Dimeric Corrole Analogs of Chlorophyll Special Pairs.
Journal
Journal of the American Chemical Society
ISSN: 1520-5126
Titre abrégé: J Am Chem Soc
Pays: United States
ID NLM: 7503056
Informations de publication
Date de publication:
30 06 2021
30 06 2021
Historique:
pubmed:
21
5
2021
medline:
5
3
2022
entrez:
20
5
2021
Statut:
ppublish
Résumé
Chlorophyll special pairs in photosynthetic reaction centers function as both exciton acceptors and primary electron donors. Although the macrocyclic natural pigments contain Mg(II), the central metal in most synthetic analogs is Zn(II). Here we report that insertion of either Al(III) or Ga(III) into an imidazole-substituted corrole affords an exceptionally robust photoactive dimer. Notably, attractive electronic interactions between dimer subunits are relatively strong, as documented by signature changes in NMR and electronic absorption spectra, as well as by cyclic voltammetry, where two well-separated reversible redox couples were observed. EPR spectra of one-electron oxidized dimers closely mimic those of native special pairs, and strong through-space interactions between corrole subunits inferred from spectroscopic and electrochemical data are further supported by crystal structure analyses (3 Å interplanar distances, 5 Å lateral shifts, and 6 Å metal to metal distances).
Identifiants
pubmed: 34014656
doi: 10.1021/jacs.1c02362
pmc: PMC8249354
mid: NIHMS1711398
doi:
Substances chimiques
Imidazoles
0
Metalloporphyrins
0
Chlorophyll
1406-65-1
Gallium
CH46OC8YV4
Aluminum
CPD4NFA903
Types de publication
Journal Article
Research Support, N.I.H., Extramural
Research Support, Non-U.S. Gov't
Langues
eng
Sous-ensembles de citation
IM
Pagination
9450-9460Subventions
Organisme : NIDDK NIH HHS
ID : R01 DK019038
Pays : United States
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