Tailoring Holey Graphene Architecture with Sulfur‐Doped Oxygen‐Deficient MoO 3 for Synergistic Capacitance Enhancement

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Abstract An eco‐friendly, cost‐effective strategy is demonstrated for developing efficient supercapacitor (SC) electrode by integrating graphene with oxygen‐deficient sulfur‐doped MoO 3 (S‐MoO 3‐x ). Graphene is produced via mechanochemical exfoliation of graphite using sucrose as the milling agent, and is then composited with S‐MoO 3‐x through hydrothermal treatment. Material characterization studies reveal that, during heat treatment, decomposition of sucrose‐derived carbon spheres introduced holes in the graphene sheets, leading to the formation of a S‐MoO 3‐x /holey graphene nanocomposite (S‐MoO 3‐x /HG). Sulfur doping induces oxygen vacancies, enhancing conductivity and electrochemical performance by modifying the electronic structure of Mo active sites, as evident from material characterization studies. Electrochemical measurements in a three‐electrode system are performed to evaluate the capacitance and durability of the S‐MoO 3‐x /HG electrode. An asymmetric SC pouch cell device is fabricated using S‐MoO 3‐x /HG as the anode and pure MoS 2 as the cathode, operating at 1.4 V. The device exhibits a maximum energy density of 36.5 Wh Kg −1 and a power density of 700 W Kg −1 , highlighting its outstanding performance. Notably, the device retains 100% of its capacitance after 15 000 cycles, highlighting its remarkable cycle life and long‐term usability. Additionally, two such asymmetric devices are connected in series to power 15 red and yellow light‐emitting diodes, further demonstrating their practical application in energy storage systems.

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