Recently, we reported a series of reversibly interlocked polymer networks(RILNs), whose mechanical robustness and functionalities improvement was believed to be derived from topological interlocking of two sub-network...Recently, we reported a series of reversibly interlocked polymer networks(RILNs), whose mechanical robustness and functionalities improvement was believed to be derived from topological interlocking of two sub-networks, although the direct evidence for the deduction is still lacking. Herein, a specially-designed RILNs system, in which the inter-component hydrogen bonds can be shielded as needed, was prepared and used to study the micro-structures of RILNs, aiming to verify the existence of mechanical interlocking in RILNs. By changing the pH of the swelling solvent, the effect exerted by the inter-component non-covalent bonds was eliminated, so detailed information of the networks structure was exposed. The small angle X-ray scattering(SAXS) and small-angle neutron scattering(SANS) results indicated that swelling-induced structural evolution of the two sub-networks mutually affected each other, even when the inter-component hydrogen bonds were absent, proving the presence of topological interlocking. The findings may help to draw a more accurate physical image and reveal the detailed structureproperty relationship of RILNs.展开更多
Mechanically interlocked networks(MINs)provide a versatile platform for engineering materials that combine mechanical strength with dynamic adaptability.Their performance hinges on the constrained intramolecular motio...Mechanically interlocked networks(MINs)provide a versatile platform for engineering materials that combine mechanical strength with dynamic adaptability.Their performance hinges on the constrained intramolecular motion of mechanical bonds,so the deliberate selection of capping groups is essential for tailoring properties.Herein,we develop an innovative capping strategy for mechanical bonds by employing graphene oxide(GO)as the capping unit,enabling the construction of a new class of mechanically interlocked networks(GOMINs)with enhanced mechanical performance.GOMINs benefit both from the reinforcing effect of GO as a nanofiller and its innovative use as a capping unit that creates continuous mechanical bonds,collectively improving their mechanical strength and adaptability.Compared to the non-interlocked control sample,GOMINs exhibit greater fracture strength(maximum stress:9.4 vs.3.6 MPa),higher toughness(22.3 vs.9.7 MJ/m^(3)),and increased elongation at break(359%vs.328%).Notably,despite these significant enhancements,GOMINs maintain good energy dissipation capacity and thermomechanical stability owing to the constrained intramolecular motion of mechanical bonds.This strategy endows GOMINs with distinctive properties,providing a promising platform for the design of advanced composite materials with enhanced and tunable multifunctionality.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos. 52033011, 52173092 and 51973237)Natural Science Foundation of Guangdong Province(Nos. 2019B1515120038, 2020A1515011276 and 2021A1515010417)+4 种基金Science and Technology Planning Project of Guangzhou City (No. 202201011568)the Talented Program of Guizhou University (No. X2022008)Fundamental Research Funds for the Central Universities,Sun Yat-sen University (No. 23yxqntd002)GBRCE for Functional Molecular Engineering,the Youth Innovation Promotion Association,CAS(No. 2020010)Guangdong Basic and Applied Basic Research Foundation (No. 2021A1515110908)。
文摘Recently, we reported a series of reversibly interlocked polymer networks(RILNs), whose mechanical robustness and functionalities improvement was believed to be derived from topological interlocking of two sub-networks, although the direct evidence for the deduction is still lacking. Herein, a specially-designed RILNs system, in which the inter-component hydrogen bonds can be shielded as needed, was prepared and used to study the micro-structures of RILNs, aiming to verify the existence of mechanical interlocking in RILNs. By changing the pH of the swelling solvent, the effect exerted by the inter-component non-covalent bonds was eliminated, so detailed information of the networks structure was exposed. The small angle X-ray scattering(SAXS) and small-angle neutron scattering(SANS) results indicated that swelling-induced structural evolution of the two sub-networks mutually affected each other, even when the inter-component hydrogen bonds were absent, proving the presence of topological interlocking. The findings may help to draw a more accurate physical image and reveal the detailed structureproperty relationship of RILNs.
基金support of the NSFC/China(22471164 and 52421006)the Shanghai Municipal Science and Technology Major Project,the NSF of Shanghai(22dz1207603)+5 种基金State Key Laboratory of Polyolefins and Catalysis and Shanghai Key Laboratory of Catalysis Technology for Polyolefins(SKL-LCTP-202301)Z.F.acknowledges the financial support of the China Postdoctoral Science Foundation(2024M761944).Z.acknowledges the financial support of Outstanding Doctoral Graduates Development Scholarship of Shanghai Jiao Tong University(SJTU Grants)Y.W.acknowledges the financial support of the NSFC/China(52403162)Z.Z.acknowledges the financial support of the NSFC/China(22475128 and 52333001)C.W.acknowledges the financial support of the NSFC/China(22505153).
文摘Mechanically interlocked networks(MINs)provide a versatile platform for engineering materials that combine mechanical strength with dynamic adaptability.Their performance hinges on the constrained intramolecular motion of mechanical bonds,so the deliberate selection of capping groups is essential for tailoring properties.Herein,we develop an innovative capping strategy for mechanical bonds by employing graphene oxide(GO)as the capping unit,enabling the construction of a new class of mechanically interlocked networks(GOMINs)with enhanced mechanical performance.GOMINs benefit both from the reinforcing effect of GO as a nanofiller and its innovative use as a capping unit that creates continuous mechanical bonds,collectively improving their mechanical strength and adaptability.Compared to the non-interlocked control sample,GOMINs exhibit greater fracture strength(maximum stress:9.4 vs.3.6 MPa),higher toughness(22.3 vs.9.7 MJ/m^(3)),and increased elongation at break(359%vs.328%).Notably,despite these significant enhancements,GOMINs maintain good energy dissipation capacity and thermomechanical stability owing to the constrained intramolecular motion of mechanical bonds.This strategy endows GOMINs with distinctive properties,providing a promising platform for the design of advanced composite materials with enhanced and tunable multifunctionality.
