Despite the intrinsic peroxidase-like activity of Prussian blue nanopartides (PBNPs), their enzyme-mimic mechanism has been scarcely investigated to date. Herein, we probed the catalytic site of PBNPs for the first ...Despite the intrinsic peroxidase-like activity of Prussian blue nanopartides (PBNPs), their enzyme-mimic mechanism has been scarcely investigated to date. Herein, we probed the catalytic site of PBNPs for the first time, by comparing their peroxidase-like activity with that of a series of Prussian blue analogs (PBAs) in which Fe atoms were replaced by Co, Ni, and Cu. The PBNPs exhibited the highest maximal reaction velocity (1.941 μM·s^-1), which was at least 13 times higher than that of the PBAs, demonstrating that the peroxidase-like properties of PBNPs could be ascribed to the FeNx (x=4-6) instead of the FeC6 units. Notably, the PBNPs/H2O2 couple also showed much higher oxidizability than .OH radicals produced from the Fenton reaction, implying that a high active Fe(W)=O intermediate might be formed in the FeNx units. This study can thus pave the way for the wider application of PBNPs in biomimetic reactions.展开更多
The tide compound is formed by controlled hydrolytic polymerization in nonaqueous solution of simple oxo-bridged binuclear ferric salts under the presence of carboxylate ligands. The rhombohedral crystalline form of t...The tide compound is formed by controlled hydrolytic polymerization in nonaqueous solution of simple oxo-bridged binuclear ferric salts under the presence of carboxylate ligands. The rhombohedral crystalline form of the cluster with six imidazole molecules, which has crystallographically required C3v symmetry, will be reported. The largest Fe-Fe distance in the undecairon oxo-hydroxo cluster is about 0.68 nm and the cluster has a diameter near 2 nm, which implies that this cluster reaches a nanometer-sized dimension.展开更多
文摘Despite the intrinsic peroxidase-like activity of Prussian blue nanopartides (PBNPs), their enzyme-mimic mechanism has been scarcely investigated to date. Herein, we probed the catalytic site of PBNPs for the first time, by comparing their peroxidase-like activity with that of a series of Prussian blue analogs (PBAs) in which Fe atoms were replaced by Co, Ni, and Cu. The PBNPs exhibited the highest maximal reaction velocity (1.941 μM·s^-1), which was at least 13 times higher than that of the PBAs, demonstrating that the peroxidase-like properties of PBNPs could be ascribed to the FeNx (x=4-6) instead of the FeC6 units. Notably, the PBNPs/H2O2 couple also showed much higher oxidizability than .OH radicals produced from the Fenton reaction, implying that a high active Fe(W)=O intermediate might be formed in the FeNx units. This study can thus pave the way for the wider application of PBNPs in biomimetic reactions.
基金Project (No. 29871003) Supported by the National Natural Science Foundation of China.
文摘The tide compound is formed by controlled hydrolytic polymerization in nonaqueous solution of simple oxo-bridged binuclear ferric salts under the presence of carboxylate ligands. The rhombohedral crystalline form of the cluster with six imidazole molecules, which has crystallographically required C3v symmetry, will be reported. The largest Fe-Fe distance in the undecairon oxo-hydroxo cluster is about 0.68 nm and the cluster has a diameter near 2 nm, which implies that this cluster reaches a nanometer-sized dimension.