View : 365 Download: 0
Repurposing a peptide antibiotic as a catalyst: a multicopper-daptomycin complex as a cooperative O-O bond formation and activation catalyst
- Title
- Repurposing a peptide antibiotic as a catalyst: a multicopper-daptomycin complex as a cooperative O-O bond formation and activation catalyst
- Authors
- Lee, Yen Jea; Kim, Haesol; Kim, Yujeong; Cho, Kang Hee; Hong, Sugyeong; Nam, Ki Tae; Kim, Sun Hee; Choi, Chang Hyuck; Seo, Jiwon
- Ewha Authors
- 김선희
- SCOPUS Author ID
- 김선희
- Issue Date
- 2022
- Journal Title
- INORGANIC CHEMISTRY FRONTIERS
- ISSN
- 2052-1553
- Citation
- INORGANIC CHEMISTRY FRONTIERS vol. 9, no. 18, pp. 4741 - 4752
- Publisher
- ROYAL SOC CHEMISTRY
- Indexed
- SCIE; SCOPUS
- Document Type
- Article
- Abstract
- In naturally occurring metalloenzymes, cooperative multimetallic sites activate, cleave, and form dioxygen bonds. Thus, molecular scaffolds providing multimetallic sites are increasingly being exploited to develop cooperative redox catalysts. Herein, we report a multicopper complex based on a peptide antibiotic, daptomycin (dap), which mediates O-O bond formation and activation reactions. In alkaline media, UV-vis and electron paramagnetic resonance (EPR) spectroscopy showed that dap stabilized up to four Cu(ii) ions (Cu-n-dap, n = 1-4) in a square planar Cu-N-4 geometry, with an axially bound H2O or OH ligand. Cooperative rate enhancement was observed for the O-2 activation, H2O2 disproportionation, and O-2 evolution reactions, only in the presence of the multimetallic Cu complex. In situ Raman spectroscopy was used to study the intermediate species involved in the electrochemical O-2 evolution reaction and understand the catalytic mechanism behind the O-O bond formation. The observed Cu-O species related to the Cu2O2 core suggested a possible radical coupling pathway for the O-O bond formation. This study provides a strategy to repurpose natural calcium-binding peptide antibiotics as ligands, to create multimetallic sites for cooperative catalysis.
- DOI
- 10.1039/d2qi01440h
- Appears in Collections:
- 자연과학대학 > 화학·나노과학전공 > Journal papers
- Files in This Item:
There are no files associated with this item.
- Export
- RIS (EndNote)
- XLS (Excel)
- XML