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Resonance Raman spectra of ferrochelatase reveal porphyrin distortion upon metal binding

  • Milton E. Blackwood
    ,
  • Thomas S. Rush
    ,
  • Amy Medlock
    ,
  • Harry A. Dailey
    ,
  • Thomas G. Spiro(corresponding author)
*Corresponding author for this work
  • Princeton University
    ,
  • University of Georgia
Scholary Output:
Contribution to journal
Article
Peer-review

Abstract

Ferrochelatase catalyzes Fe2+ insertion into porphyrins, and is inhibited by Hg2+. Resonance Raman spectra of mesoporphyrin IX show that binding to ferrochelatase restricts the conformation of the propionate side chains, but does not perturb the ring conformation. However, a pronounced perturbation is seen in the ternary complex with Hg2+. Several additional RR bands are activated, including some arising from [R-active vibrations, establishing loss of an effective symmetry center. Out-of-plane modes appear in the low frequency region. The strongest of these bands, γ5 and γ6, correspond to pyrrole tilting vibrations, which are in the same symmetry class as a doming distortion of the porphyrin. All four pyrrole N atoms are pointing toward the same side of the porphyrin plane, a geometry expected to facilitate Fe2+ insertion. This distortion is proposed to result from occupation of a metal-binding site, proximate to the prophyrin, which promotes insertion of Fe2+, while occupation by Hg2+ is inhibitory.

Publication Information

Output type

Scholary Output:
Contribution to journal
Article
Peer-review

Original language

English (US)

Pages from-to (Number of pages)

Pages 12170-12174 (5 pages)

Journal (Volume, Issue Number)

Journal of the American Chemical Society (Volume 119, Issue 50)

Publication milestones

  • Published - 12/17/1997

Publication status

Published - 12/17/1997

ISSN

0002-7863

Publication IDs

  • Scopus: 2642621590

Publication metrics

Metrics

Scopus
citations
SciVal
FWCI
1.70
SciVal
Author count
5
SciVal
citations
41
SciVal
Paper percentile
84
Fractional count
1
Fractional count
0.20
Fractional count
4
Fractional count
0.80
Fractional count
1
Fractional count
1

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Captures
21
Citation count
43