The Role of Silicon in Silicon-Graphite Composite Electrodes Regarding Specific Capacity, Cycle Stability, and Expansion

Abstract One promising way of compensating for the repeated volume expansion and contraction of silicon as an anode active material in lithium ion batteries (LIBs) is to embed silicon within a graphite matrix. Silicon-graphite (SiG) composites combine the advantageous properties of graphite, i.e., large electrical conductivity and high structural stability, with the advantageous properties of silicon, i.e., high theoretical capacity. Graphite has a much lower volume expansion upon lithiation (≈ 10%) than pure silicon (≈ 300%) and provides a mechanically stable matrix. Herein, we present an investigation into the electrochemical performance and thickness change behavior of porous SiG anode compositions with silicon contents ranging from 0 wt% to 20 wt%. The electrode composites were studied using two methods: in situ dilatometry for the thickness change investigation and conventional coin cells for the assessment of electrochemical performance. The measurements show that the initial thickness change of SiG electrodes increased significantly with the silicon content, but it leveled off during cycling for all compositions. There appears to be a correlation between silicon content and capacity loss, but no clear correlation between thickness change and capacity loss rate was found.