Unlocking the Catalytic Potential of Platinum Single Atoms for Industry‐Level Current Density Chlorine Tolerance Hydrogen Generation

Abstract Immobilizing platinum (Pt) single atoms on appropriate supports with optimized coordination environments and electronic structures is a promising strategy to address the problem of chlorine corrosion during seawater electrolysis. Herein, Pt single atoms on nickel‐vanadium layered double hydroxides (Pt‐SA/NiV‐LDH) matrix are fabricated for chlorine tolerance hydrogen generation. Due to the strong synergetic electronic interaction between atomically dispersed Pt and the ultrathin NiV LDH matrix, the adsorption/dissociation feature of *H₂O, *OH, and *H are optimized as evidenced theoretically. The as‐fabricated Pt‐SA/NiV‐LDH electrode exhibits an exceptional mass activity (i.e., 30.98 times higher) compared to the commercial Pt/C, along with an ultra‐high turnover frequency (TOF) value of 9.90 s⁻¹ in alkaline media. Impressively, only 207 mV overpotential is required to yield a current density of 2000 mA cm^‒2 in an electrolyte solution containing 1 m KOH and 2 M NaCl, indicating its robust resistance to chlorine. Moreover, this kind of material demonstrates remarkably low overpotentials of 130 and 215 mV to attain the industrial‐scale current densities of 1000 and 2000 mA cm⁻² in alkaline seawater, accompanied by exceptional stability for 500 h working at 500 mA cm⁻². This work provides an insightful reference for the production of sustainable green hydrogen through seawater electrolysis.