Abstract
Metal-ligand interactions are crucial in nature, serving as the fundamental basis for the structure of many proteins in living organisms and the process of photosynthesis in green plants. The unique coordination structures and the diversity of various metals and ligands have inspired many scientists to design numerous functional materials in many fields. In the past few decades, two-dimensional materials have garnered considerable attention in materials design. Their intriguing properties and distinctive structures also provide platforms for the integration and combination of different materials. The integration of two-dimensional materials and the atomically dispersed metals have gained popularity in the field of energy storage and conversion. The evolution from the fossil energy era to the new energy era and the increasing demand for electric vehicles have raised the standards for new energy storage systems beyond lithium-ion battery and, more significantly, for new energy storage materials. Herein, the in-plane integration and out-of-plane integration of two-dimensional materials with atomically dispersed metals are extensively investigated. By utilizing metal-ligand interactions, the coordination structures of metal atoms and the connection between two-dimensional materials are tuned to explore and adapt to different energy storage reactions in different post-lithium-ion battery systems. Different coordination structures of atomic Co in two-dimensional carbon matrix are constructed to compared their adsorption ability of Li-ions and catalytic effect towards Li⁺ to Li⁰ conversion for Li metal batteries. Moreover, the out-of-plane integration of two-dimensional carbon materials and atomically dispersed metals are studied for sodium-ion batteries. The influences of the metal junctions in layer-stacked carbon materials on Na⁺ adsorption/desorption behaviors in carbon anode and electrochemical reactions of conversion-type anode are thoroughly discussed in different sodium-based battery systems. This thesis offers valuable insights into the integration methodologies of two-dimensional materials with atomically dispersed metals, exploring their consequential effects on diverse electrochemical reactions within post-lithium-ion batteries.