Using the earth-abundant natural biomaterials to manufacture functional electronic devices meets the sustainable requirement of green electronics, especially for the practical application of memristors in data storage and neuromorphic computing. However, the sneak currents flowing though the unselected cells in a large-scale cross-bar memristor array is one of the major problems which need to be tackled. The self-selecting memristors can solve the problem to develop compact and concise integrated circuits. Here, a sustainable natural biomaterial (anthocyanin, C15H11O6) extracted from plant tissue is demonstrated for ions and electron transport. The capacitive-coupled memristive behavior of as-prepared bioelectronic device can be significantly modulated by diethylmethyl(2-methoxyethyl)ammoium bis(trifluoromethylsulfonyl)imide (DEME-TFSI) ionic liquid (IL). Furthermore, graphene was inserted into biomaterial matrix to manipulate the memristive effects by graphene protonation. This results in a battery-like self-selective memristive effect. This phenomenon is explained by a physical model and density functional theory (DFT) based first-principles calculations. Finally, the self-selective behavior was applied in 0T-1R array configuration, which indicates the battery-like self-selecting biomemristor has potential applications in the brain-inspired computing, data storage systems, and high-density device integration.
Keywords: artificial intelligence; biomemristor; graphene protonation; ionic liquid; resistive switching; self-selecting.