Vanadium atom modulated electrocatalyst for accelerated Li-S chemistry

Extensive efforts have been made to attain practically viable Li-S batteries. Nevertheless, issues mainly pertaining to the notorious polysulfide shuttle and the sluggish sulfur redox kinetics remain in enhancing the energy density and cycling lifespan of batteries. Herein, we propose an atom-level modulation engineering strategy to design a new model electrocatalyst of V-N-C delicately integrating twinborn isolated vanadium atoms and ultra small-sized vanadium nitride (VN) nanoparticles in a carbonaceous framework for Li-S chemistry. Combining results from synchrotron X-ray three-dimensional nano-computed tomography (X-ray 3D Nano-CT), operando Raman and first-principles calculations, we conclude that, such a V-N-C electrocatalyst system synergizes the merits of highly efficient single atom V-N-C coordination (SAV-N-C) as well as site-rich VN centers, and thus effectively promotes both the formation and decomposition of Li2S during discharge and charge procedures, respectively. As a result, the highly active V-N-C electrocatalyst can enable superior rate capability and long-term cycling stability with a low decay of 0.052% per cycle up to 1000 cycles at 2 C. Furthermore, the designed S/V-N-C cathode still affords favorable electrochemical performances even under the scenarios of elevated sulfur loading (8.1 mg cm(-2)) and flexible pouch cell configurations, holding great promise in future practical implementation.