Upcycling of Spent LiFePO4 Cathodes to Heterostructured Electrocatalysts for Stable Direct Seawater Splitting

Abstract The pursuit of carbon‐neutral energy has intensified the interest in green hydrogen production from direct seawater electrolysis, given the scarcity of freshwater resources. While Ni‐based catalysts are known for their robust activity in alkaline water oxidation, their catalytic sites are prone to rapid degradation in the chlorine‐rich environments of seawater, leading to limited operation time. Herein, we report a Ni(OH) 2 catalyst interfaced with laser‐ablated LiFePO 4 (Ni(OH) 2 /L‐LFP), derived from spent Li‐ion batteries (LIBs), as an effective and stable electrocatalyst for direct seawater oxidation. Our comprehensive analyses reveal that the PO 4 3− species, formed around L‐LFP, effectively repels Cl − ions during seawater oxidation, mitigating corrosion. Simultaneously, the interface between in situ generated NiOOH and Fe 3 (PO 4 ) 2 enhances OH − adsorption and electron transfer during the oxygen evolution reaction. This synergistic effect leads to a low overpotential of 237 mV to attain a current density of 10 mA cm −2 and remarkable durability, with only a 3.3 % activity loss after 600 h at 100 mA cm −2 in alkaline seawater. Our findings present a viable strategy for repurposing spent LIBs into high‐performance catalysts for sustainable seawater electrolysis, contributing to the advancement of green hydrogen production technologies.