ACS Sustainable Chemistry & Engineering
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2023
·
IF 8.4
Chumeng Luo,Weichao Wang,Wei Yang,Xingyu Liu,Jun Lin,Liqun Zhang,Shaojian He
Epoxy (EP) vitrimers are currently regarded as ideal substitutes for traditional thermosetting resins, as this class of materials combines the advantages of thermoplastic and thermoset polymers. However, maintaining the high performance of EP vitrimers with excellent healing properties remains a challenge. In this work, a novel hardener combining disulfide and imine bonds through the reaction of Schiff base (4-AFD-VAN) was designed and then used to prepare the EP vitrimer with dual-dynamic covalent bonds. Compared to the single-disulfide-containing vitrimer (EVP-4-AFD), the prepared EP vitrimer (EPV-4-AFD-VAN) exhibited a lower activation energy and a faster stress relaxation. Moreover, EPV-4-AFD-VAN showed a tensile strength of up to 71.5 MPa and maintained a recovery ratio of approximately 90.0% during the three cycles. Similar to traditional thermoset EP, EPV-4-AFD-VAN retained its good solvent resistance, high breakdown strength, and good dielectric properties, which can be chemically degraded in suitable solvents, demonstrating its environmental sustainability.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Jiaofeng Ye,Junxiang Zhang,Libang Feng,Haocheng Liu,Danbin Zhu,Yanhua Liu
The development of self-healing materials has enabled the production of more reliable and intelligent materials. However, resolving the conflict between mechanical strength and self-healing efficiency as well as limited repair options of the self-healing materials is still the most pressing scientific challenge. In this study, a self-healing polyurethane with multiple repair methods is prepared by introducing disulfide bonds into thermo-reversible imine bonds-based polyurethane . The resultant polyurethane exhibits impressive comprehensive mechanical properties and preeminent repair capabilities. More importantly, damages can be repaired through various routes such as room temperature, moderate temperature, hair dryer blowing, and ethylenediamine assistance treatments. The superior mechanical properties, repetitive self-healing performance, and multiple options for repair is attributed to the cooperation of thermally reversible imine and disulfide exchanges, thermal motion of molecular chains , and dissociation/regeneration of hydrogen bonds . So this research provides numerous ideal options for repairing cracks and other damages in materials used in construction industry under different usage environments. Consequently, high-quality repairs, improved efficiency, and extended service life of construction engineering materials can be ensured.
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POLYMER COMPOSITES
·
2024
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IF 4.8
Lingyuan Liao,Wenhong Ruan,Mingqiu Zhang,Weihao Li,Musong Lin
Incorporation of boron nitride (BN) into polymers is a promising method to obtain composites with high thermal conductivity, low dielectric constant ( D k ), and dielectric loss ( D f ), while the practical applications are limited by the poor interface between BN and polymer because of surface energy mismatch and absence of covalent bond connection between them. Herein, polydopamine (PDA) with good adhesion is deposited onto the BN. Then, a different amount of silane coupling agent containing vinyl reactive groups is grafted onto PDA-coated BN. In this way, the surface energy of modified BN (m-BN) can be adjusted to ensure BN contacts well with polymers. Moreover, reactive groups were introduced on BN for further reaction. Subsequently, covalent bonds between the m-BN and the polyphenylene oxide (PPO) were established in situ during the curing process. The effects of the m-BN surface energy on interface quality and thermal conductivity of composites are investigated. The m-BN/PPO composite achieves a through-plane thermal conductivity of 5.87 W/m · K and a low D f value of 1.53 × 10 −3 , as well as a low coefficient of thermal expansion (CTE) value (7.8 ppm/K) when the m-BN loading is 32.6 vol%. This research provides a simple and efficient strategy for fabricating high-performance composites for high-frequency applications. Highlights Hexagonal boron nitride was modified successfully by combining non-covalent and covalent modifications. Regulating surface energy and establishing covalent bonds enhances interface interaction between BN and polyphenylene oxide. Modified BN/polyphenylene oxide composites display improvements in thermal conductivity and dimensional stability as well as dielectric loss. Provides a feasible strategy for designing polymer composites with high thermal conductivity, dimensional stability, and low dielectric loss for 5G applications.
