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covalent bonds
CHEMISTRY OF MATERIALS · 2018 · IF 9.89

High-Performance Double-Network Ion Gels with Fast Thermal Healing Capability via Dynamic Covalent Bonds

Zhehao Tang,Xiaolin Lyu,Anqi Xiao,Zhihao Shen,Xinghe Fan

A tough double-network (DN) ion gel composed of chemically cross-linked poly(furfuryl methacrylate-co-methyl methacrylate) (P(FMA-co-MMA)) and physically cross-linked poly(vinylidene fluoride-co-hexafluoropropylene) (P(VDF-co-HFP)) networks with 80 wt % of ionic liquid (IL) was fabricated via a one-pot method. This ion gel exhibits excellent mechanical strength and considerable ionic conductivity, which can be used as a solid gel electrolyte. Upon an adjustment of the weight ratio of P(FMA-co-MMA) to P(VDF-co-HFP) and the content of the cross-linker, remarkably robust DN ion gel (failure tensile stress 660 kPa, strain 268%; failure compressive stress 17 MPa, strain 85%) was obtained. The high mechanical strength is attributed to the chemical/physical interpenetrating networks. The rigid chemically cross-linked P(FMA-co-MMA) network dissipates most of the loading energy, and the ductile physically cross-linked P(VDF-co-HFP) network provides stretchability for the whole gel. More importantly, the P(FMA-co-MMA) network is formed by dynamic covalent bonds that can undergo a thermally reversible reaction, giving the gel a unique and effective thermal healing capability. Furthermore, with the high content of IL, the DN ion gel possesses a high ionic conductivity of 3.3 mS cm–1 at room temperature, which is higher than those of most solid polymer electrolytes and comparable to those of commercial organic liquid electrolytes.

CAS / MDL: 74-96-4 98-00-0
研究领域: 材料科学 · 化学工程
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Journal of Energy Storage · 2023 · IF 9.4

Fused heteroaromatic benzothiazoles functionalized nitrogen-doped graphene by non-covalent bonds for high-performance supercapacitors

Shixing Chao,Danqin Li,Weiqiang Zhou,Yanmei Liang,Yao He,Jingkun Xu,Peipei Liu

Benzothiazole (Bz) molecules with excellent electrochemical stability and activity are favor of enhancing the capacitance performance of N-doped graphene (NG) by non-covalent functionalization. Herein, Bz molecules with different substituent groups (-ketone, -methoxy, -ketone and-methoxy) are used to functionalize NG nanosheets by a hydrothermal method and freeze-drying procedure. The surface chemistry and structure of as-prepared functionalized NG nanosheets are investigated through UV − vis, FTIR, SEM, AFM, XPS, TGA, XRD, Raman and BET. The electrochemical results of four functionalized NG nanosheets show that the substituent groups on Bz molecules have a great influence on their capacitive properties, among which the NG modified by the 6-methoxy benzothiazol-2-ketone (1-MhzNG) demonstrates the highest specific capacitance (420 F g −1 at 1 A g −1 ) and excellent cycle stability of 95.7 % after 10,000 cycles. In addition, the assembled supercapacitor based on the 1-MhzNG electrode delivers the highest energy density of 22.5 Wh kg −1 at 809 W kg −1 . Our work provides a new idea to modify graphene with novel organic small molecules for high-performance SCs.

研究领域: 材料科学 · 电化学
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CHINESE JOURNAL OF POLYMER SCIENCE · 2025 · IF 4

Preparation and Properties Study of Itaconic Acid-based Degradable Epoxy Resin Based on Dynamic Covalent Bonds

