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<p>High-performance nonvolatile memory devices are crucial for next-generation computing, yet achieving low-power, stable, and reproducible resistive switching remains challenging, primarily due to stochastic filament formation and limited precise control over the electronic properties of active materials. Herein, we employ a rational molecular engineering strategy to address these limitations by constructing a series of two-dimensional pyrene-based covalent organic frameworks (Py-COFs)—Py-H, Py-CH<sub>3</sub>, and Py-OH—via systematic substitution (−H, −CH<sub>3</sub> and −OH) on the phenyl linkers to modulate backbone electronics. The electron-donating −CH<sub>3</sub> and −OH motifs enrich the π-conjugated backbone with higher electron density, while the −OH moiety in Py-OH further engages in <i>p</i>-π conjugation with the benzene ring and forms intramolecular hydrogen bonds, thereby increasing framework rigidity, enhancing orbital overlap, and promoting charge delocalization. Enabled by these structural refinements, Py-OH-based devices exhibit markedly improved resistive switching behavior, characterized by a low operating voltage, an ON/OFF ratio of ∼10<sup>3.45</sup>, and excellent retention stability. Combined photophysical, electrochemical, and high-resolution TEM analyses corroborate that hydroxyl-driven <i>p</i>-π conjugation, hydrogen-bond reinforcement, and the emergent nanowire-like morphology synergistically suppress uncontrolled filament formation and promote efficient charge transport. These findings established a clear structure-property correlation in functionalized Py-COFs and underscore their promise as tunable active layers for low-power, high-performance resistive memory and neuromorphic computing.</p>

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Hydroxyl-driven p-π resonance in pyrene-based COFs realizes low-power and stable nonvolatile memory devices

  • 期刊论文

  • 发表日期：

    2026年5月6日

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  • Pan-Ke Zhou,
  • Cong Zhang,
  • Chao Lin,
  • Ziyue Yu,
  • Yuxing Huang,
  • Tao Zeng,
  • Xiong Chen

摘要

High-performance nonvolatile memory devices are crucial for next-generation computing, yet achieving low-power, stable, and reproducible resistive switching remains challenging, primarily due to stochastic filament formation and limited precise control over the electronic properties of active materials. Herein, we employ a rational molecular engineering strategy to address these limitations by constructing a series of two-dimensional pyrene-based covalent organic frameworks (Py-COFs)—Py-H, Py-CH3, and Py-OH—via systematic substitution (−H, −CH3 and −OH) on the phenyl linkers to modulate backbone electronics. The electron-donating −CH3 and −OH motifs enrich the π-conjugated backbone with higher electron density, while the −OH moiety in Py-OH further engages in p-π conjugation with the benzene ring and forms intramolecular hydrogen bonds, thereby increasing framework rigidity, enhancing orbital overlap, and promoting charge delocalization. Enabled by these structural refinements, Py-OH-based devices exhibit markedly improved resistive switching behavior, characterized by a low operating voltage, an ON/OFF ratio of ∼103.45, and excellent retention stability. Combined photophysical, electrochemical, and high-resolution TEM analyses corroborate that hydroxyl-driven p-π conjugation, hydrogen-bond reinforcement, and the emergent nanowire-like morphology synergistically suppress uncontrolled filament formation and promote efficient charge transport. These findings established a clear structure-property correlation in functionalized Py-COFs and underscore their promise as tunable active layers for low-power, high-performance resistive memory and neuromorphic computing.