polymer containing quadruple hydrogen bond units and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (BMIM-TFSI) ion liquid. The resultant IL-SHGPE demonstrates exceptional self-healing ability (with 95% healing efficiency within 30 min), excellent thermal stability over a wide temperature range up to 410 °C. It also exhibits impressive mechanical strength with 41.3% elongation and 1.9 MPa tensile stress, room temperature ionic conductivity of 1.29 × 10−3 S/cm, and a wide electrochemical stability window of 5.18V (vs Li/Li+). Lithium metal batteries with this electrolyte showed an initial discharge capacity of 139 mAh g−1 at 1C rate, and a capacity retention of 88.3% after 200 cycles. Therefore, this work provides a significant exploration for balancing self-healing ability, mechanical attributes, and electrochemical performance of lithium batteries, and thus contributing valuable insights towards the development of high-performance self-healing gel electrolytes for lithium metal batteries.

A room‐temperature self‐healing anticorrosion coating of supramolecular polyurethane based on dynamic reversible quadruple hydrogen bond

AbstractThe contradiction between the migration rate of molecular chains and mechanical strength has always been a key factor affecting the practical application of self‐healing anticorrosion coatings. In this paper, a series of supramolecular self‐healing elastomers (SPU‐MP) were prepared by the reaction of diphenylmethane diisocyanate and polyether amine. The results shown that the proportion of polyetheramine D230 (D230) in molecular segments affects the hydrogen bond density between molecular chains, thereby affecting the self‐healing efficiency and mechanical strength of SPU‐MP. When the ratio of D230 and polyetheramine D400 (D400) is 2:8, the tensile fracture strength of SPU‐MP8 is 5.08 MPa, and the self‐healing efficiency reaches 82.1% after 10 h of repair at room temperature. Further increasing the ratio of D230 increases the relaxation time of the molecular chain due to the increase in hydrogen bond density, resulting in a decrease in the self‐healing efficiency of SPU‐MP. The results of electrochemical experiments and neutral salt spray experiments indicate that the anticorrosion coating prepared by SPU‐MP8 exhibits good self‐healing performance. After immersing in 3.5 wt.% NaCl solution for 35 days, the low‐frequency impedance modulus of the intact coating and the scratch coating were both higher than 107 Ω cm2, still shown good anticorrosion ability.

The quadruple bond – 60 years – a tribute to F. Albert Cotton and other pioneers

The quadruple bond – 60 years – a tribute to F. Albert Cotton and other pioneers

NIR photoresponsive shape memory polyurethanes composite with self-healing and anti-corrosion properties

The self-healing ability of organic coatings is crucial for restoring protective functions and achieving long-lasting corrosion protection in the case of coating defects. This article prepares a shape memory-assisted self-healing polyurethane composite with the dual response of light and heat (SMPUx-Uy@CS). The shape memory performance of the material is controlled by adjusting the addition ratio of polyether glycol with different molecular weights. The introduction of reversible quadruple hydrogen bonds (UPy) further enhances the microphase separation of the system, endowing the material with excellent mechanical properties and self-healing ability. Carbon nanospheres (CS) are added to produce a photothermal conversion effect under near-infrared (NIR) irradiation. On the one hand, it can achieve precise repair, and on the other hand, it can improve corrosion resistance. When PTMG-1000:PTMG-250 = 4:1, SMPU3-U30@CS-0.5 with 30% UPy and 0.5 wt% CS has the best comprehensive performance, with a tensile strength of 8.42 MPa and an elongation at a break of 194.91%. The surface scratches of the composite coating can be healed after 60 s under 3 W/cm2 NIR irradiation. Magnesium alloy with SMPU3-U30@CS-0.5 coating has a corrosion potential of −1.34 V and corrosion current density of 5.37 × 10−9 A cm−2, and the damaged coating recovers well in corrosion resistance after 300 s of NIR irradiation. Thanks to the maze effect and hydrophobic performance, the addition of CS is beneficial for improving the anti-corrosion performance of the coating. The experimental results indicate that the repair efficiency of NIR is much higher than that of thermal repair, making it more green, environmentally friendly, and sustainable. This article provides a straightforward, green synthesis strategy for constructing self-healing coatings with efficient corrosion resistance.

Photocatalytic Multicomponent Annulation of Amide-Anchored 1,7-Diynes Enabled by Deconstruction of Bromotrichloromethane.

We present the first example of visible-light-mediated multicomponent annulation of 1,7-diynes by taking advantage of quadruple cleavage olf carbon-halogen bonds of BrCCl3 to generate a C1 synthon, which was adeptly applied to the preparation of skeletally diverse 3-benzoyl-quinolin-2(1H)-one acetates in moderate to good yields. Controlled experiments demonstrated that H2O acted as both oxygen and hydrogen sources, and gem-dichlorovinyl carbonyl compound exhibited as a critical intermediate in this process. The mechanistic pathway involves Kharasch-type addition/6-exo-dig cyclization/1,5-(SN")-substitution/elimination/binucleophilic 1,6-addition/proton transfer/tautomerization sequence.