Liu He-Chen,Zhou Xin-Xin,Zhou Song-Song,Zou Ying,Wang Yu-Li,Li Xiang-Qing

The most widely used bisphenol A-type epoxy resin (DGEBA) in electrical engineering demonstrates excellent mechanical and electrical properties. However, the insoluble and infusible characteristics of cured DGEBA make it difficult to efficiently degrade and recycle decommissioned electrical equipment. In this study, a degradable itaconic acid-based epoxy resin incorporating dynamic covalent bonds was prepared through the integration of ester bonds and disulfide bonds, with itaconic acid as the precursor. The covalent bonding effects on the mechanical, thermal, electrical, and degradation characteristics were systematically evaluated. The experimental results revealed that the introduction of dynamic ester bonds enhanced the mechanical properties and thermal stability of the resin system, achieving a flexural strength of 141.57 MPa and an initial decomposition temperature T 5% of up to 344.9 °C. The resin system containing dynamic disulfide bonds exhibited a dielectric breakdown strength of 41.11 kV/mm. Simultaneously, the incorporation of disulfide bonds endowed the epoxy resin with remarkable degradability, enabling complete dissolution within 1.5 h at 90 °C in a mixed solution of dithiothreitol (DTT) and N -methylpyrrolidone (NMP). This research provides a valuable reference for the application of itaconic acid-based vitrimer with dynamic covalent bonds in electrical materials, contributing to the development and utilization of environmentally friendly electrical equipment.

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Journal of Materials Chemistry C · 2020 ·Vol. 8 ·期 15 ·5280-5292 · IF 7.059

A healable waterborne polyurethane synergistically cross-linked by hydrogen bonds and covalent bonds for composite conductors

Yan Yang,Zushan Ye,Xiaoxuan Liu,Jiahui Su

Elastomer materials integrated with high mechanical strength and excellent self-healing ability can be used as substrates in electronic skins, soft robots, and electrical devices. However, simultaneously enhancing the mechanical and self-healing properties of elastomers is still a great challenge because the self-healing ability of polymer materials is usually antagonistic to its mechanical strength. Herein, a novel healable polyurethane elastomer was developed using a double-network (DN) structure system. In the DN system, a loosely cross-linked chemical network was obtained via a photo-curable acrylic double bond, acting as a robust molecular framework and maintaining the elasticity of the polymer. Simultaneously, the physical cross-linked network produced by quadruple H-bonds of ureidopyrimidinone (UPy) units can not only achieve rapid reformation after fracture but also dissipate strain energy as a weak dynamic bond, endowing the elastomer with excellent self-healing ability and high stretchability. Owing to the accurate design, the synthesized elastomer exhibits excellent properties, including high tensile stress (13.71 MPa), high stretchability (∼500%), exceptional resilience and self-healing ability (90%). The robust healable elastomer enables the easy fabrication of composite conductors, which the prominent performance suggests as a great potential of the healable flexible sensor in next-generation wearable stretchable electronic devices, soft robots, and strain sensors.

研究领域: 材料科学 · 电子皮肤 · 软体机器人 · 可穿戴设备
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JOURNAL OF APPLIED POLYMER SCIENCE · 2020 ·Vol. 137 ·期 41 ·49250 · IF 2.52

Aminoglycoside hydrogels based on dynamic covalent bonds with pH sensitivity, biocompatibility, self-healing, and antibacterial ability

Ya Li,Cui Cheng,Xiaoran Gao,Siyuan Wang,Hanhui Ye,Xiao Han

Despite aminoglycosides (AGs) have superior antibacterial ability, all approved AGs by FDA are associated with adverse effects such as ototoxicity and nephrotoxicity. To solve these problems, AGs hydrogels based on dynamic covalent bond cross-linking were quickly prepared within 25 s by using AGs, aldehyde hyaluronic acid (A-HA), and adipic acid dihydrazide graft hyaluronic acid (HA-ADH) as materials. FT-IR, thermal analysis, and SEM results exhibited that A-HA/HA-ADH/AGs hydrogels were successfully synthesized with highly porous and interconnected network structure. The water absorption ratio of the hydrogels increased with the decreasing pH and temperature, indicating the hydrogels were pH- and temp-responsive. The pH-dependent degradation also demonstrated pH sensitivity of the hydrogels. Rheology and self-healing analysis assessment displayed that AGs hydrogels had good mechanical property, self-healing ability, and injectability. The hydrogels had no cytotoxicity to L929 cells and their hemolysis ratios were between 0.7% and 1.3%, which reached a nontoxic level. Most importantly, inhibition zones results demonstrated that the hydrogels had excellent and sustained antibacterial performance against Escherichia coli and Staphylococcus aureus . Therefore, A-HA/HA-ADH/AGs hydrogels are potential dressings for wound healing. Further plans including antibacterial and in vivo wound healing assays will be shown in the next work.

