Mercury Methylation by Cobalt Corrinoids: Relativistic Effects Dictate the Reaction Mechanism

Publisher： John Wiley & Sons Inc

E-ISSN： 1521-3773|55|38|11503-11506

ISSN： 1433-7851

Source： ANGEWANDTE CHEMIE INTERNATIONAL EDITION, Vol.55, Iss.38, 2016-09, pp. : 11503-11506

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Abstract

AbstractThe methylation of HgII(SCH3)2 by corrinoid‐based methyl donors proceeds in a concerted manner through a single transition state by transfer of a methyl radical, in contrast to previously proposed reaction mechanisms. This reaction mechanism is a consequence of relativistic effects that lower the energies of the mercury 6p1/2 and 6p3/2 orbitals, making them energetically accessible for chemical bonding. In the absence of spin–orbit coupling, the predicted reaction mechanism is qualitatively different. This is the first example of relativity being decisive for the nature of an observed enzymatic reaction mechanism.

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