Active-material microenvironment engineering by plasticine electrode matrix for shape-customizable Li-ion batteries

Abstract

The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology. However, this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions, robust interface adhesion, and, crucially, the suitable rheological properties required for on-demand shaping. In this work, we introduce a concept of a multifunctional plasticine electrode matrix (PEM) featuring nano-interpenetrating networks (nano-IPN) to address this challenge. Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials, we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction, component binding, non-flammability, and plasticine-like moldability. With this PEM, we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material (AM) (>70 wt %) using industry-friendly extrusion and compression molding techniques. Moreover, these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility, remaining structurally intact even under severe mechanical stress. Ultimately, we have successfully produced shape-patternable and flexible batteries via extrusion molding. This study underscores the potential of the PEM to revolutionize battery microstructures, interfaces, manufacturing processes, and performance characteristics.