Electrooxidation of Alcohols Catalyzed by Amino Alcohol Ligated Ruthenium Complexes
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Department of Chemistry, Stanford University, Stanford, California 94305-5080, United States
J. Am. Chem. Soc., Article ASAP
DOI: 10.1021/ja4055564
Publication Date (Web): September 17, 2013
Copyright © 2013 American Chemical Society
Abstract
Ruthenium transfer hydrogenation catalysts physisorbed onto edge-plane graphite electrodes are active electrocatalysts for the oxidation of alcohols. Electrooxidation of CH3OH (1.23 M) in a buffered aqueous solution at pH 11.5 with [(η6-p-cymene)(η2-N,O-(1R,2S)-cis-1-amino-2-indanol)]RuIICl (2) on edge-plane graphite exhibits an onset current at 560 mV vs NHE. Koutecky–Levich analysis at 750 mV reveals a four-electron oxidation of methanol with a rate of 1.35 M–1 s–1. Mechanistic investigations by 1H NMR, cyclic voltammetry, and desorption electrospray ionization mass spectrometry indicate that the electroxidation of methanol to generate formate is mediated by surface-supported Ru–oxo complexes.
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