Acetyl-coenzyme A synthase: the case for a Ni(p)(0)-based mechanism of catalysis

Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry
Paul A Lindahl

Abstract

Acetyl-CoA synthase (also known as carbon monoxide dehydrogenase) is a bifunctional Ni-Fe-S-containing enzyme that catalyzes the reversible reduction of CO(2) to CO and the synthesis of acetyl-coenzyme A from CO, CoA, and a methyl group donated by a corrinoid iron-sulfur protein. The active site for the latter reaction, called the A-cluster, consists of an Fe(4)S(4) cubane bridged to the proximal Ni site (Ni(p)), which is bridged in turn to the so-called distal Ni site. In this review, evidence is presented that Ni(p) achieves a zero-valent state at low potentials and during catalysis. Ni(p) appears to be the metal to which CO and methyl groups bind and then react to form an acetyl-Ni(p) intermediate. Methyl group binding requires reductive activation, where two electrons reduce some site on the A-cluster. The coordination environment of the distal Ni suggests that it could not be stabilized in redox states lower than 2+. The rate at which the [Fe(4)S(4)](2+) cubane is reduced is far slower than that at which reductive activation occurs, suggesting that the cubane is not the site of reduction. An intriguing possibility is that Ni(p)(2+) might be reduced to the zero-valent state. Reinforcing this idea are Ni-organometallic compl...Continue Reading

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Citations

Sep 14, 2006·Journal of the American Chemical Society·Xiangshi TanPaul A Lindahl
Sep 20, 2008·Journal of the American Chemical Society·William G DoughertyCharles G Riordan
Aug 8, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·Piyal W G AriyanandaCharles G Riordan
May 4, 2005·Proceedings of the National Academy of Sciences of the United States of America·Guillaume IzzetOlivia Reinaud
Nov 2, 2005·Proceedings of the National Academy of Sciences of the United States of America·Kylie A VincentFraser A Armstrong
Jul 9, 2009·Proceedings of the National Academy of Sciences of the United States of America·Mikinao ItoKazuyuki Tatsumi
Jun 8, 2011·Metallomics : Integrated Biometal Science·Güneş BenderStephen W Ragsdale
Sep 20, 2008·Biochimica Et Biophysica Acta·Stephen W Ragsdale, Elizabeth Pierce
Apr 2, 2008·Annals of the New York Academy of Sciences·Stephen W Ragsdale
Jul 6, 2017·Journal of the American Chemical Society·Anastasia C ManesisHannah S Shafaat
Sep 25, 2017·Chemical Communications : Chem Comm·Regina R ReinigAaron D Sadow
Aug 10, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Regina R ReinigAaron D Sadow
Sep 26, 2007·Dalton Transactions : an International Journal of Inorganic Chemistry·Tamar Kurzion-ZilbermannDan Meyerstein
Mar 28, 2008·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Xiangshi Tan, Paul A Lindahl
Sep 30, 2005·Chemical Communications : Chem Comm·Yaw Kai YanPeter J Sadler
Feb 28, 2006·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Xiangshi TanPaul A Lindahl
Jan 28, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Rubén Mas-BallestéFélix Zamora
Feb 6, 2020·Chemical Communications : Chem Comm·Ethan A HillJohn S Anderson
Jun 1, 2011·Chembiochem : a European Journal of Chemical Biology·Yi LiuXiangshi Tan
Oct 8, 2017·Scientific Reports·W J Sandoval-EspinolaJ M Bruno-Bárcena
Aug 10, 2006·Chemical Reviews·Stephen W Ragsdale
Jun 9, 2005·Chemical Reviews·Israel ZilbermannDan Meyerstein
Apr 21, 2005·Journal of the American Chemical Society·Xiangshi TanPaul A Lindahl
Mar 19, 2008·Inorganic Chemistry·Nikolaos LevesanosTristram Chivers
May 24, 2007·Accounts of Chemical Research·Matthew T Kieber-Emmons, Charles G Riordan
Oct 4, 2013·The Journal of Physical Chemistry. a·Aleksandra ChmielowskaMaria Jaworska

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