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Journal of Energy Chemistry
·
2024
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IF 14
Yangyang Chen,Yu Liao,Ying Wu,Lei Li,Zhen Zhang,Sha Luo,Yiqiang Wu,Yan Qing
Lithium-sulfur batteries (LSBs) are considered promising candidates for next-generation battery technologies owing to their outstanding theoretical energy density and cost-effectiveness. However, the low conductivity and polysulfide shuttling effect of S cathodes severely hamper the practical performance of LSBs . Herein, in situ-generated single layer MXene nanosheet/hierarchical porous carbonized wood fiber (MX/PCWF) composites are prepared via a nonhazardous eutectic activation strategy coupled with pyrolysis-induced gas diffusion. The unique architecture, wherein single layer MXene nanosheets are constructed on carbonized wood fiber walls, ensures rapid polysulfide conversion and continuous electron transfer for redox reactions. The C–Ti–C bonds formed between MXene and PCWF can considerably expedite the conversion of polysulfides, effectively suppressing the shuttle effect. An impressive capacity of 1301.1 mA h g −1 at 0.5 C accompanied by remarkable stability is attained with the MX/PCWF host, as evidenced by the capacity maintenance of 722.6 mA h g −1 after 500 cycles. Notably, the MX/PCWF/S cathode can still deliver a high capacity of 886.8 mA h g −1 at a high S loading of 5.6 mg cm −2 . The construction of two-dimensional MXenes on natural wood fiber walls offers a competitive edge over S-based cathode materials and demonstrates a novel strategy for developing high-performance batteries.
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COMPOSITES SCIENCE AND TECHNOLOGY
·
2026
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IF 9.9
Yuchen Qu,Peiwen Yang,Siyun Liang,Yanqing Jiang,Gang Li,Xiaoping Yang
The integration of photo-thermal fillers and dual dynamic covalent bonds remains challenging for the fabrication of high-performance self-healable carbon fiber reinforced epoxy (CF/EP) composites. In this work, graphene (GN) reinforced epoxy matrices with boronic ester and Diels-Alder (DA) bonds (GN/FBA-EP, GN/FBA-DA-EP) and corresponding CF/EP composites were fabricated, and their self-healing performance by near infrared (NIR) heating was compared to that of unreinforced epoxy matrices (FBA-EP, FBA-DA-EP) and composites by conventional heating. The presence of N –C O and a negative shift in C C binding energy verified successful integration of GN and dual dynamic covalent bonds in GN/FBA-DA-EP. Compared to thermal responsive FBA-EP (93.01%, 85.97%) and FBA-DA-EP (94.99%, 91.02%), NIR responsive GN/FBA-EP and GN/FBA-DA-EP achieved higher first and second self-healing efficiencies (95.07%, 88.76% and 96.46%, 94.16%). In contrast to GN/FBA-EP containing single boronic ester bonds, dual-dynamic GN/FBA-DA-EP exhibited rapid recovery of cross-scratches under NIR heating, indicating that high photo-thermal conversion efficiency of GN activated the exchange reaction of boronic ester bonds, thereby facilitating the dissociation and rearrangement of DA bonds. Correlative 2D and 3D morphologies revealed that CF/GN/FBA-DA-EP achieved the minimal scratch depth and fastest recovery time under NIR heating compared to CF/GN/FBA-EP, which confirmed the improved first and second self-healing efficiencies (96.98%, 93.15%) from the synergy between GN and dual dynamic covalent bonds. This work presents a strategy for synergistically enhancing and accelerating the self-healing performance of epoxy matrices and CF/EP composites. Download: Download high-res image (331KB) Download: Download full-size image
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Materials Today Chemistry
·
2025
