Weaving 3D highly conductive hierarchically interconnected nanoporous web by threading MOF crystals onto multi walled carbon nanotubes for high performance Li-Se battery

Abstract Lithium-selenium (Li-Se) battery has attracted growing attention. Nevertheless, its practical application is still impeded by the shuttle effect of the formed polyselenides. Herein, we report in-situ hydrothermal weaving the three-dimensional (3D) highly conductive hierarchically interconnected nanoporous web by threading microporous metal organic framework MIL-68(Al) crystals onto multi-walled carbon nanotubes (MWCNTs). Such 3D hierarchically nanoporous web (3D MIL-68 (Al)@MWCNTs web) with a very high surface area, a large amount of micropores, electrical conductivity and elasticity strongly traps the soluble polyselenides during the electrochemical reaction and significantly facilitates lithium ion diffusion and electron transportation. Molecular dynamic calculation confirmed the strong affinity of MIL-68 (Al) for the adsorption of polyselenides, quite suitable for Li-Se battery. Their hexahedral channels (1.56 nm) are more efficient for the confinement of polyselenides and for the diffusion of electrolytes compared to their smaller triangular channels (0.63 nm). All these excellent characteristics of 3D MIL-68 (Al)@MWCNTs web with suitable confinement of a large amount of selenium and the conductive linkage between MIL-68(Al) host by MWCNTs result in a high capacity of 453 mAh/g at 0.2C with 99.5% coulombic efficiency after 200 cycles with significantly improved cycle stability and rate performance. The 3D MIL-68 (Al)@MWCNTs web presents a good performance in Li-Se battery in term of the specific capacity and cycling stability and also in terms of rate performance compared with all the metal-organic framework (MOF) based or MOF derived porous carbons used in Li-Se battery.