Guo Hongshuang, Rautiainen J Mikko, Zeng Hao, Rissanen Kari, Priimagi Arri, Puttreddy Rakesh
Faculty of Engineering and Natural Sciences, Tampere University, P.O. Box 541, Tampere, FI-33101, Finland.
Department of Chemistry, University of Jyvaskyla, P.O. Box 35, Jyväskylä, FI-40014, Finland.
Angew Chem Int Ed Engl. 2025 Jul 21;64(30):e202508101. doi: 10.1002/anie.202508101. Epub 2025 Jun 1.
Supramolecular liquid crystal elastomers (LCEs) incorporating chalcogen bonds (ChBs) have been synthesized and investigated for shape memory and actuation properties. LCEs featuring strong Se⋯N ChBs (-40 to -43 kJ mol) exhibit both shape memory effects (SME) and reversible actuation, while those with weaker S⋯N ChBs (-32 to -34 kJ mol) do not. The Se⋯N-based LCEs transition from one-way to two-way SME after three days at room temperature, enabling programmable 2D/3D shape transformations and rewritable surface patterns. They also enable the fabrication of light-powered crawling robots as well as temperature-responsive knot-like actuators. These results highlight the critical role of the ChB strength and specificity in designing functional materials. Solid-state NMR, Raman spectroscopy, and density functional theory calculations provide further molecular-level insights into ChB interactions, laying the groundwork for advanced supramolecular actuators and shape-morphing LCEs.
已合成并研究了含有硫族元素键（ChBs）的超分子液晶弹性体（LCEs）的形状记忆和驱动性能。具有强Se⋯N硫族元素键（-40至-43 kJ/mol）的LCEs表现出形状记忆效应（SME）和可逆驱动，而具有较弱S⋯N硫族元素键（-32至-34 kJ/mol）的LCEs则不具备这些特性。基于Se⋯N的LCEs在室温下放置三天后从单向形状记忆效应转变为双向形状记忆效应，实现了可编程的二维/三维形状转变和可重写的表面图案。它们还能够制造光驱动的爬行机器人以及温度响应型结状驱动器。这些结果突出了硫族元素键强度和特异性在设计功能材料中的关键作用。固态核磁共振、拉曼光谱和密度泛函理论计算为硫族元素键相互作用提供了进一步的分子水平见解，为先进的超分子驱动器和形状变形LCEs奠定了基础。
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