Abstract
Phosphorus-carbon anode materials for alkali-metal ion storage in rechargeable batteries can simultaneously achieve high-energy density and fast charging. The P-C-bonded structure in the phosphorus-carbon materials has been observed and acknowledged to be a critical structural feature that renders improved cycling stability and rate performance. However, the underlying mechanisms, especially the role played by P-C bonds, remain elusive. By combining computational simulations and spectroscopic characterizations, we reveal that the stability of P-C bonds is critical to the electrochemical performance. In the discharge process, P-P bonds are fragile, while the bonding state of the P-C bonds is almost unchanged since electrons were mainly received by the P atoms to form lone pairs. The preserved P-C clusters can effectively serve as a reunion center for the recovery of P-P bonds in the recharging process, leading to a moderate energy change and improved cycling reversibility and structural stability of the phosphorous for electrochemical energy storage.
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