Publikationsdatum:
2010-03-13
Beschreibung:
Traditional homogeneous water oxidation catalysts are plagued by instability under the reaction conditions. We report that the complex [Co4(H2O)2(PW9O34)2]10-, comprising a Co4O4 core stabilized by oxidatively resistant polytungstate ligands, is a hydrolytically and oxidatively stable homogeneous water oxidation catalyst that self-assembles in water from salts of earth-abundant elements (Co, W, and P). With [Ru(bpy)3]3+ (bpy is 2,2'-bipyridine) as the oxidant, we observe catalytic turnover frequencies for O2 production 〉 or = 5 s(-1) at pH = 8. The rate's pH sensitivity reflects the pH dependence of the four-electron O2-H2O couple. Extensive spectroscopic, electrochemical, and inhibition studies firmly indicate that [Co4(H2O)2(PW9O34)2]10- is stable under catalytic turnover conditions: Neither hydrated cobalt ions nor cobalt hydroxide/oxide particles form in situ.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Yin, Qiushi -- Tan, Jeffrey Miles -- Besson, Claire -- Geletii, Yurii V -- Musaev, Djamaladdin G -- Kuznetsov, Aleksey E -- Luo, Zhen -- Hardcastle, Ken I -- Hill, Craig L -- New York, N.Y. -- Science. 2010 Apr 16;328(5976):342-5. doi: 10.1126/science.1185372. Epub 2010 Mar 11.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, Emory University, Atlanta, GA 30322, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/20223949" target="_blank"〉PubMed〈/a〉
Print ISSN:
0036-8075
Digitale ISSN:
1095-9203
Thema:
Biologie
,
Chemie und Pharmazie
,
Informatik
,
Medizin
,
Allgemeine Naturwissenschaft
,
Physik
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