研究领域: 材料科学 · 药剂学 · 生物材料 · 生物医学工程
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MACROMOLECULAR CHEMISTRY AND PHYSICS · 2022 ·Vol. 224 ·期 2 ·2200322 · IF 2.996

Sustainable Polyurethane Networks with High Self-Healing and Mechanical Properties Based on Dual Dynamic Covalent Bonds

Yanning Zeng,Jiawei Li,Chaoying Hu,Bin Yang,Zhao Ning

Hydroxy-terminated polybutadiene (HTPB) based polyurethanes (PU) networks are broadly applied in industry and aviation, however, their nonrecyclability leads to the waste of petroleum. In this work, a series of novel self-healing, weldable, and recyclable HTPB-based PU networks with dual reversible covalent bonds are fabricated by one-pot polycondensation. To shorten the relaxation time, dual reversible covalent bonds (disulfide bonds and boronic ester bonds) are incorporated into the HTPB-based PU networks. Meanwhile, to promote tensile strength, the rigid isocyanate and cross-link agent are introduced into the networks. Obtained HTPB-based PU network structures are characterized by FTIR, Raman, and DMA measurements. Obtained HHMB-4-20 network shows the best mechanical properties (tensile strength = 6.97 MPa, elongation at break = 302 %), and the mechanical properties almost can be recovered after welding/reprocessing by hot pressing. To satisfy the demands of industrial sustainability, the synthesis of PU networks with capabilities of reprocessing, self-healing, and welding is a feasible approach.

研究领域: 材料科学 · 聚合物化学 · 可持续工程
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JOURNAL OF POLYMER SCIENCE · 2023 ·Vol. 61 ·期 15 ·1675-1687 · IF 3.4

Tough, self-healing double network hydrogels crosslinked via multiple dynamic non-covalent bonds for strain sensor

Guohui Huang,Pei Wang,Yutian Cai,Kun Jiang,Huimin Li

Double-network hydrogels have outstanding mechanical characteristics but mostly suffer from poor self-healing performance since most hydrogels are chemically crosslinked via covalent links for each network. In this work, a tough and self-healing double network hydrogel with multiple dynamic non-covalent bonds is developed by combining the hydrophobically modified polyacrylamide (HPAM) with a thermally reversible potassium ion crosslinked κ -carrageenan (K + C) network through a dual physical crosslinked network strategy. Being the multiple dynamic non-covalent bond interactions and dual physical crosslink networks, the K + C/HPAM DN hydrogel exhibits excellent mechanical characteristics (tensile strength: 1.86 MPa, tensile strain: 1637%) and good self-healing ability (maximum stress self-healing efficiency: 87%, maximum tensile strength after self-healing: 0.95 MPa). Due to the three-dimensional pore structure and the conductive ions in the system, the K + C/HPAM DN hydrogel also achieves good strain sensing capabilities with a strain sensitivity of 2.98 (gauge factor, GF) in the 100% strain range. Even after being cut and self-healed, the gel still exhibits good strain sensing capabilities (GF = 2.79), which is still better than the most similar DN hydrogel strain sensors in sensitivity. We believe this work offers a new material for self-healing flexible strain sensors. Graphical

CAS / MDL: 79-06-1
研究领域: 材料科学 · 纳米技术 · 生物医学工程 · 传感器
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PROGRESS IN ORGANIC COATINGS · 2023 · IF 6.6

Thermal-driven self-healing and green recyclable waterborne polyurethane films based on double reversible covalent bonds

Futao Sai,Haitao Zhang,Jianbo Qu,Jianyong Wang,Xiuzhong Zhu,Peng Ye,Zhiliang Zhang

