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Lecture

FRESH Lecture: NikA as versatile protein scaffold for the design of artificial oxidases/oxygenases for sustainable chemistry

  • Dr. Stéphane Ménage (Université Grenoble Alpes)
Date
Thursday 28 March 2019
Time
Location
Gorlaeus Building
Einsteinweg 55
2333 CC Leiden
Room
Havinga Lecture room

Abstract

Catalysis represents an exciting tool for the development of sustainable chemistry. Among the different approaches, biocatalysis is the most promising strategy but the repertoire of reactions has not reached yet the one of (in)organic catalysis. Artificial enzymes fulfil then the gap by allowing abiotic reactions with in some cases reaching enzyme catalytic efficiencies.1 

Our group at LCBM has been involved in the design of artificial metalloenzymes2 for oxidation reactions. Using a protein scaffold, NikA, a Ni(II) import protein, several chemical transformations have been performed thanks to the embedment of iron and ruthenium complexes within the protein cavity.3

This lecture will drive the attendance to a walk along the NikA landscape to present some assets of such artificial enzyme. In particular, a focus on the structure/activity for various oxidation reactions (sulfoxidation, alkene oxidative cleavage, hydroxychlorination and epoxidation) will be given.4 A special attention on the deciphering of their reaction mechanisms will be done. The possible transposition of homogeneous/bio-catalysis to heterogeneous catalysis for these bio-hybrids will be discussed in the light of the development of cross-linked enzyme crystal technology. 

Finally, a future perspective will be developed.

References

1 Hammer, S.C.; Kubik, G.; Watkins, E.; Huang, S.; Minges, H.; Arnold, F.H.; Science, 2017, 358,

2 a) Schwizer, F.; Okamoto, Y.; Heinisch, T.; Gu, Y.; Pellizzoni, M.M.; Lebrun, V.; Reuter, R.; K.hler, V.; Lewis, J.C.; Ward, T.R.; Chem. Rev., 2018, 118, 142;

  b) Marchi-Delapierre, C.; Rondot, L.; Cavazza, C.; Ménage, S. Isr. J. Chem., 2015, 55, 61.

  c) Drienovska, I.; Mayer, C.; Dulson, C.; Roelfes, G.; Nat. Chem. 10, 946-52.

3 Cherrier, M.V.; Girgenti, E.; Amara, P.; Iannello, M.; Marchi-Delapierre, C.; Fontecilla-Camps, J.C.; Menage, S.; Cavazza, C.J.; Biol. Inorg. Chem., 2012, 17, 817.

4 Lopez, S.; Rondot, L.; Cavazza, C.; Iannello, M.; Boeri-Erba, E.; Burzlaff, N.; Strinitz, F.; Jorge-Robin, A.; Marchi-Delapierre, C.; Menage, S.; Chem. Commun., 2017, 53, 3579.

Esmieu, C.; Cherrier, M.V.; Amara, P.; Girgenti, E.; Marchi-Delapierre, C.; Oddon, F.; Iannello, M.; Jorge-Robin, A.; Cavazza, C.; Ménage, S.; Angew Chem. Int. Ed, 2013, 52, 3922-3925.

Lopez, S.; Rondot, L.; Leprêtre, C.; Marchi-Delapierre, C.; Ménage, S. and Cavazza, C.; J. Am. Chem. Soc., 2017, 139, 17994-18002.    

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