Chemistry and Physics Faculty Articles

Title

Electrooxidation of Alcohols Catalyzed by Amino Alcohol Ligated Ruthenium Complexes

Document Type

Article

Publication Date

9-25-2013

Publication Title

Journal of the American Chemical Society

ISSN

0002-7863

Volume

135

Issue/No.

38

First Page

14299

Last Page

14305

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.

Comments

©2013 American Chemical Society

Additional Comments

NSF grant #: CHE-1213403; Air Force Office of Scientific Research grant #: AFOSR FA9550-10-1-0235

DOI

10.1021/ja4055564

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Peer Reviewed

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