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Toward the synthesis of tetrametallic terminal oxo complexes supported by aminopyrazole ligands

Han, Zhiji and Horak, Kyle and Agapie, Theodor (2016) Toward the synthesis of tetrametallic terminal oxo complexes supported by aminopyrazole ligands. In: 251st American Chemical Society National Meeting & Exposition, 13-17 March 2016, San Diego, CA.

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A proposed mechanism for the O-O bond formation in the oxygen-evolving complex (OEC) of Photosystem II (PSII) involves a terminal Mn-oxo intermediate. Thus, synthesizing multi- metallic clusters contg. such a terminal oxo group is expected to provide further mechanistic insight for the catalytic water oxidn. reaction. Here we report the synthesis and characterization of a series of tetranuclear complexes LM_3OM(L')(PhNHPz)_3 (L = 1,3,5-tris(2-(di(2-pyridyl)hydroxymethyl)phenyl) benzene; M = Mn, Fe; L' = OH, Cl; PhNHPz = 3-phenylamino-pyrazolate). Three metal centers are coordinated by a previously reported ligand, based on three dipyridyl-alkoxide units on a 1,3,5- triarylbenzene motif. The fourth metal center is site- differentiated, and is supported by three PhNHPz ligands and a μ_4-oxo. The PhNHPz bridging ligands were found to provide a hydrogen-bonding network which interacts with terminal ligands bound to the site- differentiated metal. The effect of the second coordination sphere interactions on structure and reactivity will be discussed.

Item Type:Conference or Workshop Item (Paper)
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URLURL TypeDescription Website
Han, Zhiji0000-0001-9349-1571
Agapie, Theodor0000-0002-9692-7614
Additional Information:© 2016 American Chemical Society.
Record Number:CaltechAUTHORS:20160413-103034272
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:66112
Deposited By: Tony Diaz
Deposited On:13 Apr 2016 17:59
Last Modified:20 Nov 2019 22:57

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