Aqueous Zn‒I₂ batteries based on four-electron conversion chemistry have been extensive explored due to their high voltage and large specific capacity. However, the intrinsic instability of I⁺ generated during the high-voltage conversion process and the severe electrochemical corrosion of Zn anode in aqueous electrolyte primarily hinder the construction of high-performance Zn‒I₂ batteries. Herein, trimethylammonium bromide (TMBr) with functional cation and anion has been selected as a dual-side shielding electrolyte additive to concurrently resolve these problems. On the one hand, Br⁻ in TMBr could incorporate into the electrolyte solvation structure and reconstitute the hydrogen-bond (H-bond) network, suppressing the activity of free H₂O molecules and consequently enhancing the Zn anode stability. On the other hand, the Br⁻ could electrochemically activate I⁺, followed by the stabilization of I⁺ via complexation interactions with trimethylamine cations (TM⁺) and Br⁻, synergistically achieving facile high-voltage conversion chemistry of I₂ cathode. As a result, the TMBr additive enables the four-electron conversion-type Zn‒I₂ batteries to demonstrate a remarkable capacity of 250 mAh g⁻¹ coupled with stable cycling exceeding 15000 cycles at 3 A g⁻¹. Additionally, the 160 mAh pouch cell delivers an energy density of 367.4 Wh kg⁻¹ (based on I₂ mass) with a lifetime of over 300 cycles.

Van der Waals heterostructures made up of different two-dimensional (2D) materials have garnered considerable attention as anodes for lithium-ion batteries (LIBs), and doping can significantly influence their electronic structures and lithium diffusion barriers. In this work, the effects of heteroatom (X = N, O, P, and S) doping in the graphene of the graphene/silicene (G/Si) heterostructure are comprehensively examined by using first-principles calculations. The stacking stability and mechanical stiffness of G/Si and doped G/Si (XG/Si) exhibit that N-doping can improve the structural stability of G/Si, thereby ensuring good cycling performance. The densities of states reveal that the dopants (N, O, and S) can greatly increase the electronic conductivity of G/Si. Importantly, the adsorption and diffusion behaviors of Li are primarily affected by the dopant and the doping site, resulting in ultrafast Li diffusivity. Therefore, N-doped G/Si at doping site 1 (S1) shows a good and balanced property, which exhibits high potential to enhance the electrical performance of G/Si materials and offers a reference for selecting dopants in other 2D anode materials for LIBs.