A Gold Nanoparticle Nanonuclease Relying on a Zn(II) Mononuclear Complex.
- Czescik J Department of Chemical Sciences, University of Padova, via Marzolo, 1, 35131, Padova, Italy.
- Zamolo S Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, CH-3012, Bern, Switzerland.
- Darbre T Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, CH-3012, Bern, Switzerland.
- Rigo R Department of Pharmaceutical and Pharmacological Sciences, University of Padova, via Marzolo 5, 35131, Padova, Italy.
- Sissi C Department of Pharmaceutical and Pharmacological Sciences, University of Padova, via Marzolo 5, 35131, Padova, Italy.
- Pecina A Laboratory of Molecular Modeling & Drug Discovery, Istituto Italiano di Tecnologia (IIT), Via Morego 30, 16163, Genova, Italy.
- Riccardi L Laboratory of Molecular Modeling & Drug Discovery, Istituto Italiano di Tecnologia (IIT), Via Morego 30, 16163, Genova, Italy.
- De Vivo M Laboratory of Molecular Modeling & Drug Discovery, Istituto Italiano di Tecnologia (IIT), Via Morego 30, 16163, Genova, Italy.
- Mancin F Department of Chemical Sciences, University of Padova, via Marzolo, 1, 35131, Padova, Italy.
- Scrimin P Department of Chemical Sciences, University of Padova, via Marzolo, 1, 35131, Padova, Italy.
- 2020-09-28
Published in:
- Angewandte Chemie (International ed. in English). - 2020
English
Similarly to enzymes, functionalized gold nanoparticles efficiently catalyze chemical reactions, hence the term nanozymes. Herein, we present our results showing how surface-passivated gold nanoparticles behave as synthetic nanonucleases, able to cleave pBR322 plasmid DNA with the highest efficiency reported so far for catalysts based on a single metal ion mechanism. Experimental and computational data indicate that we have been successful in creating a catalytic site precisely mimicking that suggested for natural metallonucleases relying on a single metal ion for their activity. It comprises one Zn(II) ion to which a phosphate diester of DNA is coordinated. Importantly, as in nucleic acids-processing enzymes, a positively charged arginine plays a key role by assisting with transition state stabilization and by reducing the pKa of the nucleophilic alcohol of a serine. Our results also show how designing a catalyst for a model substrate (bis-p-nitrophenylphosphate) may provide wrong indications as for its efficiency when it is tested against the real target (plasmid DNA).
- Language
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- English
- Open access status
- hybrid
- Identifiers
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- DOI 10.1002/anie.202012513
- PMID 32985766
- Persistent URL
- https://sonar.ch/global/documents/186938
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