Heteroatom(S) (N, S, P) Co‐Doped Reduced Graphene Oxide‐Based Binder‐Free Novel Energy Storage Electrode Material for High Energy Density Supercapacitor

Abstract This manuscript reports a one‐pot synthesis of ternary heteroatoms (N/S/P) co‐doped reduced graphene oxide as an electrode material by simultaneous reduction/doping of/into graphene oxide employing eco‐friendly natural molecule(s) (thiamine monophosphate (TM) and thiamine pyrophosphate (TP)) under mild heating (≤60 °C) and near‐neutral pH (≤8) conditions. It produces N, S, P co‐doped rGO‐TM and N, S, P co‐doped rGO‐TP nanohybrids displaying a well‐connected porous microstructure with significantly doped atomic(%) ‐N (10.0%), S (4.1%), P (0.1%) and N (6.7%), S (2.0%), and P (0.5%), respectively. The symmetric supercapacitor designed using N, S, P‐rGO‐TM‐10 in water‐in‐salt 17 m NaClO₄ electrolyte exhibits stable cell voltage of 3.0 V, superb gravimetric energy density (areal energy density) of 47.9 Wh kg⁻¹@522.8 W g⁻¹ (0.2363 Wh cm⁻²@ 2.5 W cm⁻²); the excellent cyclic stability (88.8 %) and Coulombic efficiency (99.2%) even after 20 000 cycles. Their energy storage capability is corroborated by the illumination of 109 white LEDs upon lighting a single SSC for 50 s each, driving a motor to run a fan, and forming the tandem device by joining three such cells in series.