A triple-longitudinal lithiophilic gradient induced uniform lithium deposition

Despite being considered as a superior alternative to traditional batteries, the practical application of lithium metal batteries is limited by the uncontrolled Li deposition. Here, we present a novel approach to prepare three longitudinal lithium-friendly gradient anodes on oxidized carbon cloth (OC/Fe2O3) using a simple and effective electrospray method. The deposition behavior observed in the OC/Fe2O3 is controllable, as it involves a bottom-up deposition process, in contrast to the traditional top deposition behavior, leading to a stable electrochemical performance. In situ XRD confirmed the formation of more lithium nuclei in OC/Fe2O3. Consequently, the lithium plating OC/Fe2O3 (Li@OC/Fe2O3) anode exhibits an excellent stability performance of half battery (over 1000 h at a low overpotential ≈10 mV with a current density of 1 mA cm−2) and full battery assembled with LiFePO4 (LFP) (109 mAh g−1 after 100 cycles at 2C). This versatility of the electrospraying technique allows for its broad applicability to various porous materials, facilitating the loading highly-dispersed gradient nanoarrays with multi-longitudinal metalophile gradient to facilitate the bottom-up deposition of metals, and provides a promising avenue for the advancement of the next generation metal batteries.