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Crystal structures of $\textrm{CLi}_4$ compounds are explored through\emph{ab} \emph{initio} evolutionary methodology. Phase transition from metalto semimetal and semiconductor, and eventually to insulator with increasingpressure are revealed under pressure. Pressure-induced evolution ofanti-metallization has been described quantitatively by Fermi Surface FillingRatio and electron energy band gap using \emph{ab} \emph{initio} \emph{GW}calculations. Anti-metallization is attributed to the hybrid valence electronsand their repulsion by core electrons into the lattice interstices. Very weakelectron-phonon coupling interactions are found in the metallic phases,resulting in very low superconducting temperature.

Crossover from Metal to Insulator in Dense Lithium-Rich Compound $\textrm{CLi}_{4}$