Zejian He

Nanoparticle toughening of polymers has long been constrained by the inherent trade-off between strength and toughness. Here, we report a supramolecular polymer nanoparticle toughening strategy based on an H2G2-type monomer (H2G2-1). During epoxy curing, H2G2-1 undergoes in situ self-assembly into supramolecular polymer nanoparticles (H2G2-NPs), which serve dual roles: acting as physical cross-linking points for reinforcement, while their reversible host–guest interactions function as sacrificial bonds that dissociate under stress to dissipate energy. This strategy ensures uniform nanoparticle dispersion and excellent interfacial compatibility. Compared to neat epoxy, the H2G2-NPs-toughened epoxy exhibits a 92.6% increase in elongation at break, a 66.0% increase in tensile strength, and a 233% increase in toughness, achieving synergistic strengthening and toughening. This work provides a new strategy to make high-performance toughened polymers.

Achieving efficient synergy between covalent and supramolecular polymers is an effective strategy for developing novel polymeric materials. However, realizing this synergy through rational chemical design to efficiently integrate both types of polymers within a single polymer network remains a significant challenge. Here, we achieve efficient synergy between covalent and supramolecular polymer chains by inducing entanglement of unsymmetrical topological nodes. Benefiting from the molecular entanglement strategy, this synergistic network effectively integrates the stability of a covalent polymer and the dynamics of a supramolecular polymer. While maintaining the integrity of the network, the reversible host-guest recognition in the supramolecular polymer dissipates the applied energy, thus allowing the mechanical properties of the entire network to be regulated. Besides, the host-guest recognition pairs can serve as splicing points for integrating additional polymers, transforming the topologically entangled covalent-supramolecular synergistic polymer platform into a multifunctional platform that accommodates a variety of polymers, significantly increasing the diversity of their structures and properties. These findings may spur further innovations in the field of polymers in general, as well as promote a deeper understanding of dynamic chemistry.

Achieving the efficient integration and synergy of multi-component polymers is an effective approach for the development of new polymer materials and breakthroughs in performance. However, there are still considerable challenges in achieving molecular-level integration of multi-component polymers. Here we report polymer chain entanglement through asymmetric entangled nodes, inspired by macroscopic woven materials with different warp and weft strands, achieving the integration of polyurethane and epoxy resin chains at the molecular level. The abundant dynamic entanglements within the polymer network, reminiscent of woven topologies, enable the flexible polyurethane chains and rigid epoxy chains to work synergistically under external stress, thereby imparting excellent mechanical and adhesive properties to the final network. This study demonstrates the potential of weaving-inspired molecular-level entanglement in polymer integration and performance modulation, while also providing an important reference for the design of novel multi-component polymeric materials through weaving-inspired strategies.

Nowadays, gastroesophageal reflux disease (GERD) has emerged as one of the major hazards to the health of the upper gastrointestinal tract, and there is an urgent need for a low‐cost, user‐friendly, and non‐invasive detection method. Herein, a paper‐based sensor (CP sensor) for the non‐invasive screening of GERD is proposed. The sensor is structured as a specially shaped cellulose paper strip embedded with fluorescent colloids, which are self‐assembled from a cleavable synthetic fluorescent polymer (P4). Benefiting from the introduction of amide bonds and the unique assembled structure of the nanocolloids, the pepsin in the sample solution will hydrolyze the water‐soluble branches in the micellar shell during detection, resulting in a corresponding output of the fluorescent signal. This responsiveness, which can be observed by the naked eye, is so sensitive with a minimum detectable concentration for pepsin as low as 0.3 ng·mL⁻¹. Clinical trials have further demonstrates that the designed paper sensor is capable of providing improved accuracy in the early diagnosis of GERD.

Slide‐ring polymers exhibit distinctive mechanical properties, making them highly promising for applications in emerging fields such as energy storage devices and smart sensing. However, existing slide‐ring polymer systems primarily rely on hydrophilic‐hydrophobic interactions to achieve ring‐axle interlocking in aqueous phases. This reliance limits the construction of slide‐ring networks mainly to water‐soluble polymers, excluding a diverse range of lipophilic polymers. Therefore, it is crucial to introduce efficient construction strategies that facilitate interpenetration in organic solvents, enabling the development of diverse slide‐ring polymers and expanding their range and applications. Herein, by utilizing the pillar[5]arene/alkyl chain host−guest interactions, we successfully facilitated the interpenetration of a pillar[5]arene and poly(caprolactone), enabling the efficient construction of two slide‐ring polymer networks in organic solvents. One of these two slide‐ring polymers demonstrates a unique network deformation mechanism along with outstanding mechanical properties compared with the control covalently cross‐linked polymer network, including maximum stress (4.43 vs 1.98 MPa), maximum strain (1285 vs 330 %), and toughness (35.4 vs 3.92 MJ/m³). More importantly, this strategy of making slide‐ring polymers is highly versatile, given the wide range of macrocyclic arenes and alkyl chain‐containing polymers it can accommodate.

