Robust silicon/carbon composite anode materials with high tap density and excellent cycling performance for lithium-ion batteries

Abstract

Achieving high density while ensuring structural stability and low volume expansion during cycling remains challenging for Si-based anode materials in lithium-ion batteries (LIBs). Herein, we introduce a novel approach to address this issue by developing high tap-density carbon-coated sub-nano-Si-embedded activated carbon (ACSC) anode materials. The resulting ACSC exhibits an ultra-high true density exceeding 0.99 g cm⁻³ and a Si content of 48 % (abbreviated as ACS_0.48C), leading to an impressive volumetric capacity of 2182 mA h cm⁻³. Despite the high tap density and Si content of ACS_0.48C, the ACS_0.48C/artificial graphite (ACS_0.48C/AG) mixture demonstrates a remarkable capacity retention rate of 97.9 % after 200 cycles at 0.5 C, with a modest volume expansion rate of 7.3 % after 50 cycles. The outstanding electrochemical performance can be attributed to the structural stability of ACS_0.48C throughout cycling. The AC scaffold provides a robust mechanical framework to prevent volume expansion and agglomeration of sub-nano-sized Si particles. Furthermore, the homogeneous mixing of amorphous Si and carbon at the atomic level ensures isotropic expansion, thereby enhancing structural stability. The unique structure of ACS_0.48C, combining high tap density and superior cycling performance, offers a solution to the low tap density issue in nanostructures and introduces innovative concepts for the morphology and structural design of Si/C secondary particles.