Recently, the self-healing and recyclability of waterborne polyurethane (WPU) has attracted significant research attention. Herein, different weight ratios of Diels-Alder (DA) diol and diacetyl oxime (DMG) were used as the reactive monomer with polytetramethylene ether glycol (PTMG), isophorone diisocyanate (IPDI) and dimethylolpropionic acid (DMPA). A series of thermal-driven self-healing and green recyclable waterborne polyurethane films (WPU-DMG x -DA y ) were prepared based on synergistic dynamic reactions of oxime-carbamate and DA bonds. We investigated the properties of WPU-DMG x -DA y emulsions by particle size and zeta potential tests, and the results show that these emulsions have excellent storage stability. The self-healing properties of WPU-DMG x -DA y films were identified by dynamic mechanical analysis . It was revealed that the WPU-DMG 4 -DA 4 film has the best self-healing capability, and the self-healing efficiency can reach 92. ± 0.1 % after self-healing at 120 °C for 4 h. The mechanism of the self-healing behavior was studied by Fourier transform infrared spectroscopy , and the effective reversibility of the oxime-carbamate and DA bonds were verified. In addition, thermal gravimetric analysis and tensile test results showed that the thermal stability and mechanical properties of the WPU-DMG x -DA y films were significantly improved. More importantly, the WPU-DMG 4 -DA 4 film can be dissolved in a mixed acetone/ethanol solvent at room temperature. The recycled polyurethane solution could be dispersed in water to obtain a WPU emulsion again. After being recycled three times, the recovery efficiency of the mechanical properties of the WPU-DMG 4 -DA 4 film was higher than 90.1 ± 0.1 %, and the recycled film maintained its thermal stability and self-healing behavior. Moreover, the synthetic leather obtained by compounding WPU-DMG 4 -DA 4 and non-woven fabrics could be easily recycled through this process. The basic properties of the recycled non-woven fabric remained unchanged and the recycled WPU-DMG 4 -DA 4 resin could be reused. Therefore, the WPU-DMG 4 -DA 4 resin has broad application prospects in the tanning industry.

研究领域: 材料科学 · 聚合物化学 · 环境科学 · 可持续材料
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Interfacial C-O covalent bonds improving the piezo-assisted photocatalytic performance of Bi4Ti3O12@Carbon Schottky heterojunction

Kun Zhou,Wei Liu,Peifang Wang,Juan Chen,Huinan Che,Bin Liu,Yanhui Ao

Rational design of piezo-assisted photocatalytic systems for simultaneously efficient ultilization of solar and mechanical energy is promising but still challenging. In this work, a novel Bi 4 Ti 3 O 12 @C (BTO@C) Schottky heterojunction with high piezo-assisted photocatalytic performance is rationaly designed, and the degradation reaction rate constant k for RhB reaches 0.092 min −1 in 30 min. Experimental results and density functional theory (DFT) calculations show that C-layer is tightly coated on the surface of BTO. Furthermore, C-O covalent bonds , which act as electron transfer channels, are formed at the interface of BTO and C-layer. Meanwhile, the presence of piezoelectric potential field of BTO@C under piezo-assisted photocatalytic conditions further promotes the transfer of photogenerated electrons from BTO to C-layer, which synergistically contributes to the performance enhancement. This work provides a new idea for the design and development of efficient piezo-assisted photocatalytic materials.

CAS / MDL: 50-99-7 5593-70-4
研究领域: 材料科学 · 环境科学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Unique MIL-53(Fe)/PDI Supermolecule Composites: Z-Scheme Heterojunction and Covalent Bonds for Uprating Photocatalytic Performance

Hui Chen,Wengao Zeng,Yutang Liu,Wanyue Dong,Tao Cai,Lin Tang,Juan Li,Wenlu Li

It is important to find an effective way to enhance the photocatalytic efficiency of metal–organic frameworks. In this work, an organic supermolecule perylene diimide (PDI) semiconductor with a carboxyl terminal was added into the synthesis process of MIL-53(Fe) crystals. The PDI/MIL-53(Fe) (PM) composite photocatalyst was first obtained. The TC-H photodegradation rate of the most efficient 5PM was nearly 94.08% within 30 min, whose apparent reaction rate constant (k) is 4 times that of PDI and 33 times that of MIL-53(Fe), respectively. By investigation and characterization, it has been found that PDI nanofibers were dispersed and fixed in MIL-53(Fe) and bonded to each other by covalent bonds. The radical trap experiments and electron spin resonance analysis illustrated that hydroxyl radical (·OH), superoxide radical (·O2–), and photogenerated holes (h+) were active species. Combined with the band structure of PDI and MIL-53(Fe), it is proposed that the PM photocatalyst was a Z-scheme heterojunction mechanism. Therefore, PM photocatalysts showed excellent charge separation and transfer ability. The performance improvement of 5PM is due to enhanced visible light absorption, efficient charge separation, and excellent redox potential. Five cyclic photocatalytic tests and experiments further demonstrate that the 5PM photocatalyst has a promising future for pollutant removal.

