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Advanced Healthcare Materials · 2025 · IF 9.6

Optimized Bio-Based Polyurethane Structure for Enhanced Durability and Biocompatibility in Artificial Ligaments

Jiamei Fu,Mengqiu Quan,Haiquan Sun,Junyi Zhou,Qingyi Xie,Minghui Cui,Xiaolin Wang,Fenglong Li,Jin Zhu,Jing Chen

In the field of sports medicine, especially in high-intensity sports such as football, basketball, and skiing, ligament injuries are extremely common. However, current artificial ligaments face multiple critical limitations, including suboptimal biocompatibility, limited host tissue integration, insufficient mechanical durability to withstand physiological stresses, and inadequate durability during long-term cyclic loading. To address these challenges, 1-(2-Hydroxyphenyl)-3-phenyl-2-propenone (HCC), which shared structural similarity with naturally occurring chalcones, is employed as the raw material for the chain extender, combined with HMDI and polycaprolactone diol (PCL diol), to synthesize a novel polyurethane (HCMPU). The results showed that the maximum stress of HCMPU-3 reached 42.1 MPa, with an elongation at break of up to 710%. It also demonstrated outstanding durability, maintaining structural integrity without significant degradation after 5000 loading cycles. Additionally, during the initial implantation period, its stability in an enzymatic environment can provide strong support to the human body before new tissue regeneration, making it a promising candidate for an ideal artificial ligament. Moreover, the favorable biocompatibility of HCMPUs is demonstrated through cytotoxicity testing and rat pathological staining sections. Therefore, this work demonstrated the potential of HCMPU to overcome key limitations in current artificial ligaments and advance the development of next-generation materials for ligament repair.

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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Biomimetic stiffness modulator driven by bi-mode hydrogen bond locking mediated nano-heterogeneous aggregation

Chentong Gao,Xu Zhou,Yi Yang,Zhaoxu Yang,Xin Jing,Zemian Zuo,Jing Li,Binbin Dong,Hao-Yang Mi,Chuntai Liu,Changyu Shen

The ability to dynamically adjust mechanical stiffness is crucial for materials requiring adaptive responses. However, simultaneously achieving broad-range reversible modulus regulation, high toughness, and robust impact resistance remains a significant challenge. Herein, inspired by the stiffness modulation mechanisms in biological systems, we developed a bi-mode biomimetic stiffness modulator (BSM) with reversible modulus transition, high toughness, and impact-resistant properties. The BSM has a comb-like molecular configuration structure with a hydrophobic main chain and hydrophilic side chains. This unique design enables a bi-mode soft–stiff transition, mediated by hydrogen bond locking and nano-heterogeneous aggregation. When exposed to polar or nonpolar molecules, the hydrophilic and hydrophobic segments are selectively locked. This leads to the formation of nano-heterogeneous aggregation microdomains and a substantial improvement in mechanical properties. This strategy allows the modulus to reversibly increase by 9.9 times, while still maintaining ultrahigh toughness (254.44 MJ m −3 ) and exceptional impact resistance. Moreover, the soft-stiff transition of bi-mode BSM is fully reversible and it can be thermally recycled and remediated with negligible property loss. The bi-mode BSM demonstrates excellent functionality in the smart protection of automotive windows and wearable electronics from harsh conditions and serious impacts. Bi-mode BSM provides a new molecular design paradigm for high-performance modulators in flexible electronics and protective systems.

CAS / MDL: 5124-30-1 36890-68-3
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Surfaces and Interfaces · 2025 · IF 6.3

Shape Memory Polyurethane Material with Programmable Interface Promotes Osteogenesis in vitro

Xingguo Zhou,Bin Zou,Qinghua Chen,Gongxian Yang,Qingguo Lai,Xinfeng Wang

Micropatterns with bionic properties influence cellular behavior through mechanotransduction, a process that plays a crucial role in promoting bone repair. However, bone regeneration is a complicated physiological process that involves multiple cell types and mechanisms. In the early stages of bone restoration, micropatterned surfaces on bone implants can prematurely promote osteogenic differentiation. This premature differentiation is detrimental to the accumulation of initial cell numbers, ultimately delaying both bone growth and overall bone accumulation. In light of this, the fabrication of thermally stimulated polyurethane with exceptional shape memory properties enabled dynamic response of the micropatterned interfaces, enabling precise switching between proliferation and differentiation phases for enhanced osseointegration. Furthermore, cell proliferation and ALP activity assays of MC3T3-E1 were used to assess the osteoinductive effects of shape memory polyurethane. The results demonstrated that the temporary flat interface of the smart dynamic membrane effectively promoted cell proliferation, while the responsive microstructure significantly improved early osteogenic differentiation compared to the static micropatterned membrane.

