Hydrogen-bond-driven neuron-mimic hierarchical heterostructures for fast lithium-ion storage.

Two-dimensional (2D) materials have attracted increasing interest as battery electrode materials due to their short ion diffusion pathways and large surface areas. However, their high aspect ratio leads to reduced ion mobility within the electrolyte-filled pores, and the stacking effect further impedes ion diffusion, thereby limiting their performance in fast-charging applications. It is imperative to expedite the transport of lithium ions into the interior of 2D materials to surmount this limitation. In this study, we present a neuron-mimic heterostructure that has been constructed via a hydrogen bond-driven assembly of functionalized carbon nanotubes (OCNTs) with 2D graphdiyne oxide (GDYO). In this configuration, OCNTs act as both a Li+ reservoir and a pump, simultaneously boosting ion transport/diffusion and lowering the desolvation and charge-transfer barriers. This facilitates the rapid access of Li+ to the entirety of the GDYO electrode during cycling. Leveraging its neuron-like architecture, the composite anode delivers high-rate capability, ultra-long cyclability, and reliable operation across extreme temperatures. It is noteworthy that, at low temperatures as low as -20 °C, a stable capacity of 314.1 mAh g-1 can still be achieved after 3000 cycles at a current density of 2 A g-1. Inspired by the structural and functional characteristics of neurons, this biomimetic design provides a structural strategy for improving ion transport kinetics in 2D-material-based lithium-ion storage electrodes, offering a promising solution for enhancing the efficiency and reliability of energy storage devices.