Lithium Sulfur (Li/S) chemistries are amongst the most promising next-generation battery technologies due to their high theoretical energy density. However, the detrimental effects of their intermediate byproducts, polysulfides (PS), have to be resolved to realize these theoretical performance limits. Confined approaches on using porous carbons to entrap PS have yielded limited success. In this study, we deviate from the prevalent approach by introducing catalysis concept in Li/S battery configuration. Engineered current collectors were found to be catalytically active towards PS, thereby eliminating the need for carbon matrix and their processing obligatory binders, additives and solvents. We reveal substantial enhancement in electrochemical performance and corroborate our findings using a detailed experimental parametric study involving variation of several kinetic parameters such as surface area, temperature, current rate and concentration of PS. The resultant novel battery configuration delivered a discharge capacity of 700 mAh g⁻¹ with the two dimensional (2D) planar Ni current collectors and an enhancement in the capacity up to 900 mAh g⁻¹ has been realized using the engineered three dimensional (3D) current collectors. The battery capacity has been tested for stability over 100 cycles of charge-discharge.

Suppressing Li dendrite growth has gained research interest due to the high theoretical capacity of Li metal anodes. Traditional Celgard membranes which are currently used in Li metal batteries fall short in achieving uniform Li flux at the electrode/electrolyte interface due to their inherent irregular pore sizes. Here, the use of an ultrathin (≈1.2 nm) carbon nanomembrane (CNM) which contains sub‐nanometer sized pores as an interlayer to regulate the mass transport of Li‐ions is demonstrated. Symmetrical cell analysis reveals that the cell with CNM interlayer cycles over 2x longer than the control experiment without the formation of Li dendrites. Further investigation on the Li plating morphology on Cu foil reveals highly dense deposits of Li metal using a standard carbonate electrolyte. A smoothed‐particle hydrodynamics simulation of the mass transport at the anode–electrolyte interface elucidates the effect of the CNM in promoting the formation of highly dense Li deposits and inhibiting the formation of dendrites. A lithium metal battery fabricated using the LiFePO₄ cathode exhibits a stable, flat voltage profile with low polarization for over 300 cycles indicating the effect of regulated mass transport.