The effects of a biomass-derived hard carbon matrix and a sustainable cross-linked binder are investigated as electrode components for a silicon-based anode in lithium-ion half-cells, in order to reduce the capacity fade due to volume expansion and shrinkage upon cycling. Ex situ Raman spectroscopy and impedance spectroscopy are used to deeply investigate the structural and interfacial properties of the material within a single cycle and upon cycling. An effective buffering of the volume changes of the composite electrode is evidenced, even at a high Si content up to 30% in the formulation, resulting in the retention of structural and interfacial integrity. As a result, a high capacity performance and a very good rate capability are displayed even at high current densities, with a stable cycling behavior and low polarization effects.
Keywords: distribution of relaxation times; ex situ Raman spectroscopy; hard carbon; impedance spectroscopy; interfacial characterization; lithium-ion battery; silicon composite anode.