Core@shell-structured nanomaterials as catalytic electrodes for rechargeable lithium–based batteries

Abstract

This thesis reports the experimental and theoretical investigations on a promising type of electrocatalytic nanomaterials (i.e., electrocatalysts), featuring different configurations of core@shell structure and physicochemical properties. It also presents the development of the nanomaterials into novel catalytic electrodes and their rechargeable lithium (Li)-based batteries. The nanomaterials, catalytic electrodes, and Li-based batteries under study include: (1) FeSn2@C nanocapsules, having a FeSn2 stannide alloy nanoparticle core coated by a carbon onion-like layer shell, as an improved electrocatalytic anode for lithium-ion batteries (LIBs); and (2) Mn3O4@C mesoporous multihollow microspheres, having a Mn3O4 manganese oxide nanoparticle-assembled hollow microsphere core coated by a carbon spongy-like layer shell, as an enhanced electrocatalytic cathode for lithium-oxygen batteries (LOBs). The introduction of the specific configurations of the core@shell structure aims to inspire an interesting and appropriate set of physicochemical properties in the nanomaterials and, hence, higher electrochemical performance in the catalytic electrodes for enabling emerging rechargeable batteries and energy storages. Proposals of the theoretical formation mechanism of materials are suggested by adopting the observations of the physicochemical properties. Through establishing electrochemical models and applying scientific computations, the experimental observations are analysed, and the underlying reaction mechanisms are revealed. The original work, findings, and contributions are summarised in the 'Contributions' section.