Non‐Conjugated Dicarboxylate Anode Materials for Electrochemical Cells

Abstract

Classical organic anode materials for Na-ion batteries are mostly based on conjugated carboxylate compounds, which can stabilize added electrons by the double-bond reformation mechanism. Now, 1,4-cyclohexanedicarboxylic acid (C₈ H₁₂ O₄ , CHDA) with a non-conjugated ring (-C₆ H₁₀ -) connected with carboxylates is shown to undergo electrochemical reactions with two Na ions, delivering a high charge specific capacity of 284 mA h g^-1 (249 mA h g^-1 after 100 cycles), and good rate performance. First-principles calculations indicate that hydrogen-transfer-mediated orbital conversion from antibonding π* to bonding σ stabilize two added electrons, and reactive intermediate with unpaired electron is suppressed by localization of σ-bonds and steric hindrance. An advantage of CHDA as an anode material is good reversibility and relatively constant voltage. A large variety of organic non-conjugated compounds are predicted to be promising anode materials for sodium-ion batteries.