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CN-deficient Prussian blue analogues (PBAs), [M N (H 2 O)  x  ]  y  [Fe II (CN) 5 (NH 3 )] (M N = Cu II , Co II , or Ga III ), were synthesized and examined as a new class of heterogeneous catalysts for hydrolytic decomposition of organophosphates often used as pesticides. The active species of the CN-deficient PBAs were mainly C-bound Fe II ions with only single open sites generated by liberation of the NH 3 ligand during the catalytic reactions. [Cu II (H 2 O) 8/3 ] 3/2 [Fe II (CN) 5 (NH 3 )] showed higher catalytic activity than [Co II (H 2 O) 8/3 ] 3/2 [Fe II (CN) 5 (NH 3 )] and [Ga III (H 2 O)][Fe II (CN) 5 (NH 3 )], although N-bound Cu II species has been reported as less active than Co II and Ga III species in conventional PBAs. IR measurements of a series of the CN-deficient PBAs after the catalytic reactions clarified that a part of the NH 3 ligands remained on [Co II (H 2 O) 8/3 ] 3/2 [Fe II (CN) 5 (NH 3 )] and that hydrogen phosphate formed as a product strongly adsorbed on the Fe II ions of [Ga III (H 2 O)][Fe II (CN) 5 (NH 3 )]. Hydrogen phosphate also adsorbed, but weakly, on the Fe II ions of [Cu II (H 2 O) 8/3 ] 3/2 [Fe II (CN) 5 (NH 3 )]. These results suggest that heterogeneous catalysis of the Fe II ions with single open sites were tuned by the M N ions through metal-metal interaction.

inorganic chemistry

Single Open Sites on Fe<sup>II</sup> Ions Stabilized by Coupled Metal Ions in CN-Deficient Prussian Blue Analogues for High Catalytic Activity in the Hydrolysis of Organophosphates

Single Open Sites on FeII Ions Stabilized by Coupled Metal Ions in CN-Deficient Prussian Blue Analogues for High Catalytic Activity in the Hydrolysis of Organophosphates

Single Open Sites on Fe^II Ions Stabilized by Coupled Metal Ions in CN-Deficient Prussian Blue Analogues for High Catalytic Activity in the Hydrolysis of Organophosphates