Multidimensional Co₃O₄/NiO heterojunctions with rich-boundaries incorporated into reduced graphene oxide network for expanding the range of lithiophilic host

The commercial application of lithium (Li) metal anode is hindered by the growth of Li dendrites. Here, we develop a multidimensional composite structure composed of Co₃O₄/NiO heterojunction particles and reduced graphene oxide (rGO) nanosheets, that allows Li to nucleate and deposit selectively in one direction. Among, two transition metal oxides (TMOs) without lithiophilicity are transformed into lithiophilic species due to the rich phase boundaries and high Li adsorption energies on interfaces, which can provide uniform active sites and reduce nucleation overpotential for Li deposition. Meanwhile, the rGO substrate with high electrical conductivity and large specific surface area can form a conductive network between TMOs and alleviate volume expansion caused by Li deposition. Benefitting from the synergistic effect of the heterojunctions and carbon substrate, the Co₃O₄/NiO-rGO regulates the local current density and enables the dendrite-free Li plating/stripping behavior. At a current density of 1 mA cm⁻², the Li metal anode with the Co₃O₄/NiO-rGO host exhibits remarkable electrochemical performance, consistently maintaining high Coulombic efficiency (>93.8%) over 1000 cycles. Additionally, the full cells matched with LiFePO₄ cathode also display high rate capability of 130 mAh g⁻¹ at 1 C and stable cycling life over 500 cycles.