Sulfur‐Deficient Bismuth Sulfide/Nitrogen‐Doped Carbon Nanofibers as Advanced Free‐Standing Electrode for Asymmetric Supercapacitors

Abstract

The use of free-standing carbon-based hybrids plays a crucial role to help fulfil ever-increasing energy storage demands, but is greatly hindered by the limited number of active sites for fast charge adsorption/desorption processes. Herein, an efficient strategy is demonstrated for making defect-rich bismuth sulfides in combination with surface nitrogen-doped carbon nanofibers (dr-Bi₂ S₃ /S-NCNF) as flexible free-standing electrodes for asymmetric supercapacitors. The dr-Bi₂ S₃ /S-NCNF composite exhibits superior electrochemical performances with an enhanced specific capacitance of 466 F g^-1 at a discharge current density of 1 A g^-1 . The high performance of dr-Bi₂ S₃ /S-NCNF electrodes originates from its hierarchical structure of nitrogen-doped carbon nanofibers with well-anchored defect-rich bismuth sulfides nanostructures. As modeled by density functional theory calculation, the dr-Bi₂ S₃ /S-NCNF electrodes exhibit a reduced OH^- adsorption energy of -3.15 eV, compared with that (-3.06 eV) of defect-free bismuth sulfides/surface nitrogen-doped carbon nanofiber (df-Bi₂ S₃ /S-NCNF). An asymmetric supercapacitor is further fabricated by utilizing dr-Bi₂ S₃ /S-NCNF hybrid as the negative electrode and S-NCNF as the positive electrode. This composite exhibits a high energy density of 22.2 Wh kg^-1 at a power density of 677.3 W kg^-1 . This work demonstrates a feasible strategy to construct advanced metal sulfide-based free-standing electrodes by incorporating defect-rich structures using surface engineering principles.