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IF 6.7
Xin Song,Chunfeng Li,Lei Le,Ruiwen Yu,Mingli Liu
Waterborne polyurethane (WPU) coatings have emerged as a preferred alternative to epoxy–based coatings for carbon fiber (CF) sizing, owing to their superior surface adhesion and environmental sustainability. However, conventional WPUs often suffer from insufficient mechanical strength, limited thermal stability, and inadequate adhesion. To address these limitations, molecular design and modification of WPU are imperative. Herein, a polyetheramine diol (PHBA–D1000) was synthesized via aldol condensation and Schiff base formation between 4–hydroxybenzaldehyde and Jeffamine D1000. This diol, along with co–monomers 4–amino–1–butanol, o–anisidine, and 2–aminophenol, was employed to fabricate modified WPUs (MPWPUs). The molecular architecture of the resulting MPWPUs incorporates dynamic reversible imine bonds, π–π conjugated stacking, aromatic ether linkages, polyurea, carbamate groups, and long alkyl chains. The synergistic interplay between the polar and rigid segments endowed the MPWPUs with enhanced thermal stability (T10 % at 331.2 °C), tensile strength (36.4 MPa), elastic modulus (14.2 MPa), and adhesion strength (21.9 kPa). Applying MPWPU as sizing coatings on CF significantly improved the fiber bundling capability, surface reactivity, wettability, and mechanical properties. The surface energy and tensile strength of MPWPU–coated CF monofilaments increased to 57.1 mN/m and 6.121 GPa, respectively, representing remarkable improvements of 57.3 % and 18.1 % compared to unsized CF. MPWPUs effectively repaired defects and microcracks on CF surfaces, thereby enhancing surface roughness. These findings underscore the exceptional performance of the developed MPWPUs and their considerable potential for advanced CF composite applications.
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Jin Qian,Xiaoting Hao,Duo Li,Chengshuai Lu,Lulu Chen,Wenjia Han,Zhuqing Liu
High mechanical strength (41.5 MPa) and self-healing efficiency (119%) achieved via DA dynamic covalent bonds and BC reinforcement. • BC-dispersed MWCNTs enable high sensitivity (GF = 10.15) and stable sensing over 0–130% strain. • The flexible electronic skin enables real-time monitoring of joint motions and ECG/EMG signals. Conventional waterborne polyurethane (WPU)-based flexible sensors often exhibit insufficient strength, limited self-healing capacity, and unstable cyclic performance. Herein, a self-healing WPU/bacterial cellulose (BC) composite matrix was fabricated by combining BC nanofiber reinforcement with thermally reversible Diels-Alder (DA) dynamic covalent bonds. Multi-walled carbon nanotubes (MWCNTs) were incorporated as the conductive phase. BC nanofibers interweave with WPU chains to provide topological confinement, while interfacial hydrogen bonding and physical entanglement anchor the polymer chains. At a BC loading of only 5‰, the composite achieved a tensile strength of 41.5 MPa and an elongation at break of 674%. The reversible DA bonds mitigate the trade-off between mechanical strength and self-healing, yielding a self-healing efficiency of 119% after thermal treatment, together with good thermal stability and recyclability. BC also suppresses MWCNT agglomeration and promotes the formation of stable conductive networks. The resulting films exhibited a gauge factor (GF) of 10.15, a stable sensing response over a strain range of 0–130%, and the ability to detect human motion, electromyographic, and electrocardiographic signals. These multifunctional composite films combine mechanical robustness, self-healing performance, and reliable sensing behaviour, indicating their potential for wearable electronics and physiological monitoring. Download: Download high-res image (146KB) Download: Download full-size image
