Homogeneous water oxidation by a di-μ-oxo dimanganese complex in the presence of Ce4+

被引：83

作者：

Tagore, Ranitendranath ^{[1
]}

Chen, Hongyu ^{[1
]}

Zhang, Hong ^{[1
]}

Crabtree, Robert H. ^{[1
]}

Brudvig, Gary W. ^{[1
]}

机构：

[1] Yale Univ, Dept Chem, New Haven, CT 06520 USA

来源：

INORGANICA CHIMICA ACTA | 2007年 / 360卷 / 09期

关键词：

cerium; manganese; oxygen evolution; water oxidation;

D O I：

10.1016/j.ica.2007.02.020

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

O-2 evolution was observed upon mixing aqueous [(terpy)(H2O)Mn(O)(2)Mn(H2O)(terpy)](NO3)(3) (1, terpy = 2,2':6',6"-terpyridine) with aqueous solutions of Ce4+. However, when the solution of 1 was incubated at pH 1 (by dissolving in dilute HNO3) before mixing with Ce4+, very small amounts of O-2 were observed. This observation of acid-induced deactivation suggests an explanation, both for the previously reported lack of O-2 evolution from aqueous solutions of 1 with Ce4+ as oxidant, and the present observation of low amounts of O-2 production with the very acidic Ce4+ reagent. Evidence is provided for water being the source of evolved O-2, and for the requirement of a high valent multinuclear Mn species for O-2 evolution. We test the possibility of complications in the use of ceric ammonium nitrate (CAN) in oxidation chemistry due to the presence of the oxidizable NH4+ ion. (c) 2007 Elsevier B.V. All rights reserved.

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页码：2983 / 2989

页数：7

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