Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in Li-S Batteries.

ABSTRACT: Spin-engineering with electrocatalysts have been exploited to suppress the "shuttle effect" in Li-S batteries. Spin selection, spin-dependent electron mobility and spin potentials in activation barriers can be optimized as quantum spin exchange interactions leading to a significant reduction of the electronic repulsions in the orbitals of catalysts. Herein, we anchor the MgPc molecules on fluorinated carbon nanotubes (MgPc@FCNT), which exhibits the single active Mg sites with axial displacement. According to the density functional theory calculations, the electronic spin polarization in MgPc@FCNT not only increases the adsorption energy toward LiPSs intermediates but also facilitates the tunneling process of electron in Li-S batteries. As a result, the MgPc@FCNT provides an initial capacity of 6.1 mAh cm^-2 even when the high sulfur loading is 4.5 mg cm^-2, and still maintains 5.1 mAh cm^-2 after 100 cycles. This work provides a new perspective to extend the main group single-atom catalysts enabling high-performance Li-S batteries.

SUBMITTER: Du Y 

PROVIDER: S-EPMC10825106 | biostudies-literature | 2024 Jan

REPOSITORIES: biostudies-literature