In Situ Electrophoretic Decorated Cactus-Type Metallic-Phase MoS2 on CaMn2O4 Nanofibers for Binder-Free Next-Generation LIBs

ACS Appl Mater Interfaces. 2024 Apr 10;16(14):17728-17744. doi: 10.1021/acsami.4c03650. Epub 2024 Mar 29.

Abstract

Ternary manganese-based oxides, such as CaMn2O4 (CMO) nanofibers fabricated via the electrospinning technique, have the potential to offer higher reversible capacity through conversion reactions in comparison to that of carbon-based anodes. However, its poor electrical conductivity hinders its usage in lithium-ion batteries (LIBs). Hence, to mitigate this issue, controlled single-step in situ decoration of highly conducting metallic-phase MoS2@CMO nanofibers has been achieved for the first time via the electrophoretic deposition (EPD) technique and utilized as a binder-free nanocomposite anode for LIBs. Further, the composition of MoS2@CMO nanofibers has also been optimized to attain better electronic and ionic conductivity. The morphological investigation revealed that the flakes of MoS2 nanoflowers are successfully and uniformly decorated over the CMO nanofibers' surface, forming a cactus-type morphology. As a binder-free nanocomposite LIB anode, CMOMS-7 (7 wt % MoS2@CMO) demonstrates a specific capacity of 674 mA h g-1 after 60 cycles at 50 mA g-1 and maintains a capacity of 454 mA h g-1 even after 300 cycles at 1000 mA g-1. Further, the good rate performance (102 mA h g-1 at 5000 mA g-1) of CMOMS-7 can be ascribed to the enhanced electrical conductivity provided by the metallic-phase MoS2. Moreover, the feasibility of CMOMS-7 is thoroughly investigated by using a full Li-ion cell incorporating a binder-free cathode of LiNi0.3Mn0.3Co0.3O2 (NMC). This configuration showcases an impressive energy density of 154 Wh kg-1. Thus, the hierarchical and aligned structure of CMO nanofibers combined with highly conductive MoS2 nanoflowers facilitates charge transportation within the composite electrodes. This synergistic effect significantly enhances the energy density of the conversion-based nanocomposites, making them highly promising anodes for advanced LIBs.

Keywords: Mn-based oxides; anode; binder-free electrode; lithium-ion battery; nanocomposite.