Three-Dimensional MOFs@MXene Aerogel Composite Derived MXene Threaded Hollow Carbon Confined CoS Nanoparticles toward Advanced Alkali-Ion Batteries

Abstract MXene combining high metal-like conductivity, high hydrophilicity, and abundant surface functional groups has been recognized as a class of versatile two-dimensional materials for many applications. However, the aggregation of MXene nanosheets from interlayer van der Waals force and hydrogen bonds represents a major problem that severely limits their practical use. Here, we report an aerogel structure of MOFs@MXene, in which the in situ formed MOF particles can effectively prevent the accumulation of MXene, enabling a three-dimensional (3D) hierarchical porous conductive network to be composed with an ultralight feature. Subsequently, a 3D porous MXene aerogel threaded hollow CoS nanobox composite ((CoS NP@NHC)@MXene) derived from the MOFs@MXene aerogel precursor was synthesized, and the highly interconnected MXene network and hierarchical porous structure coupled with the ultrafine nanocrystallization of the electrochemically active phase of CoS yield the hybrid system with excellent electron and ion transport properties. Benefiting from the synergistic effect of the components, the (CoS NP@NHC)@MXene composite manifests outstanding electrochemistry properties as electrode materials for all of the lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), and potassium-ion batteries (PIBs). It demonstrated the excellent cycle stability and high capacities of 1145.9 mAh g–1 at 1 A g–1 after 800 cycles and 574.1 mAh g–1 at 5 A g–1 after 1000 cycles for LIBs, 420 mAh g–1 at 2 A g–1 after 650 cycles for SIBs, and 210 mAh g–1 at 2 A g–1 after 500 cycles for PIBs. First-principle calculations confirmed that the (CoS NP@NHC)@MXene hybrid could enhance the charge transfer reaction kinetics, particularly at the interface. More importantly, the excellent rate performance under high mass loading and the high volumetric energy and power density of the entire electrode represent the potential of (CoS NP@NHC)@MXene composites for applications to practical electrochemical energy storage devices. The synthesis method reported in this Article is versatile and can be easily extended to produce other porous MXene-aerogel-based materials for various applications.