Comparison and Analysis of Zinc and Cobalt-Based Systems as Catalytic Entities for the Hydration of Carbon Dioxide

Edmond Y Lau, Sergio E. Wong, Sarah E. Baker, Jane P. Bearinger, Lucas Koziol, Carlos A. Valdez, Joseph H. Satcher, Roger D. Aines, Felice C Lightstone

Research output: Contribution to journalArticle

9 Citations (Scopus)

Abstract

In nature, the zinc metalloenzyme carbonic anhydrase II (CAII) efficiently catalyzes the conversion of carbon dioxide (CO2) to bicarbonate under physiological conditions. Many research 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 Zn2+ or the Co2+ ion and studied their reaction coordinate for CO2 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. Furthermore, 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.

Original languageEnglish (US)
Article numbere66187
JournalPLoS One
Volume8
Issue number6
DOIs
StatePublished - Jun 20 2013
Externally publishedYes

Fingerprint

cobalt
Cobalt
Carbon Dioxide
Hydration
Zinc
phosphine
zinc
carbon dioxide
Bicarbonates
bicarbonates
Carbonic Anhydrase II
carbonate dehydratase
amines
catalytic activity
Amines
Environmental impact
Catalyst activity
environmental impact
Ions
ions

ASJC Scopus subject areas

  • Agricultural and Biological Sciences(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Medicine(all)

Cite this

Comparison and Analysis of Zinc and Cobalt-Based Systems as Catalytic Entities for the Hydration of Carbon Dioxide. / Lau, Edmond Y; Wong, Sergio E.; Baker, Sarah E.; Bearinger, Jane P.; Koziol, Lucas; Valdez, Carlos A.; Satcher, Joseph H.; Aines, Roger D.; Lightstone, Felice C.

In: PLoS One, Vol. 8, No. 6, e66187, 20.06.2013.

Research output: Contribution to journalArticle

Lau, Edmond Y ; Wong, Sergio E. ; Baker, Sarah E. ; Bearinger, Jane P. ; Koziol, Lucas ; Valdez, Carlos A. ; Satcher, Joseph H. ; Aines, Roger D. ; Lightstone, Felice C. / Comparison and Analysis of Zinc and Cobalt-Based Systems as Catalytic Entities for the Hydration of Carbon Dioxide. In: PLoS One. 2013 ; Vol. 8, No. 6.
@article{a94433f9b5ac4244ab6cbce323552d85,
title = "Comparison and Analysis of Zinc and Cobalt-Based Systems as Catalytic Entities for the Hydration of Carbon Dioxide",
abstract = "In nature, the zinc metalloenzyme carbonic anhydrase II (CAII) efficiently catalyzes the conversion of carbon dioxide (CO2) to bicarbonate under physiological conditions. Many research 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 Zn2+ or the Co2+ ion and studied their reaction coordinate for CO2 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. Furthermore, 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.",
author = "Lau, {Edmond Y} and Wong, {Sergio E.} and Baker, {Sarah E.} and Bearinger, {Jane P.} and Lucas Koziol and Valdez, {Carlos A.} and Satcher, {Joseph H.} and Aines, {Roger D.} and Lightstone, {Felice C}",
year = "2013",
month = "6",
day = "20",
doi = "10.1371/journal.pone.0066187",
language = "English (US)",
volume = "8",
journal = "PLoS One",
issn = "1932-6203",
publisher = "Public Library of Science",
number = "6",

}

TY - JOUR

T1 - Comparison and Analysis of Zinc and Cobalt-Based Systems as Catalytic Entities for the Hydration of Carbon Dioxide

AU - Lau, Edmond Y

AU - Wong, Sergio E.

AU - Baker, Sarah E.

AU - Bearinger, Jane P.

AU - Koziol, Lucas

AU - Valdez, Carlos A.

AU - Satcher, Joseph H.

AU - Aines, Roger D.

AU - Lightstone, Felice C

PY - 2013/6/20

Y1 - 2013/6/20

N2 - In nature, the zinc metalloenzyme carbonic anhydrase II (CAII) efficiently catalyzes the conversion of carbon dioxide (CO2) to bicarbonate under physiological conditions. Many research 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 Zn2+ or the Co2+ ion and studied their reaction coordinate for CO2 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. Furthermore, 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.

AB - In nature, the zinc metalloenzyme carbonic anhydrase II (CAII) efficiently catalyzes the conversion of carbon dioxide (CO2) to bicarbonate under physiological conditions. Many research 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 Zn2+ or the Co2+ ion and studied their reaction coordinate for CO2 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. Furthermore, 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.

UR - http://www.scopus.com/inward/record.url?scp=84879269967&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84879269967&partnerID=8YFLogxK

U2 - 10.1371/journal.pone.0066187

DO - 10.1371/journal.pone.0066187

M3 - Article

C2 - 23840420

AN - SCOPUS:84879269967

VL - 8

JO - PLoS One

JF - PLoS One

SN - 1932-6203

IS - 6

M1 - e66187

ER -