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However, comprehensive studies addressing how cation substitution influences surface chemistry and governs OER activity and durability in chromite spinels remain limited. Here, a systematic investigation of the multicationic chromite series Ni\n                    <jats:sub>x<\/jats:sub>\n                    Fe\n                    <jats:sub>y<\/jats:sub>\n                    Cr\n                    <jats:sub>3\u2212x\u2212y<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    is presented, identifying composition\u2010dependent Lewis acidity as a descriptor of superior OER performance. It is further demonstrated that tuning surface acidity directly controls dynamic reconstruction processes and lattice\u2010oxygen participation during spinel\u2010based electrocatalysis. Following activation, the optimized Ni\n                    <jats:sub>0<\/jats:sub>\n                    .\n                    <jats:sub>8<\/jats:sub>\n                    Fe\n                    <jats:sub>0<\/jats:sub>\n                    .\n                    <jats:sub>3<\/jats:sub>\n                    Cr\n                    <jats:sub>1<\/jats:sub>\n                    .\n                    <jats:sub>9<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    catalyst delivers a current density of 10\u00a0mA\u00a0cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at an overpotential of 235\u00a0mV, surpassing RuO\n                    <jats:sub>2<\/jats:sub>\n                    , with excellent long\u2010term stability. Integrating microscopic and spectroscopic analysis with operando impedance spectroscopy, it shows that activation generates an oxyhydroxide overlayer and reveals a previously unrecognized link between surface Lewis acidity and the growth kinetics and activity of these shells. Density functional theory calculations indicate that Fe incorporation at octahedral sites raises the O\u00a02p\u2010band center and lowers oxygen\u2010vacancy formation energy, promoting lattice\u2010oxygen activation and triggering reconstruction, yielding enhanced OER. This work integrates cation\u2010driven surface\u2010acidity modulation, acidity\u2010governed reconstruction, and OER activity enhancement into a unified predictive framework for designing earth\u2010abundant spinel\u2010based catalysts.\n                  <\/jats:p>","DOI":"10.1002\/smll.202508245","type":"journal-article","created":{"date-parts":[[2025,9,27]],"date-time":"2025-09-27T16:05:32Z","timestamp":1758989132000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Lewis Acid Site Engineering in Chromite Spinels Orchestrated Surface Reconstruction and Surpasses RuO\n                    <sub>2<\/sub>\n                    in Oxygen Evolution"],"prefix":"10.1002","volume":"21","author":[{"given":"Abhirami V","family":"Krishnan","sequence":"first","affiliation":[{"name":"Department of Chemistry and Biochemistry The University of Texas at El Paso  El Paso TX 79968 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kavish","family":"Saini","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry The University of Texas at El Paso  El Paso TX 79968 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lissette Garcia","family":"Enriquez","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biochemistry The University of Texas at El Paso  El Paso TX 79968 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"C. 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