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Here, we report an operando chlorination strategy that harnesses corrosive ions (Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    , SO\n                    <jats:sub>4<\/jats:sub>\n                    <jats:sup>2<\/jats:sup>\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) to self\u2010assemble a renewable catalytic layer on a defective RuIrAg pre\u2010catalyst for highly selective water oxidation. In acidic brine (0.5\u00a0M H\n                    <jats:sub>2<\/jats:sub>\n                    SO\n                    <jats:sub>4<\/jats:sub>\n                    + 3.0 M KCl), it achieves a remarkably low oxygen evolution reaction (OER) overpotential of 108\u00a0mV at 10\u00a0mA cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    , with a full\u2010cell energy consumption of 41.01\u00a0kWh kg\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    H\n                    <jats:sub>2<\/jats:sub>\n                    at 1 A cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    . In seawater containing 0.25\u00a0M Na\n                    <jats:sub>2<\/jats:sub>\n                    SO\n                    <jats:sub>4<\/jats:sub>\n                    , the system ensures exclusive OER, completely suppressing chlorine evolution up to 3.0 A cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    , and demonstrates 200 h of continuous stability at 1 A\u00a0cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    (2.59\u00a0V). Mechanistically, this robust performance stems from Ag\u2010induced frustrated Lewis pairs (FLPs). These continuously regenerating FLPs accelerate OER kinetics via enhanced water activation. Simultaneously, the spatially offset FLPs, synergizing with embedded lattice chlorines and AgCl domains, strictly block Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    chemisorption and dimerization to prohibit Cl\n                    <jats:sub>2<\/jats:sub>\n                    evolution. This work establishes a new paradigm for high\u2010performance electrolysis via operando chlorination and provides a viable route to green hydrogen from direct seawater.\n                  <\/jats:p>","DOI":"10.1002\/adma.75268","type":"journal-article","created":{"date-parts":[[2026,10,6]],"date-time":"2026-10-06T05:35:23Z","timestamp":1791264923000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Operando Chlorination Engineering in PEMWE for Direct Brine Electrolysis to Produce Green Hydrogen"],"prefix":"10.1002","author":[{"given":"Xu","family":"Ren","sequence":"first","affiliation":[{"name":"National Engineering Research Center for Fuel Cell and Hydrogen Source Technology Beijing Key Laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical Technology  Beijing 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