Lithium-Ion Conducting Self-Assembled Organic Nanowires: Optimizing Mechanical Performance and Ionic Conductivity through Programmable Supramolecular Interactions.

Abstract

Abstract : The emergence of wearable devices has led to a greater need for battery materials that are safe, resilient, exhibit high levels of ionic conductivity. Here, we present a supramolecular design as a useful tactic through fine tuning of the noncovalent interactions to overcome the standard trade-off in solid state Li-ion conductors between ionic conductivity and mechanical resilience. We report solution processable self-assembled organic nanowires (SONs) with varying supramolecular interactions through structural mutation to boost Li-ion conductivity and mechanical integrity. The findings indicate that precise H-bonding plays a crucial role in achieving a maximum Young's modulus (1050.5 ± 38 MPa), and toughness (15666 ± 423 kJ/m³), surpassing the impact of the number of H-bonding sites. Highly structured H-bonded morphology facilitated the creation of binding pockets, enhancing lithiation, in achieving the highest ionic conductivity (3.12 × 10^-4 Scm^-1) with Li-ion transference number of 0.8 at 298 K. The molecular dynamics simulation demonstrates that, among the various interaction sites, the hopping of Li-ions through the axial pathway is favoured over the planar pathway. This study represents a pioneering example illustrating the methodology behind the impact of noncovalent interactions within nanoscale assemblies on the ion conductivity and mechanical characteristics of supramolecular Li-ion conductors.