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Investigations of the Efficient Electrocatalytic Interconversions of Carbon Dioxide and Carbon Monoxide by Nickel-Containing Carbon Monoxide Dehydrogenases

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The Metal-Driven Biogeochemistry of Gaseous Compounds in the Environment

Part of the book series: Metal Ions in Life Sciences ((MILS,volume 14))

Abstract

Carbon monoxide dehydrogenases (CODH) play an important role in utilizing carbon monoxide (CO) or carbon dioxide (CO2) in the metabolism of some microorganisms. Two distinctly different types of CODH are distinguished by the elements constituting the active site. A Mo-Cu containing CODH is found in some aerobic organisms, whereas a Ni-Fe containing CODH (henceforth simply Ni-CODH) is found in some anaerobes. Two members of the simplest class (IV) of Ni-CODH behave as efficient, reversible electrocatalysts of CO2/CO interconversion when adsorbed on a graphite electrode. Their intense electroactivity sets an important benchmark for the standard of performance at which synthetic molecular and material electrocatalysts comprised of suitably attired abundant first-row transition elements must be able to operate. Investigations of CODHs by protein film electrochemistry (PFE) reveal how the enzymes respond to the variable electrode potential that can drive CO2/CO interconversion in each direction, and identify the potential thresholds at which different small molecules, both substrates and inhibitors, enter or leave the catalytic cycle. Experiments carried out on a much larger (Class III) enzyme CODH/ACS, in which CODH is complexed tightly with acetyl-CoA synthase, show that some of these characteristics are retained, albeit with much slower rates of interfacial electron transfer, attributable to the difficulty in making good electronic contact at the electrode. The PFE results complement and clarify investigations made using spectroscopic investigations.

Please cite as: Met. Ions Life Sci. 14 (2014) 71–97

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Acknowledgments

The authors thank the UK Research Councils (BBSRC (grants H003878-1 and BB/I022309) and EPSRC (Supergen 5, EH/H019480/1)), and NIH (GM39451) for supporting their research. Vincent Wang thanks the Ministry of Education, Taiwan (R.O.C) for financial support through a scholarship for study abroad.

Author information

Authors and Affiliations

  1. Department of Chemistry, Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, Oxford, OX1 3QR, UK

    Vincent C.-C. Wang & Fraser A. Armstrong

  2. Department of Biological Chemistry, University of Michigan Medical School, Ann Arbor, MI, 48109-0606, USA

    Stephen W. Ragsdale

Authors
  1. Vincent C.-C. Wang
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  2. Stephen W. Ragsdale
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  3. Fraser A. Armstrong
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Corresponding author

Correspondence to Fraser A. Armstrong .

Editor information

Editors and Affiliations

  1. Univ. Konstanz Fachbereich Biologie, Konstanz, Baden-Württemberg, Germany

    Peter M.H. Kroneck

  2. Facultad de Química Universidad Autónoma de México, Departamento de Química Inorganica y Nuclear, México, Distrito Federal, Mexico

    Martha E. Sosa Torres

Abbreviations

Abbreviations

acetyl-CoA:

acetyl-coenzyme A

ACDS:

acetyl-CoA decarbonylase synthase

Ch :

Carboxydothermus hydrogenoformans

CoA:

coenzyme A

CODH:

carbon monoxide dehydrogenase

CODH/ACS:

carbon monoxide dehydrogenase/acetyl-CoA synthase

CoFeSP:

corrinoid-iron-sulfur protein

E FB :

flatband potential

EPR:

electron paramagnetic resonance

Mb :

Methanosarcina barkeri

MES:

2-(N-morpholino)ethanesulfonic acid

Mt :

Moorella thermoacetica

PDB:

Protein Data Base

PFE:

protein film electrochemistry

PGE:

pyrolytic graphite edge

Rr :

Rhodospirillum rubrum

SHE:

standard hydrogen electrode

XAS:

X-ray absorption spectroscopy

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Wang, V.CC., Ragsdale, S.W., Armstrong, F.A. (2014). Investigations of the Efficient Electrocatalytic Interconversions of Carbon Dioxide and Carbon Monoxide by Nickel-Containing Carbon Monoxide Dehydrogenases. In: Kroneck, P., Torres, M. (eds) The Metal-Driven Biogeochemistry of Gaseous Compounds in the Environment. Metal Ions in Life Sciences, vol 14. Springer, Dordrecht. https://doi.org/10.1007/978-94-017-9269-1_4

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