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Title: Comparison and analysis of zinc and cobalt-based systems as catalytic entities for the hydration of carbon dioxide

Journal Article · · PLoS ONE
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  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
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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.

Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
1237575
Report Number(s):
LLNL-JRNL-589234
Journal Information:
PLoS ONE, Vol. 8, Issue 6; ISSN 1932-6203
Publisher:
Public Library of ScienceCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

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Cited By (2)

Improving carbon capture from power plant emissions with zinc- and cobalt-based catalysts journal January 2014
Carbonic anhydrase mimics for enhanced CO 2 absorption in an amine-based capture solvent journal January 2016

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