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BIOMATERIALS · 2026 · IF 13.6

Constructing highly bioactive and tough polyurethane bone adhesives by covalently integrating nanohydroxyapatite

Lei Tong,Yaling Cheng,Yuxiang Wang,Na Li,Jie Liang,Yong Sun,Yujiang Fan,Xingdong Zhang

Achieving both robust mechanical and osteogenic properties of bone adhesives remains challenging. Here, we developed a novel polyurethane-based bone adhesive (PCLU- g -nHA) by covalently incorporating aminated nanohydroxyapatite (nHA-NH 2 ) into a biodegradable poly (ε-caprolactone) urethane (PCLU) network. This design promoted uniform nHA dispersion and strong organic–inorganic integration through urea linkages, significantly enhancing compressive modulus (4.91 ± 0.10 MPa) and adhesive strength (3.41 ± 0.24 MPa in lap-shear). The adhesive cured rapidly under mild conditions with minimal heat release. PCLU- g -nHA showed improved biocompatibility and stimulated bone marrow mesenchymal stem cells (BMSCs) osteogenic differentiation in vitro . Transcriptomics revealed upregulation of extracellular matrix remodeling and collagen synthesis pathways. In vivo , PCLU- g -nHA enhanced bone regeneration and osseointegration in rabbit femoral condyle defect and tibial fracture models, outperforming a commercial PMMA bone cement. This study offers a scalable strategy for developing highly bioactive and tough bone adhesives with clinical translational potential.

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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Dual-crosslinked polyurethane elastomers based on diselenide bonds and strain-induced crystallization for high elasticity, self-healing, and strain/temperature-responsive sensing

Ke Zheng,Shaoyun Guo,Xianlong Zhang

Thermoplastic polyurethane elastomers (TPUs) have been increasingly applied in soft robotics and flexible electronics. However, conventional TPUs often exhibit limited thermal stability and poor interfacial fatigue resistance, and single reinforcement strategies are insufficient to achieve a balanced enhancement of strength, elasticity, and thermal stability. In this study, we propose a dual-crosslinking strategy coupled with strain-induced crystallization to address these challenges. Poly(ε-caprolactone) diol (PCL) is incorporated into the polyurethane backbone, enabling the formation of a crystalline reinforcement phase under deformation. A covalent network is formed via the polyaddition of trimethylolpropane (TMP) and isocyanate groups (-NCO), while the incorporation of 2-(1-hydroxyethyl) diselenide (DiSe-DiOH) introduces a dynamically reversible diselenide network, together producing a double-crosslinked structure. The resulting polyurethane elastomer (DiSe-PU) exhibits outstanding overall performance, including high tensile strength (18.31 MPa), large elongation at break (1881%), high toughness (114.46 MJ/m 3 ), and good thermal stability (Td 5%  = 280 °C). It also exhibits controllable self-healing behavior, achieving stress and strain healing efficiencies of 66.67% and 98.25%, respectively, when activated by ethanol and further promoted by heating. Furthermore, a flexible sensor fabricated by integrating DiSe-PU with the ionic liquid [EMIm][TFSI] demonstrates dual strain and temperature responsiveness, achieving a gauge factor of 0.41 and a temperature coefficient of resistance of −0.02 °C −1 . This work offers an effective strategy for developing high-performance, self-healing, multifunctional polyurethane elastomers.

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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Fluorinated bi-layer E-textile enabled by electrospinning rotary collection for self-powered dual-functional electrochemical sweat sensing and motion detection

He Zhao,Chu Xu,Caobin Zhou,Ling Zhang,Chunzhong Li

Existing triboelectric nanogenerators (TENGs) for wearable sweat sensors are plagued by low power density, which restricts their practical application. This study focuses on boosting TENGs output power via a fluorinated bi-layer electronic textile (e-textile) fabricated by electrospinning rotary collection, enabling self-powered dual functionality: real-time electrochemical sweat sensing and human motion detection. The key design includes a PCLU-HFDD negative triboelectric layer (molecularly incorporated with hexadecafluorodecanediol to enhance electron affinity) and a poly(lactic- co -glycolic acid) (PLGA) positive layer. Rotary collection creates vein-like nanostructures on PCLU-HFDD yarns (6.2 μm roughness, 114.8° water contact angle), increasing contact area. The PCLU-HFDD TENG achieves a high power density of 0.66 W m −2 , an open-circuit voltage (Voc) of 117.08 V, and excellent stability over 35,000 contact-separation cycles. Critically, integrated with both sweat-sensing and motion-detection capabilities, the e-textile enables 180-min continuous glucose monitoring (under sedentary conditions) and recognition of human motions. This work confirms that the power enhancement not only overcomes the bottleneck of TENGs for wearable sensors but also facilitates dual-modal health monitoring, advancing the development of practical wearable bioelectronics.