研究领域: 材料科学 · 环境科学 · 化学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

Multiple non-covalent bonds reinforced pH/glucose-responsive alginate-stabilized Pickering emulsion for diacylated anthocyanin intestinal delivery

Qile Chen,Tong Ye,Shujuan Yang,Linwang Fan,Chaonan Shang,Yuhong Feng,Jiacheng Li,Yujuan Wang,Gaobo Yu,Jun Dai

The effective management of Type 2 Diabetes Mellitus (T2DM) depends on the development of streamlined, sustainable, and intelligent delivery systems. In this context, targeted stimulus-responsive Pickering emulsions (PEs) derived from biomass have emerged as a promising candidate. However, the interfacial films of PEs exhibit insufficient strength to endure the harsh gastric environment and lack the capability for targeted and responsive delivery. To address these limitations, an amphiphilic phenylboronic acid-functionalized sodium alginate (SA-PBA) was integrated into a ternary complex platform composed of soybean protein-isolated polyphenol (SPI-PSPAs), where it self-assembled into soft colloidal particles through multiple non-covalent interactions. A multiscale coupling methodology was proposed to investigate and elucidate the structure-function relationship between interfacial characteristics (e.g., thickness, viscoelasticity, and microstructures) and the stability of PEs, thereby providing a foundation for effectively controlling their targeted delivery properties. Notably, owing to the enhanced strength of the interfacial composite particle films, the PEs demonstrated the ability to withstand the harsh gastric environment while maintaining their structural integrity. Furthermore, the self-assembly process of the soft SA-PBA@SPI-PSPAs colloids could be modulated by external glucose stimuli, enabling the targeted and intelligent release of PSPAs in the intestinal environment. Consequently, the well-designed PE system achieved intestinal-targeted responsive release effects, highlighting the potential of the natural α-glucosidase (αG) inhibitor PSPAs as a viable clinical treatment for T2DM.

研究领域: 食品科学 · 生物医药 · 材料科学
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Polymer Chemistry · 2026 · IF 3.9

Mild-Temperature Self-Healing Bio-Based Polyurethane Film Enabled by Dual Dynamic Covalent Bonds and Segmental Design

Yingcheng Han,Dingchuan Zhang,Junjiang Li,Yulei Qi,Zixuan Tao,Hang Yin,Panfang Lu

This study successfully developed a bio-based polyurethane (PU-S-D) film that combines high mechanical strength with excellent mild-temperature self-healing properties. The material was prepared by pre-polymerizing castor oil with isophorone diisocyanate (IPDI), followed by chain extension using a mixture of 2-hydroxyethyl disulfide (HED) and dimethylglyoxime (DMG) as mixed chain extenders, constructing a multi-dynamic synergistic network wherein weaker disulfide bonds afford mild-temperature self-healing, stronger oxime-urethane bonds provide robust mechanical strength, and multiple hydrogen bonds serve to reinforce and integrate these functionalities. The structure and properties of the bio-based polyurethane film were thoroughly analyzed and discussed. This bio-based polyurethane film exhibits a high gel fraction (~90%) after more than 72 h and relatively high thermal stability (T₅₀% > 400℃). The glass transition temperature (Tg) of the film material is controlled near 30℃, ensuring it possesses sufficient molecular chains mobility at mild-temperature to trigger self-healing while simultaneously maintaining excellent mechanical strength. The mechanical performance results of film are outstanding: compared to the pure PU film, the tensile strength of the PU-S-D film increased by approximately 862% (reaching 12.4 MPa), while the elongation at break exceeded 310%. The film demonstrates remarkable self-healing performance, achieving a repair efficiency of 83% under conditions of 35℃ for 12 h. Molecular dynamics simulations and in situ infrared spectroscopy indicated that the dynamic disulfide bonds spontaneously recombine after fracture and induce the film's repair process. This research provides a method for developing bio-based, low-cost, high-performance materials. The developed dynamic covalent polyurethane network holds significant potential for practical applications requiring long-term durability and high reparability, such as protective coatings, high-performance adhesives, and durable composite matrices.

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