2019
DOI: 10.1002/ange.201904713
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Die Hydrogenobyrsäure‐Struktur enthüllt den Corrin‐Liganden als entatisches Zustandsmodul zur Steigerung der Katalyseaktivität von B12‐Cofaktoren

Abstract: Die B 12 -Cofaktoren erzeugen eine natürliche Neugier bezüglichd er ursprünglichen Selektion und Evolution ihres Corrin-Liganden. Bisher entzogs ich dieser wichtige na-türlicheM akrocyclus überraschenderweise einer detaillierten Untersuchung, sodass seine spezifischeR olle bei der Prädisposition des eingebauten Cobalt-Ions zur organometallischen Katalyse ungeklärt blieb.H ier berichten wir über die Hydrogenobyrsäure (Hby), den cobaltfreien Corrin-Liganden von Vitamin B 12 ,der über eine neuartig programmierte … Show more

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Cited by 8 publications
(14 citation statements)
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“…Acomparison of the crystal structures of Znby and Hby [3] (Figure 4a nd Supporting Information, Table S4) indicates am inor increase only in the radial size of the coordination hole on Zn-binding. Thea verage lengths of the N1-N3 and N2-N4 diagonals in Hby (d = 3.82 )a nd in Znby (d = 3.84 )are similar.…”
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confidence: 95%
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“…Acomparison of the crystal structures of Znby and Hby [3] (Figure 4a nd Supporting Information, Table S4) indicates am inor increase only in the radial size of the coordination hole on Zn-binding. Thea verage lengths of the N1-N3 and N2-N4 diagonals in Hby (d = 3.82 )a nd in Znby (d = 3.84 )are similar.…”
mentioning
confidence: 95%
“…The biological use of cobalt as the specific transition metal center in natural B 12 -cofactors and the interaction between cobalt and the corrin ligand raise intriguing questions concerning the origins of its natural selection. [1] Engineered B 12 -biosynthesis [2] has opened up ap reparative route to hydrogenobyric acid (Hby), [3] the metal-free corrin ligand of vitamin B 12 ,p roviding an excellent opportunity for the synthesis of transition-metal analogues of the natural cobaltcorrinoids. [4] Zn II -analogues of natural corrinoids have hardly been explored [4b] but are attractive,asZn-and low-spin Co IIcenters exhibit similar structural properties in small complexes and in metalloproteins.…”
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confidence: 99%
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“…The joint groups of Watter and Kräutler reported the biosynthesis of the cobalt-free B 12 corrin and concluded from its X-ray structure that ''the corrin ligand coordinates cobalt ions in de-symmetrized 'entatic' states''. 5 This assignment actually presents a head-on collision with the original entatic-state hypothesis which mandatorily required the presence of a protein (or a similarly large structure with a flattened energy landscape). The entatic cobalamin is actually a present-day mark of an increasing trend that developed over the last two decades in which ever more non-protein, free coordination compounds were stickered as entatic-state complexes.…”
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confidence: 99%
“…Note that entasis has been a framework to describe the chemistry of radical-forming Co(II)balamin systems but only for the metal site and only for the situation before the homogeneous Co-C bond splitting. 5 Likewise, entasis in the active site of Fusarium spp. galactose oxidase was ascribed solely to the Cu(II) site and not to the Cu-coordinating tyrosine radical.…”
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confidence: 99%