Urea‐Mediated Monoliths Made of Nitrogen‐Enriched Mesoporous Carbon Nanosheets for High‐Performance Aqueous Zinc Ion Hybrid Capacitors

Aqueous zinc ion hybrid capacitors (aZHCs) are of great potential for large-scale energy storage and flexible wearable devices, of which the specific capacity and energy density need to be further enhanced for practical applications. Herein, a urea-mediated foaming strategy is reported for the efficient synthesis of monoliths consisting of nitrogen-enriched mesoporous carbon nanosheets (NPCNs) by prefoaming drying a solution made of polyvinylpyrrolidone, zinc nitrate, and urea at low temperatures, foaming and annealing at high temperatures, and subsequent acid etching. NPCNs have a large lateral size of ≈40 µm, thin thickness of ≈55 nm, abundant micropores and mesopores (≈3.8 nm), and a high N-doping value of 9.7 at.%. The NPCNs as the cathode in aZHCs provide abundant zinc storage sites involving both physical and chemical adsorption/desorption of Zn²⁺ ions, and deliver high specific capacities of 262 and 115 mAh g^-1 at 0.2 and 10 A g^-1 , and a remarkable areal capacity of ≈0.5 mAh cm^-2 with a mass loading of 5.3 mg cm^-2 , outperforming most carbon cathodes reported thus far. Moreover, safe and flexible NPCNs based quasi-solid-state devices are fabricated, which can withstand drilling and mechanical bending, suggesting their potential applications in wearable devices.