Abstract
Regulating the adsorption and dissociation equilibrium of electrocatalytic materials towards lithium polysulfides (LiPS) is a crucial yet challenging step in achieving efficient conversion and utilization of LiPS. To address this, we employed theoretical calculations and designed a carbon hollow cage (CHC) structure embedded with nano-heterostructure particles of Co9S8/Ni3S4, leveraging the dual interaction of strong adsorption from Co9S8 and high catalysis from Ni3S4. Theoretical simulations demonstrated that Co9S8, acting as an electron acceptor, forms a built-in electric field with Ni3S4, enhancing intrinsic conductivity and optimizing electron cloud structure. The Co9S8/Ni3S4 heterostructure regulated the adsorption and dissociation capabilities of LiPS, lowering Gibbs free energy. Simultaneously, three-dimensional computed tomography (3D-CT) found that the skeleton of the electrode sheet was stable before and after cycling and effectively alleviated the sulfur volume change. Multiple in-situ characterization techniques validated the in-situ phase transformation of sulfur-active materials, confirming the outstanding reversibility of the Co9S8/Ni3S4@CHC/S cathode. Especially under the high current of 5C, the capacity decay rate is only 0.021 % after 400 cycles. These findings indicate that the nano-heterostructure regulates the balance of adsorption and dissociation of LiPS, offering new insights into the control and mechanism of nano-heterostructure electronic structures.
Published Version
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