Abstract
Polymer-derived ceramics (PDCs) have risen to prominence for applications in electrochemical energy storage, electromagnetic absorbing, and sensing materials, among others. However, a multitude of critical properties in PDCs are still limited by their intrinsic poor electrical conductivity. Herein, novel vinyl and zirconium-modified polycarbosilane precursors with improved electrical conductivity were synthesized through a Grignard coupling reaction of vinyl magnesium chloride and zirconocene dichloride, followed by the insertion polymerization with dichlorodimethylsilane and sodium. Our findings reveal a complex structural evolution from amorphous ZrO2 to distinct phases like m-ZrO2, t-ZrO2, and ZrC. This transformation significantly impacts the distribution and morphology of free carbon ribbons, influencing the material conductive network and resulting in an enhanced electrical conductivity of 0.28 S cm-1 and reduced bandgap. Through density functional theory analysis, a unique interaction between the energy bands of the carbon ribbons and the native cell is discovered, leading to a narrowed energy bandgap and conductive behavior. This advancement not only offers insight into the material structure-conductivity relationship but also opens new avenues for applications such as lithium battery anodes.
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