
“Artificial enzymes based on metal oxo-clusters:
from discrete species to extended materials”
Thursday March 13th at 11 am
Department of Chemistry of ENS, Salle des Eléments (E012)
24, rue Lhomond, 75005 Paris
Prof. Tatjana N. Parac-Vogt
Department of Chemistry, KU Leuven, 3001 Leuven, Belgium
Effective catalysts for the controlled transformation of large and complex biomolecules are rare and challenging to develop. In particular, selective hydrolysis of proteins by non-enzymatic catalysis is difficult to achieve, yet it is crucial for many modern applications in biotechnology and proteomics. In recent years we developed conceptually new way for selectively cleaving proteins by combining the enzyme-like molecular recognition ability of polyoxometalates (POM), a large group of soluble metal-oxo clusters, with the hydrolytic activity of a strong Lewis acid metal cations (Zr, Hf, Ce) imbedded into the POM structure. Selective cleavage has been demonstrated in a range of proteins differing in structure, size, and charge. More recently, we have shown that metal-organic frameworks (MOFs) based on {Zr6O8} clusters act as very effective heterogeneous catalysts for the hydrolysis of the peptide bond. The catalytic activity of MOFs was shown to be excellent through a broad pH range, resulting in large rate accelerations compared to the uncatalyzed reaction. In addition, UiO-66 Zr-MOF has been found to effectively catalyze intramolecular and intermolecular peptide bond formation without any signs of epimerization. The potential of metal-oxo clusters as nanozymes for protein hydrolysis has been further demonstrated on the example of discrete {Zr6O8} cluster which showed excellent selectivity in the hydrolysis of myoglobin, cleaving the protein only at six solvent accessible Asp residues among 154 residues.Ultimately, these findings indicate that materials based on Zr(IV)-oxo clusters have a large potential to be developed as a novel class of nanozymes for peptide bond formation and hydrolysis.
Key References:
[1] Ly, H.G.T. et.al. J. Am. Chem. Soc. 2018,140, 6325. [2] Moons, J. et.al. Angew. Chem. Int. Ed. 2020, 59, 9094. [3] de Azambuja F., et.al. Acc. Chem. Res., 2021, 54, 1673. [4] de Azambuja, F.; ACS Catal., 2021, 11, 7647. [5] Wang, S. et.al. Nat. Commun. 2022, 13, 1284. [6] S. A. M. Abdelhameed, et.al. Nat. Commun., 2023, 14, 486. [7] K. Declerck, et al. J. Am. Chem. Soc., 2024, 146,11400. [8] S. Dai, et. al. Nat. Commun., 2024, 15, 3434.
Short Biography
Tatjana N. Parac-Vogt is a full professor and head of the laboratory of bioinorganic chemistry at KU Leuven, where she is pursuing interdisciplinary research at the interface of inorganic chemistry, biochemistry, materials science and catalysis. Her main research lines are the development of metal cluster-based complexes and materials such as polyoxometalates (POMs) and metal-organic frameworks (MOFs) for biologically inspired reactions with biomolecules and model systems. The group is also creating new hybrid structures based on polyoxometalates using principles of biomolecular recognition and supramolecular chemistry. Tatjana is the recipient of IUPAC 2023 Distinguished Women in Chemistry and Chemical Engineering award. She is a Fellow of the Royal Society of Chemistry and has been elected as a Chemistry Europe Fellow (Class 2020/2021), the highest award given by an association of European Chemical Societies. Tatjana is a member of AcademiaNet, a global portal of outstanding female scientists, and she is currently the Vice-President of the European Rare-Earth and Actinide Society. She serves on the Editorial Board of Chemical Society Reviews and is a member of the Advisory Board of Inorganic Chemistry.
web: https://lbc.chem.kuleuven.be