Atomically dispersed Zn moieties are efficient active sites for accelerating the electrode kinetics of carbons for sodium-ion hybrid capacitors (SIHCs), but the low utilization and symmetric configuration of Zn single-atom… Click to show full abstract
Atomically dispersed Zn moieties are efficient active sites for accelerating the electrode kinetics of carbons for sodium-ion hybrid capacitors (SIHCs), but the low utilization and symmetric configuration of Zn single-atom greatly hamper the Na ion storage capability. Herein, a molecular design strategy is employed to synthesize high-density Zn single atoms with asymmetric Zn-N3 S coordination embedded in nitrogen/sulfur codoped carbon (Zn-N3 S-NSC). The key to this strategy lies in the Zn power-catalyzed condensation of trithiocyanuric acid molecules to generate S-doped g-C3 N4 , which can in situ coordinate with Zn sources to form Zn-N3 S moieties during pyrolysis. By virtue of the highly exposed Zn-N3 S moieties, Zn-N3 S-NSC presents ultrahigh reactivity, efficient electron transfer, and decreased ion diffusion barriers for SIHCs, rendering an impressive energy density of 215 Wh kg-1 and a maximum power density of 15625 W kg-1 . Moreover, the pouch cell displays a high capacity of 279 mAh g-1 after 4000 cycles. This work provides a new avenue for the regulation of the coordination configuration of single metal atoms in carbons toward high-performance electrochemical energy technologies at the molecular level.
               
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