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Precise design and construction of catalysts with satisfied performance for ambient electrolytic nitrogen reduction reaction (e‐NRR) is extremely challenging. By in situ integrating an electron‐rich polyoxometalates (POMs) into stable metal organic frameworks (MOFs), five POMs‐based MOFs formulated as [FexCoy(Pbpy)9(ox)6(H2O)6][P2W18O62]·3H2O (abbreviated as FexCoyMOF‐P2W18) are created and directly...