Side-Chain Poly[2]rotaxane-Toughened Graphene Films

IF 5.2 Q1 POLYMER SCIENCE

ACS Macro Letters Pub Date : 2025-09-04 DOI:10.1021/acsmacrolett.5c00459

Mengling Yang, Guoquan Liu, Wenbin Wang, Shaolei Qu, Zhiwei Fan, Zhaoming Zhang, Li Yang*, Chunyu Wang* and Xuzhou Yan*,

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Abstract

Graphene-based films are highly valued for their superior conductivity, thermal stability, and mechanical strength, yet their brittleness and low ductility limit their full potential. Current toughening strategies for graphene-based composites mainly focus on interfacial reinforcement between polymers and graphene substrates. However, research on energy dissipation arising from the intrinsic properties of polymers remains limited. Herein, we develop a toughened graphene film (^PRrGO) incorporating side-chain poly[2]rotaxane (PR) bearing anthracene units, where both interfacial reinforcement and intramolecular motion contribute to energy dissipation, greatly upgrading the film’s mechanical properties. Results show that ^PRrGO films exhibit a tensile strength of 183 MPa, strain at break of 20.9%, Young’s modulus of 896 MPa, and toughness of 17.2 MJ/m³, which are 4.27, 2.37, 1.25, and 8.33 times higher than those of original rGO films, respectively, while significantly outperforming conventional polymer-modified graphene films (^CrGO). Molecular dynamics simulations reveal a synergistic toughening mechanism: the intramolecular motion of side-chain [2]rotaxane units and the π–π interactions with graphene nanosheets. This study exploits the application of PRs in graphene engineering and provides unique insights into enhancing the performance of two-dimensional materials.

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侧链聚[2]轮烷增韧石墨烯薄膜。

石墨烯基薄膜因其优异的导电性、热稳定性和机械强度而受到高度重视，但其脆性和低延展性限制了其全部潜力。目前石墨烯基复合材料的增韧策略主要集中在聚合物与石墨烯衬底之间的界面增强。然而，对聚合物固有特性引起的能量耗散的研究仍然有限。在此，我们开发了一种含有侧链聚[2]轮烷（PR）的增韧石墨烯薄膜（PRrGO），其中界面增强和分子内运动有助于能量耗散，大大提高了薄膜的机械性能。结果表明，PRrGO薄膜的抗拉强度为183 MPa，断裂应变为20.9%，杨氏模量为896 MPa，韧性为17.2 MJ/m3，分别是原始rGO薄膜的4.27倍、2.37倍、1.25倍和8.33倍，显著优于传统聚合物改性石墨烯薄膜（CrGO）。分子动力学模拟揭示了一种协同增韧机制：侧链[2]轮烷单元的分子内运动以及与石墨烯纳米片的π-π相互作用。本研究开发了pr在石墨烯工程中的应用，并为提高二维材料的性能提供了独特的见解。

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来源期刊

ACS Macro Letters 化学-

CiteScore

10.40

自引率

3.40%

发文量

209

审稿时长

1 months

期刊介绍： ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science. With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.