Slide‐ring polymers exhibit distinctive mechanical properties, making them highly promising for applications in emerging fields such as energy storage devices and smart sensing. However, existing slide‐ring polymer systems primarily rely on hydrophilic‐hydrophobic interactions to achieve ring‐axle interlocking in aqueous phases. This reliance limits the construction of slide‐ring networks mainly to water‐soluble polymers, excluding a diverse range of lipophilic polymers. Therefore, it is crucial to introduce efficient construction strategies that facilitate interpenetration in organic solvents, enabling the development of diverse slide‐ring polymers and expanding their range and applications. Herein, by utilizing the pillar[5]arene/alkyl chain host−guest interactions, we successfully facilitated the interpenetration of a pillar[5]arene and poly(caprolactone), enabling the efficient construction of two slide‐ring polymer networks in organic solvents. One of these two slide‐ring polymers demonstrates a unique network deformation mechanism along with outstanding mechanical properties compared with the control covalently cross‐linked polymer network, including maximum stress (4.43 vs 1.98 MPa), maximum strain (1285 vs 330 %), and toughness (35.4 vs 3.92 MJ/m³). More importantly, this strategy of making slide‐ring polymers is highly versatile, given the wide range of macrocyclic arenes and alkyl chain‐containing polymers it can accommodate.

The Biginelli reaction, a three-component cyclocondensation reaction, is an important member of the multicomponent reaction (MCR) family. In this study, we conducted end-group modifications on a variety of biodegradable polyesters, including poly(1,4-butylene adipate) (PBA), poly(ε-caprolactone) (PCL), polylactic acid (PLA), and poly(p-dioxanone) (PPDO), based on the precursor polyethylene glycol (PEG). By combining two polymers through the Biginelli multi-component reaction, four new biodegradable polyester copolymers, namely DHPM–PBA, DHPM–PCL, DHPM–PLA, and DHPM–PPDO, were formed. These Biginelli reactions demonstrated exceptional completeness, validating the efficiency of the synthesis strategy. Although the introduction of various polyesters lead to different properties, such as crystallinity and cytotoxicity, the newly synthesized 3,4-dihydro-2(H)-pyrimidinone compounds (DHPMs) exhibit enhanced hydrophilicity and can self-assemble in water and N,N-dimethylformamide (DMF) solution to form micelles with a controllable size. Furthermore, DHPM–PPDO promotes cellular growth and has potential applications in wound healing and tissue engineering. In conclusion, this method demonstrates great universality and methodological significance and offers insights into the medical applications of polyethylene glycol.

The raw materials of Poly(ethylene terephthalate) (PET) are derived from petroleum‐based resources, which are no sustainable. Therefore, previous researchers introduced biomass‐derived 2,5‐tetrahydrofurfuryl dimethanol (THFDM) into PET. However, its heat resistance has decreased compared to PET. In this paper, a novel bio‐based copolyester, poly(ethylene glycol‐co‐2,5‐tetrahydrofuran dimethanol‐co‐isosorbide terephthalate) (PEIFT), is prepared by introducing biomass‐derived isosorbide (ISB) and THFDM into the PET chains through melting copolymerization process. With the introduction of ISB content, copolyesters' hydrophilicity and rigidity improve. Compared to PET, glass transition temperature (T_g) increases by over 5 °C. In addition, the toughness and spinning performance of PEIFT have also been improved as a result of the addition of THFDM components. The hydrophobicity of PEIFTs electrospinning is greatly improved, with a contact angle exceeding 135°. Finally, due to the good hydrophobicity of PEIFTs nanofibers, they have potential application value in the manufacture of hydrophobic nanofiber and filter films. Given its biomass source and excellent performance, they make it easier to replace materials derived from petroleum.