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POLYMER COMPOSITES
·
2024
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IF 4.8
Fangshan Li,Heng Wang,Yuchao Ke,Yuan Hu,Ru Xia
[AMIm]Cl@GNP/SBR composites were prepared by blending ionic liquid 1-allyl-3-methylimidazolium chloride salt([AMIm]Cl) modified graphene nanoplatelets (GNP) and styrene-butadiene rubber (SBR). The mechanical and thermal properties as well as the structure–activity relationship of the obtained composites based on the modified filler were investigated under the synergistic effect of non-covalent and covalent bonding. The experimental results indicated that the modification of GNP by [AMIm]Cl occurred under mild conditions. The dispersibility of [AMIm]Cl@GNP in SBR was enhanced by its participation in vulcanization and the synergistic effect of non-covalent and covalent cross-linking networks such as cation-π, π-π, and hydrogen bonds. This improvement led to an increase in the interfacial bond strength of the composites and a reduction in the interfacial thermal resistance. These effects resulted in both reinforcement and thermal conductivity properties. The tensile strength and elongation at break of [AMIm]Cl@GNP/SBR composites increased from 18.2 to 22.9 MPa and from 737.9% to 923.5%, respectively, when the modification ratio of [AMIm]Cl was 1% and the loading of [AMIm]Cl@GNP was only 4 phr (mass ratio). At the same time, the thermal conductivity in the vertical direction of the composites increased from 0.25 to 0.44 W/(m·K), and the thermal conductivity in the horizontal direction increased from 0.27 to 0.81 W/(m·K). Highlights Modified powder [AMIm]Cl@graphene nanoplatelets were prepared; [AMIm]Cl@graphene nanoplatelet/styrene-butadiene rubber blend was prepared; Mechanical properties of blends significantly improved over blank; The horizontal thermal conductivity of the blends increases obviously; The vertical thermal conductivity of the blends was improved.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 38
·18039-18048
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IF 3.3
Yuan Nie,Mei Li,Shouhai Li,Mingtao Lin,Na Yao,Tianxiang Deng,Xiao Feng,Xiaohua Yang,Haiyang Ding,Lina Xu
The development of recyclable biopolymers from renewable resources is of great importance to sustainable development and environmental protection. Biopolymers not only provide a platform for achieving a friendly environment, but also reduce dependence on fossil fuel elements. In this study, a castor oil-based macromolecule prepolymer containing reactive isocyanate groups was firstly synthesized, and next a series of recyclable bio-polymers containing dynamic Diels–Alder bonds, imine bonds and hydrogen bonds were designed and fabricated by the introduction of furfural derivatives and vanillin. Dynamic covalent bonds and hydrogen bonds can bestow biopolymers with excellent comprehensive properties, including high self-healing efficiency, shape memory and reprocessability. Meanwhile, the formation of a reversible cross-linked network of hydrogen and dynamic bonds significantly improved the mechanical properties and endowed the biopolymers with self-healing capability. Fourier transform infrared spectroscopy and 1H nuclear magnetic resonance indicate the successful preparation of the biopolymers. Thermal gravimetric analysis demonstrates that the materials as-prepared possess high thermal stability. Mechanical tests show that the materials have excellent mechanical properties with a maximum stress of 36.44 MPa. Surface scratches can be repaired at 120 °C for 5 minutes. The biopolymers also exhibit shape memory properties. This work will contribute to the development and study of functional self-healing biopolymers.
