Abstract

Lithium-ion batteries (LIBs) are renowned for their high energy density, long lifespan, and minimal self-discharge, making them a prominent power supply system. However, the persistent demand for improved energy density coupled with mechanical stability remains a significant challenge, as efforts to enhance electrode thickness or achieve geometric complexity through conventional ink-casting methods have yielded limited results. To tackle this challenge, we applied a three-dimensional (3D) printing technique to swiftly construct 3D thick electrodes with ultrahigh mass loading. Combined with unidirectional ice-templating process, high mass loading electrodes with hierarchically porous structures were successfully fabricated. The mass loading of the 3D electrodes can reach up to 73.83 mg cm−2, significantly enhancing the areal capacity. The low tortuosity and good mechanical resilience of these structures enable fast ion and charge transport, leading to significant improvements in areal energy density without sacrificing the power density. The assembled full cell exhibits an impressive areal capacity of 10.34 mAh cm⁻2 at 0.2 C and an excellent energy density of 18.41 mWh cm−2, surpassing other 3D printed lithium-ion batteries. This approach marks a significant advancement in electrode structural design towards higher areal capacity and energy density, showcasing the intriguing potential of 3D printed batteries for practical applications. Additionally, it also highlights the scalability and design versatility provided by 3D printing technique.

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