Mechanistic Insight into Wettability Enhancement of Lithium-Ion Batteries Using a Ceramic-Coated Layer.

The crucial issue of wettability in high-energy-density lithium-ion batteries (LIBs) has not been comprehensively addressed to date. To overcome the challenge, state-of-the-art LIBs employing a ceramic-coated separator improves the safety- and wettability-related aspects of LIBs. Here, we present a mechanistic study of the effects of a ceramic-coated layer (CCL) on electrode wettability and report the optimal position of the CCL in LIBs. The electrolyte wetting was investigated using the multiphase lattice Boltzmann method and electrochemical impedance spectroscopy for capturing the electrolyte-transport dynamics in porous electrodes and impedance spectra in pouch-type LIBs, respectively. Results indicate that the CCL caused the velocity vector to transport the electrolyte further, resulting in an increase in the wetting rate. Moreover, the location of the CCL considerably affected the wettability of the LIBs. This study provides mechanical insight into the design and fabrication of high-performance LIBs by incorporating CCLs.

Nanoarchitectonics of the cathode to improve the reversibility of Li-O2 batteries.

The strategic design of the cathode is a critical feature for high-performance and long-lasting reversibility of an energy storage system. In particular, the round-trip efficiency and cycling performance of nonaqueous lithium-oxygen batteries are governed by minimizing the discharge products, such as Li2O and Li2O2. Recently, a metal-organic framework has been directly pyrolyzed into a carbon frame with controllable pore volume and size. Furthermore, selective metallic catalysts can also be obtained by adjusting metal ions for outstanding electrochemical reactions. In this study, various bimetallic zeolitic imidazolate framework (ZIF)-derived carbons were designed by varying the ratio of Zn to Co ions. Moreover, carbon nanotubes (CNTs) are added to improve the electrical conductivity further, ultimately leading to better electrochemical stability in the cathode. As a result, the optimized bimetallic ZIF-carbon/CNT composite exhibits a high discharge capacity of 16,000 mAh·g-1, with a stable cycling performance of up to 137 cycles. This feature is also beneficial for lowering the overpotential of the cathode during cycling, even at the high current density of 2,000 mA·g-1.

Synergistic nanoarchitecture of mesoporous carbon and carbon nanotubes for lithium-oxygen batteries.

A rechargeable lithium-oxygen battery (LOB) operates via the electrochemical formation and decomposition of solid-state Li2O2 on the cathode. The rational design of the cathode nanoarchitectures is thus required to realize high-energy-density and long-cycling LOBs. Here, we propose a cathode nanoarchitecture for LOBs, which is composed of mesoporous carbon (MPC) integrated with carbon nanotubes (CNTs). The proposed design has the advantages of the two components. MPC provides sufficient active sites for the electrochemical reactions and free space for Li2O2 storage, while CNT forests serve as conductive pathways for electron and offer additional reaction sites. Results show that the synergistic architecture of MPC and CNTs leads to improvements in the capacity (~ 18,400 mAh g- 1), rate capability, and cyclability (~ 200 cycles) of the CNT-integrated MPC cathode in comparison with MPC.