Surface N Sites Mediate the Formation of Li Metal Cluster@N-Enriched Hierarchically Porous Carbon for Ultrahigh-Capacity Lithium Storage.

Graphite is the popular anode material of current lithium-ion batteries (LIBs). However, its low specific capacity and poor lithium intercalation potential hinder its use for high-power and large-scale energy storage. To meet the demand for energy storage, novel anode materials with high capacity, fast chargeable capability, and long cycle life are of great interest. Herein, we demonstrate an advanced nitrogen-enriched hierarchical porous carbon serving as a lithiophilic anode material for ultrahigh capacity and long-life LIBs. NHPC-700 (under optimal synthetic conditions), featuring a high surface area, rich N-doping, high porosity, and partially graphitized nanosheet structures, is successfully fabricated from a Schiff-base copolymer via a template-incipient wetness impregnation method. NHPC-700 exhibits an ultrahigh reversible lithium storage capacity of 2796 mA h g-1 at 0.1 A g-1 while still maintaining a high capacity of 526 mA h g-1 at 10 A g-1 after 1000 cycles. Theoretical and experimental studies reveal that this remarkable Li storage performance can be attributed to the large number of N lithiophilic sites on the inner surface of the small mesoporous pores. These sites guide Li metal nucleation in the initial period and control well the volume variation during charge/discharge cycles, thus exhibiting excellent cycle stability and great potential for practical application.