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<p>Supramolecular helical architectures hold immense promise for enantioselective catalysis. Nevertheless, the role of screw pitch, a critical structural parameter governing spatial asymmetry, remains underexplored in this aspect. To address this gap, herein, 5-aminoisophthalic acid dimer (DAIPA)-based right-/left-handed helical nanoribbons (<i>P</i>/<i>M</i>-DAIPA) were constructed. Through an alcohol-mediated self-assembly strategy, the average screw pitch of <i>P</i>/<i>M</i>-DAIPA can be tuned across a broad range of 360–3152 nm. Mechanistic study reveals that hydrogen-bonding interactions between DAIPA, modulated by alcohol identity and alcohol/H<sub>2</sub>O ratios, dictate helical morphology and varied screw pitch. Upon encapsulation of Fe<sub>3</sub>O<sub>4</sub> nanoparticles, the <i>P</i>-DAIPA-Fe<sub>3</sub>O<sub>4</sub> nanozyme shows higher catalytic efficiency toward S-3,4-dihydroxyphenylalanine (DOPA). The <i>M</i>-DAIPA-Fe<sub>3</sub>O<sub>4</sub> nanozyme demonstrates favorable catalysis toward <i>R</i>-DOPA. More importantly, the catalytic enantioselectivity exhibits a striking inverse correlation with screw pitch, achieving selectivity factors ranging from 1.52 to 2.01. Experimental evidence proves that the shorter the screw pitch, the higher the adsorption enantioselectivity of <i>R</i>/<i>S</i>-DOPA on <i>M</i>/<i>P</i>-DAIPA-Fe<sub>3</sub>O<sub>4</sub>, offering critical mechanistic insight into screw pitch-dependent asymmetric catalysis. Overall, our work not only deciphers solvent-driven control toward supramolecular screw pitch but also establishes a universal framework for engineering chiral nanozymes with tunable enantioselectivity, advancing the frontier of enantioselective synthesis.</p>

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Chiral supramolecular helical nanozymes with tunable screw pitch and catalytic enantioselectivity

  • 期刊论文

  • 发表日期：

    2026年1月29日

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  • Mendi Bkhit Nill Khamis,
  • Xiaohuan Sun,
  • Pengyuan Hang,
  • Shixin Li,
  • Jie Han

摘要

Supramolecular helical architectures hold immense promise for enantioselective catalysis. Nevertheless, the role of screw pitch, a critical structural parameter governing spatial asymmetry, remains underexplored in this aspect. To address this gap, herein, 5-aminoisophthalic acid dimer (DAIPA)-based right-/left-handed helical nanoribbons (P/M-DAIPA) were constructed. Through an alcohol-mediated self-assembly strategy, the average screw pitch of P/M-DAIPA can be tuned across a broad range of 360–3152 nm. Mechanistic study reveals that hydrogen-bonding interactions between DAIPA, modulated by alcohol identity and alcohol/H2O ratios, dictate helical morphology and varied screw pitch. Upon encapsulation of Fe3O4 nanoparticles, the P-DAIPA-Fe3O4 nanozyme shows higher catalytic efficiency toward S-3,4-dihydroxyphenylalanine (DOPA). The M-DAIPA-Fe3O4 nanozyme demonstrates favorable catalysis toward R-DOPA. More importantly, the catalytic enantioselectivity exhibits a striking inverse correlation with screw pitch, achieving selectivity factors ranging from 1.52 to 2.01. Experimental evidence proves that the shorter the screw pitch, the higher the adsorption enantioselectivity of R/S-DOPA on M/P-DAIPA-Fe3O4, offering critical mechanistic insight into screw pitch-dependent asymmetric catalysis. Overall, our work not only deciphers solvent-driven control toward supramolecular screw pitch but also establishes a universal framework for engineering chiral nanozymes with tunable enantioselectivity, advancing the frontier of enantioselective synthesis.