Synthesis and vibrational spectroscopy of 57Fe-labeled models of [NiFe] hydrogenase: first direct observation of a nickel–iron interaction

David Schilter; Vladimir Pelmenschikov; Hongxin Wang; Florian Meier; Leland B. Gee; Yoshitaka Yoda; Martin Kaupp; Thomas B. Rauchfuss; Stephen P. Cramer

doi:10.1039/C4CC04572F

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Synthesis and vibrational spectroscopy of ⁵⁷Fe-labeled models of [NiFe] hydrogenase: first direct observation of a nickel–iron interaction†

David Schilter,*^a Vladimir Pelmenschikov,^b Hongxin Wang,^cd Florian Meier,^b Leland B. Gee,^c Yoshitaka Yoda,^e Martin Kaupp,^b Thomas B. Rauchfuss^a and Stephen P. Cramer*^cd

Author affiliations

* Corresponding authors

^a Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, USA
E-mail: schilter@illinois.edu

^b Institut für Chemie, Technische Universität Berlin, 10623 Berlin, Germany

^c Department of Chemistry, University of California, Davis, USA
E-mail: spjcramer@ucdavis.edu

^d Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, USA

^e JASRI, SPring-8, Sayo-gun, Hyogo 679-5198, Japan

Abstract

A new route to iron carbonyls has enabled synthesis of ⁵⁷Fe-labeled [NiFe] hydrogenase mimic (OC)₃⁵⁷Fe(pdt)Ni(dppe). Its study by nuclear resonance vibrational spectroscopy revealed Ni–⁵⁷Fe vibrations, as confirmed by calculations. The modes are absent for [(OC)₃⁵⁷Fe(pdt)Ni(dppe)]⁺, which lacks Ni–⁵⁷Fe bonding, underscoring the utility of the analyses in identifying metal–metal interactions.

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DOI: https://doi.org/10.1039/C4CC04572F
Article type: Communication
Submitted: 16 Jun 2014
Accepted: 09 Sep 2014
First published: 10 Sep 2014
This article is Open Access

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Chem. Commun., 2014,50, 13469-13472

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Synthesis and vibrational spectroscopy of ⁵⁷Fe-labeled models of [NiFe] hydrogenase: first direct observation of a nickel–iron interaction

D. Schilter, V. Pelmenschikov, H. Wang, F. Meier, L. B. Gee, Y. Yoda, M. Kaupp, T. B. Rauchfuss and S. P. Cramer, Chem. Commun., 2014, 50, 13469 DOI: 10.1039/C4CC04572F

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