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

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

doi:10.1039/c4cc04572f

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

Journal Article · Wed Sep 10 00:00:00 EDT 2014 · ChemComm

DOI:https://doi.org/10.1039/c4cc04572f· OSTI ID:1624906

Schilter, David ^[1]; Pelmenschikov, Vladimir ^[2]; Wang, Hongxin ^[3]; Meier, Florian ^[2]; Gee, Leland B. ^[4]; Yoda, Yoshitaka ^[5]; Kaupp, Martin ^[2]; Rauchfuss, Thomas B. ^[6]; Cramer, Stephen P. ^[3]

Univ. of Illinois at Urbana-Champaign, IL (United States). Dept. of Chemistry; DOE/OSTI
Technische Universität Berlin (Germany). Institut für Chemie
Univ. of California, Davis, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Physical Biosciences Division
Univ. of California, Davis, CA (United States). Dept. of Chemistry
JASRI, Sayo-gun (Japan)
Univ. of Illinois at Urbana-Champaign, IL (United States). Dept. of Chemistry

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1624906

Journal Information:: ChemComm, Journal Name: ChemComm Journal Issue: 88 Vol. 50; ISSN 1359-7345

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Hydride bridge in [NiFe]-hydrogenase observed by nuclear resonance vibrational spectroscopy Ogata, Hideaki; Krämer, Tobias; Wang, Hongxin Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8890	journal	August 2015

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