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pH2ae_Fw_BorgesDeAvila2026_ACS-AEM.pdf
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Abstract
K-ion intercalation in Prussian blue analogues (PBAs) is a well-established charge storage mechanism in potassium-ion batteries; here, we demonstrate that this process also responsible for nanoscale resistive switching in PBA-based material. Using conductive atomic force microscopy (C-AFM), we directly visualize and electrically control reversible conductance modulation within sub-100 nm volumes, linking localized K + redistribution to Fe 2+ /Fe 3+ redox reconfiguration. The switching is polarity-selective, with Prussian white (PW) and Prussian blue (PB) both exhibiting unidirectional resistive switching (URS) at opposite bias polarities, consistent with oxidation-and reduction-driven transport, respectively. These processes are governed by electrically confined ion−electron coupling, where K-ion motion modulates small-polaron hopping within the PBA framework. The switching dynamics are strongly dependent on ionic mobility, with PW sustaining operation up to 200 V/s and PB up to 50 V/s, highlighting the critical role of K-ion concentration in enabling fast redox kinetics. This nanoscale switching mechanism, combined with spatial confinement below 100 nm, enables high-density device integration without interference between them. Moreover, PBAs provide a chemically versatile, earth-abundant platform with tunable ionic and electronic properties, fabricated via a single-step, aqueous, room-temperature process compatible with CMOS technology. This solution-processable approach enables low-temperature fabrication, scalability to large-area substrates, and integration into diverse device architectures. The use of simple salt precursors ensures low-cost manufacturing, while environmentally friendly synthesis and nontoxic, noncontaminating disposal enhance overall sustainability. KEYWORDS: nanoscale resistive switching, Prussian blue analogs, metal−organic framework materials, ion intercalation ■ INTRODUCTION With the rapid expansion of big data and artificial intelligence, the demand for computing technologies capable of delivering high processing speed and low energy consumption has grown dramatically, especially for tasks such as pattern recognition, real-time image processing, and autonomous decision-making. 1−3 However, modern computing still relies predominantly on the traditional von Neumann architecture, in which memory and processing units are physically separated. This structural distinction imposes a severe bottleneck on data throughput and leads to substantial energy losses during frequent memory access. 4−6 In contrast, the human brain performs computation in a massively parallel fashion through densely interconnected networks of neurons and synapses, achieving remarkable efficiency with only a few tens of watts of power consumption. 7,8 Memristive devices whose conductance can encode a synaptic weight, offer a promising route toward hardware systems that emulate synaptic plasticity and neural information processing. 9−12 Multiple switching mechanisms have been employed to reproduce biological functionality, including conductive filament formation, phase transitions, magnetization switching, and ion migration. 13−16 Among these, ion migration-based memristors are especially attractive because their operation closely mimics the ionic dynamics of biological synapses,
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Borges de Avila Junior, L., de Leuze, O., Pohlitz, M., Villena, M., Torres-Cavanillas, R., Ducarme, C., Lopes Temporao, A., Coppee, T., Moureaux, A., Arib, S., Coronado, E., Müller, C., Roldán, J., Hackens, B., & Abreu Araujo, F. (2026). Nanoscale Resistive Switching in Electrodeposited MOF Prussian Blue Analogs Driven by K-Ion Intercalation Probed by C-AFM. ACS Applied Electronic Materials, 8(15), 6614-6624. https://doi.org/10.1021/acsaelm.6c00766 (Original work published 2026)