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Mechanistic study by XPS and 31P SS-NMR substantiated the selective phosphate adsorption pathway as the formation of inner-sphere complexes by HZO@N201, which exhibited enhanced reactivity than HZO@D201. Lastly, fixed-bed runs of HZO@N201 was conducted, achieving an effective treatable volume of 2000 BV, which was 600 BV more than HZO@D201. Additional adsorption-regeneration cycle confirmed its reusability and potential for practical application. We believe the gel-type polymeric host could facilitate the formation and dispersion of small