Lithium–sulfur (Li–S)
and sodium–sulfur (Na–S)
batteries, with the advantages of ultrahigh energy density, natural
abundance, and ecofriendliness, are regarded as next-generation rechargeable
batteries. However, polysulfide shuttling and sluggish charging/discharging
kinetics in sulfur cathodes severely hamper their practical applications.
In this study, via employing first-principles calculations, we investigate
two-dimensional ferroelectric In2Se3 as a promising
additive to overcome these obstacles. Our studies reveal the following
findings: (1) the In2Se3 monolayer has a modest
adsorption strength to soluble polysulfides, which not only eliminates
the notorious shuttle effect but also prevents polysulfide dissolution;
(2) In2Se3 is able to significantly reduce the
free energy barriers of sulfur reduction reaction and the decomposition
barriers of Li2S and Na2S, thus greatly enhancing
the charging and discharging efficiency; and (3) due to the strong
binding ability, the polarization downward (P↓) surface always
outperforms the polarization upward (P↑) surface during charging/discharging
processes, enabling the effective control of battery performance by
ferroelectric switching. Given these advantages, it is expected that
ferroelectric In2Se3 and similar ferroelectric
additives will open a new route to enhance Li–S and Na–S
battery performance.