AI Article Synopsis
- Four new dinuclear Ni/Mn model complexes were synthesized through a series of four reactions involving six new precursors, enabling the study of their catalytic properties.
- The synthesis process included steps such as the aminolysis of Ph2PCl to create azadiphosphine ligands and the coordination with NiCl2 to develop mononuclear complexes, leading to a higher yield of final dinuclear complexes.
- The new complexes have been characterized structurally, and model complexes 7 and 9 demonstrated catalytic activity in reducing acetic acid to hydrogen in cyclic voltammetry experiments.
Article Abstract
Four new dinuclear Ni/Mn model complexes RN(PPh2)2Ni(μ-SEt)2(μ-Cl)Mn(CO)3 (7, R = p-MeC6H4CH2; 8, R = EtO2CCH2) and RN(PPh2)2Ni(μ-SEt)2(μ-Br)Mn(CO)3 (9, R = p-MeC6H4CH2; 10, R = EtO2CCH2) have been prepared via the four separated step-reactions involving six new precursors RN(PPh2)2 (1, R = p-MeC6H4CH2; 2, R = EtO2CCH2), RN(PPh2)2NiCl2 (3, R = p-MeC6H4CH2; 4, R = EtO2CCH2), and RN(PPh2)2Ni(SEt)2 (5, R = p-MeC6H4CH2; 6, R = EtO2CCH2). The Et3N-assisted aminolysis of Ph2PCl with p-MeC6H4CH2NH2 or EtO2CCH2NH2·HCl in CH2Cl2 gave the azadiphosphine ligands 1 and 2 in 38% and 53% yields, whereas the coordination reaction of 1 or 2 with NiCl2·6H2O in CH2Cl2/MeOH afforded the mononuclear Ni dichloride complexes 3 and 4 in 59% and 78% yields, respectively. While thiolysis of 3 or 4 with EtSH under the assistance of Et3N in CH2Cl2 produced the mononuclear Ni dithiolate complexes 5 and 6 in 64% and 68% yields, further treatment of 5 and 6 with Mn(CO)5Cl or Mn(CO)5Br resulted in formation of the dinuclear Ni/Mn model complexes 7-10 in 31-73% yields. All the new compounds 1-10 have been structurally characterized, while model complexes 7 and 9 have been found to be catalysts for HOAc proton reduction to hydrogen under CV conditions.
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| http://dx.doi.org/10.1021/ic401978h | DOI Listing |
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Synthesis, structural characterization, and electrochemical properties of dinuclear Ni/Mn model complexes for the active site of [NiFe]-hydrogenases.
Inorg Chem
October 2013
Department of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin 300071, China.
Article Synopsis
- Four new dinuclear Ni/Mn model complexes were synthesized through a series of four reactions involving six new precursors, enabling the study of their catalytic properties.
- The synthesis process included steps such as the aminolysis of Ph2PCl to create azadiphosphine ligands and the coordination with NiCl2 to develop mononuclear complexes, leading to a higher yield of final dinuclear complexes.
- The new complexes have been characterized structurally, and model complexes 7 and 9 demonstrated catalytic activity in reducing acetic acid to hydrogen in cyclic voltammetry experiments.
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