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MACROMOLECULAR RAPID COMMUNICATIONS · 2026 · IF 4.3

Photothermal Self-Healing Waterborne Polyurethane with Antibacterial, Hydrophobic, and Oleophobic Properties Based on Dynamic Hindered Urea Bonds

Jianhua Zhou,Jing Zheng,Fangxin Dong

To endow polyurethane coating with photothermal self-healing, antibacterial, hydrophobic, and oleophobic properties, in this study, cellulose nanofiber coated with polydopamine and silver nanoparticles (CNF@PDA@AgNPs) and hindered urea bonds were introduced into fluorinated waterborne polyurethane as functional nanofillers and dynamic motifs, respectively. Owing to the remarkable photothermal property of CNF@PDA@AgNPs and the presence of dynamic hindered urea bonds, the photothermal self-healing fluorinated waterborne polyurethane urea (PSF-WPU) film exhibited excellent self-healing capability. Under a xenon lamp irradiation with an intensity of 100 mW/cm 2 for 4 h, the self-healing efficiency of its tensile strength and elongation at break reached 95.20% and 95.19% of its original properties, respectively. With the increase of CNF@PDA@AgNPs dosage, the water-oil contact angles of the PSF-WPU film increased. Furthermore, silver nanoparticles (AgNPs) as antibacterial agents endowed PSF-WPU finished fabrics with excellent antibacterial properties, with 99.37% and 90.29% against E. coli and S. aureus , respectively. This work offers a feasible approach for fabricating self-healing waterborne polyurethanes with outstanding photothermal antibacterial, mechanical, hydrophobic, and oleophobic performances that have great potential in the areas of coatings, textiles, leather, and biomedicine.

CAS / MDL: 4062-60-6 36890-68-3
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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Polyurethane-based high-performance strain sensor with sliding cyclodextrin molecules

Qifan Guo,Caobin Zhou,Yuan Xu,Ling Zhang,Chunzhong Li

Dissipates stress and stabilizes AgNWs networks via polyrotaxane sliding rings • Achieves 700% strain, GF = 141, and 20,000-cycle stability at 200% strain • Realizes 98% self-healing at 50 °C for 30 min, 13.8 g/(m 2 ·h) air permeability and alkaline degradation • Enables monitoring of human motions for long-term wearable use Flexible resistive strain sensors based on silver nanowires (AgNWs) demonstrate significant potential for wearable electronics and human motion monitoring; however, they face substantial challenges due to severe modulus mismatch and limited cyclic stability under large-amplitude strain. In this context, a sandwich-structured strain sensor was developed based on supramolecular polyurethane functionalized with dynamic polyrotaxane (PR) sliding rings, where the freely mobile α-cyclodextrin units dissipate interfacial stress and stabilize the AgNWs conductive network under repeated stretching. The optimized sensor achieves an ultra-wide operational strain up to 700% and a high gauge factor of 141. Importantly, it maintains a stable resistance response over 20,000 loading-unloading cycles at 200% strain, surpassing all previously reported pristine AgNWs-based counterparts. Additionally, it exhibits 98% mechanical self-healing efficiency at 50 °C within 30 min, along with excellent breathability and alkaline degradability. This research presents a promising strategy for the development of high-performance, sustainable wearable sensing devices.