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MACROMOLECULAR MATERIALS AND ENGINEERING
·
2020
·Vol. 306
·期 2
·2000577
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IF 3.853
Minglei Ma,Jumin Yang,Zhanpeng Ye,Anjie Dong,Jinwei Zhang,Jianhua Zhang
The self-healable hydrogels have attracted increasing attention due to their promising potential for ensuring the durability and reliability of hydrogels. However, they still face a serious challenge to achieve a positive balance between mechanical and healing performance, especially for the room-temperature autonomous self-healable hydrogels. Herein, a simple but efficient strategy to fabricate a kind of dynamic boronate and hydrogen bonds dual-crosslinked double network (DN) hydrogel based on a UV-initiated one-pot in situ polymerization of N -acryloyl glycinamide (NAGA) in polyvinyl alcohol-borax slime is reported. The obtained PN- x /PB hydrogels, especially with high content of PNAGA, are shown to possess high mechanical strength, high toughness, and fatigue-resistance properties as well as excellent self-healability at room temperature (nearly 88% self-healing efficiency based on the strain compression test), due to the dynamic DN structure, and the combination of the adaptable and reconfigurable dynamic boronate bonds and hydrogen bonds. Considering the easily available materials and simple preparation process, this novel strategy should offer not only a kind of dynamic DN hydrogel with robust mechanical performance and high self-healing capability, but also enrich the methodological toolbox for synergistic integration of dynamic covalent bonds and hydrogen bonds to surmount the tradeoff between mechanical properties and self-healing capacity of hydrogels.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2019
·Vol. 95
·期 4
·1116-1125
·
IF 2.659
Han Zhang,Shao-Feng Hua,Lei Zhang
BACKGROUND The objective of this research was to use a step-by-step method to prepare a novel biocatalytic system (GO-CEL-E/N-GA-GOD): -OH and -COOH on the surface of graphene oxide (GO) were used to immobilize cellulase (CEL) and glucose oxidase (GOD), respectively, which may be easier to control the loading of enzymes with different kinds, to achieve the one-pot conversion of gluconic acid from carboxymethyl cellulose (CMC). RESULTS The loadings capability of CEL and GOD on GO-CEL-E/N-GA-GOD were 49.07 ± 7.47 mg g −1 and 10.22 ± 2.03 mg g −1 , respectively. The multi-enzyme systems had shallow temperature and pH optima of 40 °C and 5.0. The kinetic constants of GO-CEL-E/N-GA-GOD (of CEL-GOD) were K m = 0.15 ± 0.02 (0.43 ± 0.09) mmol L −1 , V max = 0.18 ± 0.01 (0.21 ± 0.07) μmol L −1 s −1 , and k cat / K m = 24.12 ± 0.52 (17.74 ± 0.85) s −1 mmol −1 L. Nearly 65% of the initial activity of GO-CEL-E/N-GA-GOD could be retained after seven cycles. Notably the conversion of gluconic acid was able to reach 63.82 ± 8.03% within 2 h. CONCLUSION Step-by-step immobilization method made full use of different functional groups on GO, avoiding the competition for fixed sites between CEL and GOD in the immobilization processes. The results reflected the feasibility of the strategy to build bio-microsystem as CEL and GOD immobilized on GO by covalent bonds to achieve the conversion from CMC to gluconic acid in one-step. © 2019 Society of Chemical Industry
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yating Ai,Jiajie Hu,Xianqiang Xiong,Sónia A.C. Carabineiro,Yuesheng Li,Nikolay Sirotkin,Alexander Agafonov,Kangle Lv
Efficient interfacial charge transfer and robust interface interactions are crucial to achieve superior spatial separation of carriers and develop advanced heterogeneous photocatalysts . This study describes the synthesis of a novel S-scheme heterojunction of ZnO/In 2 S 3 , with S−O covalent bonds , achieved through a hydrothermal method . The optimized heterojunction shows exceptional photocatalytic activity , achieving a H 2 generation rate of 2488 μmol g −1 h −1 and a degradation efficiency of 86 % for tetracycline hydrochloride (TCH) within 2 h. These values surpass those of In 2 S 3 alone by 35 and 1.4 times, respectively. Various techniques, including electron spin resonance, X-ray photoelectron spectroscopy, Kelvin probe force microscopy and density functional theory calculations confirm the S-scheme heterojunction. The establishment of a chemical S−O bond between In 2 S 3 and ZnO facilitates an atomic level interfacial pathway, enabling efficient transportation of interfacial electrons.
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