is still hindered by some main fundamental obstacles, including the insulating nature of sulfur and lithium sulfides (Li 2 S), and the notorious shuttle effect of lithium polysulfides (LiPSs) intermediates during cycling process. The shuttle effect brings about not only the loss of the active materials but also the anode corrosion, leading to rapid capacity degradation and low Coulombic efficiency. [4,5] Carbon nanomaterials with high electrical conductivity, desirable porous structure, and controlled dimensions have been devoted to the design of sulfur hosts [6][7][8][9][10][11][12][13] or interlayers [14][15][16] to physically restrain LiPSs in the cathode area, however, the weak interactions between nonpolar carbon and polar LiPSs discount the effectiveness during the long-term cycling. Chemical trapping of LiPSs with polar transition metal compounds such as TiO 2 , MnO 2 , etc., via polar-polar interactions is an available approach to mitigate the LiPSs shuttling. [17][18][19][20][21] Nonetheless, when the sulfur content and electrode mass loading are high, the massive generated LiPSs are difficult to be immobilized due to the adsorption saturation by these compounds. The detrimental shuttle effect in lithium-sulfur batteries mainly results from the mobility of soluble polysulfide intermediates and their sluggish conversion kinetics. Herein, presented is a multifunctional catalyst with the merits of strong polysulfides adsorption ability, superior polysulfides conversion activity, high specific surface area, and electron conductivity by in situ crafting of the TiO 2 -MXene (Ti 3 C 2 T x ) heterostructures. The uniformly distributed TiO 2 on MXene sheets act as capturing centers to immobilize polysulfides, the hetero-interface ensures rapid diffusion of anchored polysulfides from TiO 2 to MXene, and the oxygen-terminated MXene surfaceis endowed with high catalytic activity toward polysulfide conversion. The improved lithium-sulfur batteries deliver 800 mAh g −1 at 2 C and an ultralow capacity decay of 0.028% per cycle over 1000 cycles at 2 C. Even with a high sulfur loading of 5.1 mg cm −2 , the capacity retention of 93% after 200 cycles is still maintained. This work sheds new insights into the design of highperformance catalysts with manipulated chemical components and tailored surface chemistry to regulate polysulfides in Li-S batteries.

Aqueous zinc batteries, that demonstrate high safety and low cost, are considered promising candidates for large‐scale energy storage. However, Zn anodes suffer from rapid performance deterioration due to the severe Zn dendrite growth and side reactions. Herein, with a low‐cost ammonium acetate (NH4OAc) additive, a self‐regulated Zn/electrolyte interface is built to address these problems. The NH4+ induces a dynamic electrostatic shielding layer around the abrupt Zn protuberance to make the Zn deposition uniform, and the OAc− acts as an interfacial pH buffer to suppress the proton‐induced side reactions and the precipitation of insoluble by‐products. As a result, in the electrolyte with the NH4OAc additive, Zn anodes exhibit a long cycling stability of 3500 h at 1 mA cm−2, an impressive cumulative areal capacity of 5000 mAh cm−2 at 10 mA cm−2, and a high Coulombic efficiency of ≈99.7%. A prototype full cell coupled with a NH4V4O10 cathode performs much better in terms of capacity retention than the additive‐free case. The findings pave the way for developing practical Zn batteries.