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ACS Applied Materials & Interfaces · 2026 · IF 7.8

Healable, Strong, and Tough Polyphenol-Based Polyurethanes Engineered via Synergistic Reversible Cross-Linked Microphase: Breaking the Performance Trilemma for Artificial Ligaments

Yan Huang,Qingqing Hao,Hao Chen,Jianyu Liu,Jie Liu,Zhirong Xin,Chunyang Bao

Achieving a harmonious balance among healability, high mechanical strength, and exceptional toughness remains a persistent and formidable challenge in the development of artificial ligaments. Herein, we report a class of polyphenol-based reversible cross-linked polyurethanes (RCPUs) designed to overcome this long-standing performance trilemma. By synergistically integrating dynamic hydrogen bonds, phenolic urethane bonds, and finely engineered microphase separation structures, the RCPUs achieve an exceptional combination of mechanical robustness, self-healing capability, and antibacterial activity. The optimized RCPU1.8 demonstrates a tensile strength of ∼57.5 MPa and toughness of ∼323.8 MJ m–3, along with a healing efficiency of ∼88.1% after 12 h at 75 °C. Furthermore, a simple prestretching treatment significantly enhances the tensile strength to ∼167.7 MPa while maintaining excellent fatigue resistance over 100 loading cycles. This work provides a scalable and synergistic strategy for developing next-generation multifunctional artificial ligaments with well-balanced performance.

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Materials Today Communications · 2022 · IF 3.662

Temperature-dependent adhesive polymer-based composites with shape adaptability and low thermal contact resistance for thermal management

Zhihui Lei,Chengyi Song

This work presents a new concept of incorporating temperature-dependent reversible adhesion and shape memory performances into the application of three-dimensional thermal management. Both the two performances root in the temperature-triggered crystallization characteristic of poly(ε-caprolactone) (PCL). The dynamic interfacial bonding helps to reduce the thermal contact resistance of polymer-based composites to 0.085 K·cm 2 ·W −1 , and the shape memory ability can be adapted to various heat sources with complex structures. The cooperation of adhesion and shape memory properties endows the PCL-based composites with more advantages than the traditional matrixes in a wide range of applications including thermal management, flexible electronics, and wearable devices .

CAS / MDL: 814-68-6 36890-68-3
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INDUSTRIAL CROPS AND PRODUCTS · 2023 · IF 5.9

Ultra-strong and solvent-free castor oil-based polyurethane thermally conductive structural adhesives for heat management

Cui Xu,Xiao Jia,Jun Du,Feng Zhou,Bin Liu,Yamin Deng,Xiulan Huai

Thermally conductive structural adhesives (TCSAs) are rendered high requirements with the rapid development of electronic devices towards miniaturization, light-weight and electrically insulating performance. Improving heat dissipation capacity and mechanical properties are both critical for the application of TCSAs as the interconnected materials between chips and metal substrates. Herein, we prepared environment-friendly TCSAs with different hard segments (HS) contents by using castor oil-based polyurethane (PU) as matrix and alumina (Al 2 O 3 ) as thermal conductive filler through an extremely facile mechanical-mixing process. Impressively, the TCSA with 49.3% HS content exhibited an intense notable tensile stress of 8.6 MPa, a high elongation at break of 21%, and an excellent lap shear strength to different substrates, including organic glass (7.7 MPa), steel (9.5 MPa), cooper (10.3 MPa) and aluminum (14.2 MPa). Furthermore, the thermal conductive pathways in composites with 75 wt% Al 2 O 3 fillers endow its good thermal conductivity with thermal conductivity k of 1.23 W/(m·K), 4.7 times higher than that of pure PU ( k = 0.26 W/m·K). Overall, our fabricated TCSAs not only possessed superior mechanical performances but also high thermal conductivity, as well as showed great potential in thermal management application fields due to its simple and environmental fabricating method.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Dual-hard phase structures make mechanically tough and autonomous self-healable polyurethane elastomers

Xiankun Wu,Jiale Zhang,Haonan Li,Huihui Gao,Mang Wu,Zhongkai Wang,Zhong Wang

It is a key challenge to combine high mechanical strength and excellent autonomous self-healing properties in one elastomer to match the requirements of commercial applications. Chemical cross-linking or ordered crystalline domains can afford high mechanical strength but are often based on the cost of losing autonomous self-healing performance. To address this dilemma, a strategy involving dual hard-phase structures was developed to reinforce self-healing polyurethane elastomers, by introducing plant oil-derived aliphatic chains into the hard segments. The dangling fatty acids not only allow segmental motion of the hard domains but also suppress the crystallization within polyurethane soft segments. The tailored dual-hard phase structure and dynamic chain motion are responsible for outstanding mechanical properties (tensile strength to 21.8 MPa and toughness of 131.6 MJ m −3 ) and autonomous self-healing ability (∼100 % healing efficiency). Furthermore, a versatile mechanical robust flexible conductor is conveniently constructed with an auto-repair capability at ambient conditions. This work represents a molecular design paradigm of simultaneously integrating balanced mechanical strength, durability, and self-healing ability for high-performance elastomers that can find applications such as skin-inspired wearable devices.

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