Enhancing the performance of polyoxometalate-based memristors in harsh environments based on hydrogen bonding cooperative π-conjugation interaction

Polyoxometalate (POMs), as a class of structurally well-defined compounds with excellent charge trapping and releasing capabilities, are ideal candidates for high-performance memory devices. However, their performance optimization in conventional environments remains limited. Here, three water-soluble organic-inorganic hybridized POMs-based nonvolatile memory devices are proposed. Pure inorganic POM clusters are assembled with organic ligands by electrostatic and covalent interactions. This approach that modulates the hydrophilicity and stability of the resulting compounds. Structural analysis and two-dimensional correlation infrared spectroscopy (2D-COS-IR) reveal that hydrogen bonding and π-conjugation interactions may influence the performance of POMs-based memristors. The resistive switching (RS) mechanism could be controlled by the synergistic effect of space-charge-limited current and oxygen vacancies. Notably, the FTO/VB3/Ag, modified with hydrogen bonding and constructed with Li+, exhibits rewritable RS behavior and a high ON/OFF current ratio of 2.62 × 104, even at 270 °C and various harsh environments. Additionally, this study is the first example of investigating the dynamics of weak forces in the structure of the device during heating using 2D-COS-IR, and elucidating the mechanisms that memristors enable stable operation at high temperatures. This work explores the relationship between structure and RS performance of the material, proposes a method for designing and enhancing memristor performance at the molecular level, and offers a theoretical foundation for the development of high-performance memory devices for extreme environments.