Issue 34, 2024

Exploring the role of viologen and iodocuprate in the enhanced resistive switching performance of Anderson polyoxometalate-based three-component hybrids

Abstract

Polyoxometalate (POM)-based materials are ideal candidates for implementing molecular memories, and rational POM molecule design is key to higher resistive switching (RS) performance. In this work, in order to obtain a deep structure–property correlation of POM-based memristors, three Anderson-based hybrids, i.e. two-component hybrids (MV)3(MnMo6O18L2)2·4DMF (1) and (MV)2[Cu(DMF)2](MnMo6O18L1)2·6DMF (2), and the three-component one (MV)2(Cu2I3)(MnMo6O18L2)·4CH3CN (3) (L = 2-(hydroxymethyl)-2-(pyridine-4-yl)-1,3-propanediol) have been structurally determined. These hybrids together with the precursors (methyl viologen (MV2+), CuI, and (MnMo6O18L2)) were further fabricated as memristors with the structure of ITO/active layer/Ag. Interestingly, three precursors are RS silent or have bad RS performance, but the incorporation of MV2+ in 1 and 2 can trigger the RS performances, and the further decoration of iodocuprate in 3 can render enhanced RS behavior (ON/OFF ratio: 2.32 × 102) with high thermal-tolerance temperature (240 °C) and extremely long-term stability. The RS mechanism could be assigned to the valence change (VC) induced by oxygen vacancy migrations. The presence of air-stable (MnMo6O18L2)3−-MV2+ donor–acceptor couples can stabilize the oxygen vacancies, which not only trigger the RS behaviors in ITO/1/Ag and ITO/2/Ag, but also result in extremely long-term stability in ITO/3/Ag. Besides, the oxygen vacancies can also be stabilized by Cu2I3 with intense cuprophilic interactions, which corresponds to enhanced RS properties in ITO/3/Ag. This mechanism could be validated by the following structural characters in 3: the stronger POM-MV2+ interactions, the better planarity of MV2+, the very short Cu⋯Cu distances and the ABAB-type packing fashion. The structure–property correlation in this work can provide a new strategy for the development of highly efficient and reliable memristors.

Graphical abstract: Exploring the role of viologen and iodocuprate in the enhanced resistive switching performance of Anderson polyoxometalate-based three-component hybrids

Supplementary files

Article information

Article type
Paper
Submitted
27 May 2024
Accepted
15 Jul 2024
First published
18 Jul 2024

J. Mater. Chem. C, 2024,12, 13555-13561

Exploring the role of viologen and iodocuprate in the enhanced resistive switching performance of Anderson polyoxometalate-based three-component hybrids

H. Chen, M. He, T. Li, C. Deng, H. Xiao, M. Qi, X. Kong, H. Li, X. Li and S. Zheng, J. Mater. Chem. C, 2024, 12, 13555 DOI: 10.1039/D4TC02172J

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