TY - JOUR
T1 - Synthesis of pyridine-alkoxide ligands for formation of polynuclear complexes
AU - Shopov, Dimitar Y.
AU - Sharninghausen, Liam S.
AU - Sinha, Shashi Bhushan
AU - Borowski, Julia E.
AU - Mercado, Brandon Q.
AU - Brudvig, Gary W.
AU - Crabtree, Robert H.
N1 - Funding Information:
This work (L. S. S., S. B. S., and D. Y. S.) was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences under Award Number DE-SC0001059 as part of the Argonne-Northwestern Solar Energy Research (ANSER) Energy Frontier Research Center (spectroscopy and characterization) and under Award Number DEFG02-07ER15909 (synthesis).
PY - 2017
Y1 - 2017
N2 - We have prepared and characterized a series of novel polydentate N,O-donor ligands derived from our well-studied ligand 2-(2-pyridinyl)-2-propanol (pyalkH), having the general formula Me{C(OH)(2-py)CH2}nH, where n = 2 or 3. Like pyalkH, these analogues bind via N and O with deprotonation at the latter, thus extending the strongly donor pyridine-alkoxide chelation power of pyalkH to polydentate forms. The greater denticity allows for more effective binding and polynuclear cluster formation with first-row transition metals. Several stable alkoxo-bridged polynuclear clusters of these ligands with Mn, Cu, Co and Ni have been prepared; all reported ligands and complexes have been characterized, including by X-ray crystallography. We report a one-step synthesis of these ligands, alongside pyalkH, on a multi-gram scale from inexpensive starting materials. We have also developed a new scalable procedure for the isolation of pyalkH that avoids the need for chromatography, making large-scale production of this ligand commercially viable.
AB - We have prepared and characterized a series of novel polydentate N,O-donor ligands derived from our well-studied ligand 2-(2-pyridinyl)-2-propanol (pyalkH), having the general formula Me{C(OH)(2-py)CH2}nH, where n = 2 or 3. Like pyalkH, these analogues bind via N and O with deprotonation at the latter, thus extending the strongly donor pyridine-alkoxide chelation power of pyalkH to polydentate forms. The greater denticity allows for more effective binding and polynuclear cluster formation with first-row transition metals. Several stable alkoxo-bridged polynuclear clusters of these ligands with Mn, Cu, Co and Ni have been prepared; all reported ligands and complexes have been characterized, including by X-ray crystallography. We report a one-step synthesis of these ligands, alongside pyalkH, on a multi-gram scale from inexpensive starting materials. We have also developed a new scalable procedure for the isolation of pyalkH that avoids the need for chromatography, making large-scale production of this ligand commercially viable.
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U2 - 10.1039/c7nj01845b
DO - 10.1039/c7nj01845b
M3 - Article
AN - SCOPUS:85022329258
VL - 41
SP - 6709
EP - 6719
JO - New Journal of Chemistry
JF - New Journal of Chemistry
SN - 1144-0546
IS - 14
ER -