Comparison and analysis of zinc and cobalt-based systems as catalytic entities for the hydration of carbon dioxide [electronic resource].

Published:: Washington, D.C. : United States. Dept. of Energy, 2013.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description:: Article numbers e66,187 : digital, PDF file
Additional Creators:: Lawrence Berkeley National Laboratory, United States. Department of Energy, and United States. Department of Energy. Office of Scientific and Technical Information

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Summary:

In nature, the zinc metalloenzyme carbonic anhydrase II (CAII) efficiently catalyzes the conversion of carbon dioxide (CO ₂) to bicarbonate under physiological conditions. Efforts have been directed towards the development of small molecule mimetics that can facilitate this process and thus have a beneficial environmental impact, but these efforts have met very limited success. Herein, we undertook quantum mechanical calculations of four mimetics, 1,5,9-triazacyclododedacane, 1,4,7,10-tetraazacyclododedacane, tris(4,5-dimethyl-2-imidazolyl)phosphine, and tris(2-benzimidazolylmethyl)amine, in their complexed form either with the Zn ²⁺ or the Co ²⁺ ion and studied their reaction coordinate for CO ₂ hydration. These calculations demonstrated that the ability of the complex to maintain a tetrahedral geometry and bind bicarbonate in a unidentate manner were vital for the hydration reaction to proceed favorably. Moreover, these calculations show that the catalytic activity of the examined zinc complexes was insensitive to coordination states for zinc, while coordination states above four were found to have an unfavorable effect on product release for the cobalt counterparts.

Report Numbers:

E 1.99:llnl-jrnl--589234
llnl-jrnl--589234

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Note:

Published through SciTech Connect.
06/20/2013.
"llnl-jrnl--589234"
PLoS ONE 8 6 ISSN 1932-6203 AM
E. Y. Lau; S. E. Wong; S. E. Baker; J. P. Bearinger; L. Koziol; C. A. Valdez; J. H. Satcher; R. D. Aines; F. C. Lightstone.

Funding Information:

AC52-07NA27344

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