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<p>Two bridged core-brominated pyromellitic diimide (BrPMDI) derivatives functionalized with four or two ethylene glycol side chains (BrPMDI-1-B and BrPMDI-2-B) are synthesized and copolymerized with 2-(2-methoxyethoxy)ethyl methacrylate (MEP) and low-coverage polyrotaxane (Pr) to construct supramolecular elastomers with distinct mechano-enhanced or mechanochromic pure phosphorescence. A facile side-chain shortening strategy enables a switch of BrPMDI from a luminescence-quenching to an emissive molecule; that is, BrPMDI-2-B exhibits orange phosphorescence in the solid state, whereas BrPMDI-1-B suffers from luminescence quenching. Single-crystal structural analysis reveals that increased side-chain length strengthens <i>π</i>-<i>π</i> stacking and disrupts intermolecular halogen bonds, leading to luminescence weakening or even quenching. Significantly, the elastomer 5 wt%-BrPMDI-1-B-0.5 wt%Pr shows a 2.2-fold enhancement in green phosphorescence intensity (500 nm) upon stretching, while 5 wt%-BrPMDI-2-B-0.5 wt%Pr undergoes a phosphorescence color transition from orange (600 nm) to green (500 nm). In addition, the bridged architecture not only promotes chromophore aggregation but also endows the elastomers with intrinsic reversible mechanoresponse. Furthermore, Pr incorporation improves the tensile strain of the elastomers by 1.2-fold, facilitating the thorough dispersion of chromophores into a monomolecular state. This work provides novel insights into the molecular design of BrPMDI derivatives and, more importantly, extends stretch-responsive luminescent materials to the realm of pure phosphorescence.</p>

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Polyrotaxane-derived unique supramolecular mechanoresponsive elastomers

  • 期刊论文

  • 发表日期：

    2026年7月28日

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  • Peiao Sun,
  • Jiaqi Liu,
  • Xu Pan,
  • Zhuo Lei,
  • Xiaoyong Yu,
  • Miao Yu,
  • Yulu Zhang,
  • Chen Zhang,
  • Yingming Zhang,
  • Yong Chen,
  • Xuejian Zhang,
  • Yu Liu

摘要

Two bridged core-brominated pyromellitic diimide (BrPMDI) derivatives functionalized with four or two ethylene glycol side chains (BrPMDI-1-B and BrPMDI-2-B) are synthesized and copolymerized with 2-(2-methoxyethoxy)ethyl methacrylate (MEP) and low-coverage polyrotaxane (Pr) to construct supramolecular elastomers with distinct mechano-enhanced or mechanochromic pure phosphorescence. A facile side-chain shortening strategy enables a switch of BrPMDI from a luminescence-quenching to an emissive molecule; that is, BrPMDI-2-B exhibits orange phosphorescence in the solid state, whereas BrPMDI-1-B suffers from luminescence quenching. Single-crystal structural analysis reveals that increased side-chain length strengthens π-π stacking and disrupts intermolecular halogen bonds, leading to luminescence weakening or even quenching. Significantly, the elastomer 5 wt%-BrPMDI-1-B-0.5 wt%Pr shows a 2.2-fold enhancement in green phosphorescence intensity (500 nm) upon stretching, while 5 wt%-BrPMDI-2-B-0.5 wt%Pr undergoes a phosphorescence color transition from orange (600 nm) to green (500 nm). In addition, the bridged architecture not only promotes chromophore aggregation but also endows the elastomers with intrinsic reversible mechanoresponse. Furthermore, Pr incorporation improves the tensile strain of the elastomers by 1.2-fold, facilitating the thorough dispersion of chromophores into a monomolecular state. This work provides novel insights into the molecular design of BrPMDI derivatives and, more importantly, extends stretch-responsive luminescent materials to the realm of pure phosphorescence.