Shifting the mechanical strength-healing efficiency trade-off of polyurethanes by incorporating boronic ester bonds and hydrogen bonding

It is challenging to design and synthesize elastomers with both good mechanical performance and high healing efficiency because their mechanisms are mutually exclusive. This work aims to shift the trade-off between them by incorporating dynamic non-covalent bonds via 2-ureido-4[1H]-pyrimidione (UPy) and dynamic covalent bonds via boronic ester bonds into polyurethane. The quadruple hydrogen bonds between UPy dimers serve as physical crosslinks, improving the overall mechanical properties of the polyurethane, while the boronic esters facilitate its healing. The resulting polyurethane can achieve an ultimate stress of 27.4 MPa and a healing efficiency of 90 %. The effect of healing time on the healing efficiency is modeled and discussed.

High-Toughness CO2-Sourced Ionic Polyurea Adhesives.

Polyurea (PUa) adhesives are renowned for their exceptional adhesion to diverse substrates even in harsh environments. However, the presence of quadruple bidentate intermolecular hydrogen bonds in the polymer chains creates a trade-off between cohesive energy and interfacial adhesive energy. To overcome this challenge, a series of CO2-sourced ionic PUa adhesives with ultratough adhesion to various substrates are developed. The incorporated ionic segments within the adhesive serve to partially mitigate the intermolecular hydrogen bonding interactions while conferring unique electrostatic interactions, leading to both high cohesive energy and interfacial adhesive energy. The maximum adhesive strength of 10.9MPa can be attained by ionizing the CO2-sourced PUa using bromopropane and subsequently exchanging the anion with lithium bis(trifluoromethylsulfonyl)imide. Additionally, these ionic PUa adhesives demonstrate several desirable properties such as low-temperature stability (-80°C), resistance to organic solvents and water, high flame retardancy, antibacterial activity, and UV-fluorescence, thereby expanding their potential applications. This study presents a general and effective approach for designing high-strength adhesives suitable for a wide array of uses.

A self-healing waterborne acrylic latex coating based on intrinsic hydrogen bonding

Acrylic coatings suffer damage in the form of cracking, which degrades both their protective and aesthetic performance over time. Self-healing technology offers the ability to solve this problem by allowing cracks to spontaneously heal without external diagnosis or intervention, offsetting the enormous costs associated with coating damage and repair. However, there is currently no efficient self-healing acrylic coating design, and research in the area remains noticeably sparse. In this research we sought to imbue a mechanically tough methyl methacrylate (MMA)/butyl acrylate (BA)/acrylic acid (AA) acrylic coating with self-healing functionality by incorporating self-healing monomers within the formulation. We synthesized a library of four acrylic monomers containing both a long amphiphilic spacer of variable length, and the 2-ureido-4[1H]-pyrimidinone (UPy) unit, which forms strong self-complementary quadruple hydrogen bonds. These UPy-monomers were able to participate in the emulsion polymerization of MMA, BA and AA, forming intrinsic hydrogen bonding networks within the subsequent acrylic coatings. These UPy functionalized coatings displayed optical self-healing and strain recovery over 24 h both at room temperature (∼28 %), and at elevated temperatures up to 50 °C (∼80 %). The coatings also displayed repeatable self-healing after four healing cycles, relative to an MMA/BA/AA coating.

Tough and Self-Healing Waterborne Polyurethane Elastomers via Dynamic Hydrogen Bonds Design for Flexible Conductive Substrate Applications.

Balancing the mechanical strength and self-healing performance of polyurethane (PU) remains a significant challenge in achieving excellent self-repairing PU materials. In this study, a self-healing waterborne PU elastomer was designed from a bionic concept by incorporating 2'-deoxythymidine (2'-dT) and isophorone diamine (IPDA) into the polymer chain. The loose stacking of IPDA's irregular cycloaliphatic structure resulted in the irregular arrangement of urethane bonds in the hard domain. The formation of sextuple hydrogen bonds between 2'-dT and urethane bonds, as well as quadruple hydrogen bonds between urethane bonds themselves, enhanced the mechanical properties of the material. The multiple hydrogen bonds can dissociate, recombine, and dissipate energy, thereby improving the material's repair capability. The hierarchical self-assembly of hydrogen bonds enabled the PU to achieve a tensile strength of 15.3 MPa and toughness of 100.75 MJ/m3. The prepared PU film is highly transparent and has a transmittance of more than 90%. Additionally, it can undergo rapid repair under high temperatures or under trace solvent conditions. When used as a flexible conductive substrate, it quickly restored the conductivity and enhanced the material's lifespan after surface damage. This environmentally friendly and self-healing waterborne PU elastomer will hold broad application prospects in the field of flexible electronic devices.