Electrocatalytic Reduction of O2 by a Cu(II)-Substituted Electron-Rich Wheel-Type Oxomolybdate Nanocluster |
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Authors: | Israel M Mbomekallé Fang Bian Henry Tebba Achim Müller Ira A Weinstock |
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Institution: | (1) Department of Chemistry, City College of the City University of New York, 138th Street and Convent Avenue, New York, NY 10031, USA;(2) Faculty of Chemistry, University of Bielefeld, P. O. Box 100131, D-33501 Bielefeld, Germany |
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Abstract: | Catalysis of electron transfer by a Cu-substituted wheel-type oxomolybdate cluster–anion,
, (1), is demonstrated. Data provided include aqueous-solution chemistry (stability) studies of 1 and
, (2), derivatives of the “plenary” {Mo154} anion,
, (3). Combined use of cyclic voltammetry and UV–vis spectroscopy shows that, while both 1 and 2 appear to be stable in solution at pH 0.33 (0.5 M H2SO4), 1 is more stable than 2 at pH 3 (in 0.2 M Na2SO4). Cyclic voltammetric analysis in the presence of O2 shows that 1 is an electrocatalyst for electron transfer to O2. Bulk electrolysis of 1 in the presence of O2 (ca. 1 mM) is used to assess catalyst stability under turnover conditions, and to demonstrate that the final product of electrocatalytic reduction is water, rather than H2O2. Finally, control experiments using 1, 2, and CuSO4 (no oxomolybdate-cluster present), show that catalytic activity is due to specific interaction(s) between Cu ions and the Mo142 type oxomolybdate structure of 1. |
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Keywords: | Oxomolybdate nanocluster copper catalysis oxygen |
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