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Electrochemical nitrate reduction reaction (NO\n                    <jats:sub>3<\/jats:sub>\n                    RR) offers a sustainable alternative by coupling NH\n                    <jats:sub>3<\/jats:sub>\n                    synthesis with water remediation. However, challenges such as weak NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    adsorption, competing hydrogen evolution, and suboptimal catalyst microenvironments hinder performance. Here, we report a family of electrocatalysts, Pd\u2282QA\u2010Cage\n                    <jats:italic>\n                      <jats:sup>x<\/jats:sup>\n                    <\/jats:italic>\n                    <jats:sup>+<\/jats:sup>\n                    (\n                    <jats:italic>x<\/jats:italic>\n                    = 24, 12, 6), constructed by encapsulating Pd clusters within quaternized organic cages. These discrete hosts enable uniform metal cluster confinement and precise control over the interfacial microenvironment. Increasing cage charge density enriches interfacial NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    concentration, upshifts Pd\n                    <jats:italic>d<\/jats:italic>\n                    \u2010band center, and enhances *NO\n                    <jats:sub>3<\/jats:sub>\n                    activation. Simultaneously, potential\u2010driven electron transfer from the counterion (Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    ) to \u2013NH\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>+<\/jats:sup>\n                    \u2013 generates stable radicals in the cage skeleton, which mediate water activation to form hydrogen radicals (H\u2022) that spill over to Pd sites, accelerating intermediate hydrogenation. The optimized Pd\u2282QA\u2010Cage\n                    <jats:sup>24+<\/jats:sup>\n                    delivers a Faradaic efficiency of 95.44% and an NH\n                    <jats:sub>3<\/jats:sub>\n                    yield of 25.70 mg h\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    mg\n                    <jats:sub>cat<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    in neutral electrolytes, outperforming its lower\u2010charge analogs. Moreover, it enables &gt; 99.4% nitrate removal from eutrophic seawater, reducing NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    concentrations below potable water standards. This work introduces ionic cages as programmable interfacial modifiers, offering a supramolecular strategy to regulate electrochemical microenvironments and boost electrocatalytic NO\n                    <jats:sub>3<\/jats:sub>\n                    RR performance.\n                  <\/jats:p>","DOI":"10.1002\/anie.4155022","type":"journal-article","created":{"date-parts":[[2026,4,21]],"date-time":"2026-04-21T10:31:22Z","timestamp":1776767482000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Interfacial Charge\u2010Regulated Microenvironments Enabled by Ionic Organic Cages for Boosting Electrocatalytic Nitrate Reduction to Ammonia"],"prefix":"10.1002","volume":"65","author":[{"given":"Shuyuan","family":"Li","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectronic\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"},{"name":"Institute of Technology for Carbon Neutrality Shenzhen Institutes of Advanced Technology (SIAT) Chinese Academy of Sciences (CAS)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun\u2010Hao","family":"Zhou","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectronic\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shi\u2010Long","family":"Han","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectronic\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Doufeng","family":"Wang","sequence":"additional","affiliation":[{"name":"Institute of Technology for Carbon Neutrality Shenzhen Institutes of Advanced Technology (SIAT) Chinese Academy of Sciences (CAS)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ying\u2010Ying","family":"Yu","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectronic\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun\u2010Yu","family":"Li","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectronic\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Si\u2010Hua","family":"Liu","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectronic\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaojie","family":"Chen","sequence":"additional","affiliation":[{"name":"Institute of Technology for Carbon Neutrality Shenzhen Institutes of Advanced Technology (SIAT) Chinese Academy of Sciences (CAS)  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8084-4630","authenticated-orcid":false,"given":"Xinchun","family":"Yang","sequence":"additional","affiliation":[{"name":"Institute of Technology for Carbon Neutrality Shenzhen Institutes of Advanced Technology (SIAT) Chinese Academy of Sciences (CAS)  Shenzhen 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