Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles
- Author
- Melissa Reith, Sinan Kardas, Chiel Mertens, Mathieu Fossepre, Mathieu Surin, Jan Steinkoenig and Filip Du Prez (UGent)
- Organization
- Abstract
- Macromolecules found in Nature display a precise control over the primary as well as higher ordered architectures. To mimic the folding found in Nature, we herein demonstrate the design and characterization of single-chain nanoparticles that are formed by the folding of sequence-defined macromolecules with metal ions. The study showcases the influence of the loop size of such precision macromolecules on their relative hydrodynamic radius. The sequence-defined structures are fabricated using thiolactone chemistry, where two picolyl moieties are installed forming a valuable ligand system for subsequent metal complexation. Next, metal ions such as Ni(ii) and Cu(ii) ions are introduced to fold the unimers into sequence-defined single-chain nanoparticles (SD-SCNPs). After proving the successful complexation using a trimer, a systematic study is conducted altering the distance between the respective ligands by incorporating variable numbers of non-functionalized spacer units. Finally, the loop size formation of the SD-SCNPs is evidenced by DOSY measurements. The result indicates that the positioning of the ligands plays a crucial role on the compaction process and, more specifically, on the final size of the SD-SCNP. In addition, molecular dynamics (MD) simulations show the effects of the sequence and Ni(ii) complexation on the structure and compaction of the SD-SCNPs, and highlight the differences of the nanoparticles' shape when varying the number of spacer units. Finally, the system is further expanded to a dodecamer and even a heptadecamer with drastically decreased hydrodynamic radii after compaction.
- Keywords
- SEQUENCE-DEFINED MACROMOLECULES, POLYMERIC NANOPARTICLES, CROSS-LINKING, DATA-STORAGE, OLIGOMERS, MONODISPERSE, STRATEGY, AFFINITY, DELIVERY, MONOMER
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Citation
Please use this url to cite or link to this publication: http://hdl.handle.net/1854/LU-8721890
- MLA
- Reith, Melissa, et al. “Using Nickel to Fold Discrete Synthetic Macromolecules into Single-Chain Nanoparticles.” POLYMER CHEMISTRY, vol. 12, no. 34, 2021, pp. 4924–33, doi:10.1039/d1py00229e.
- APA
- Reith, M., Kardas, S., Mertens, C., Fossepre, M., Surin, M., Steinkoenig, J., & Du Prez, F. (2021). Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles. POLYMER CHEMISTRY, 12(34), 4924–4933. https://doi.org/10.1039/d1py00229e
- Chicago author-date
- Reith, Melissa, Sinan Kardas, Chiel Mertens, Mathieu Fossepre, Mathieu Surin, Jan Steinkoenig, and Filip Du Prez. 2021. “Using Nickel to Fold Discrete Synthetic Macromolecules into Single-Chain Nanoparticles.” POLYMER CHEMISTRY 12 (34): 4924–33. https://doi.org/10.1039/d1py00229e.
- Chicago author-date (all authors)
- Reith, Melissa, Sinan Kardas, Chiel Mertens, Mathieu Fossepre, Mathieu Surin, Jan Steinkoenig, and Filip Du Prez. 2021. “Using Nickel to Fold Discrete Synthetic Macromolecules into Single-Chain Nanoparticles.” POLYMER CHEMISTRY 12 (34): 4924–4933. doi:10.1039/d1py00229e.
- Vancouver
- 1.Reith M, Kardas S, Mertens C, Fossepre M, Surin M, Steinkoenig J, et al. Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles. POLYMER CHEMISTRY. 2021;12(34):4924–33.
- IEEE
- [1]M. Reith et al., “Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles,” POLYMER CHEMISTRY, vol. 12, no. 34, pp. 4924–4933, 2021.
@article{8721890,
abstract = {{Macromolecules found in Nature display a precise control over the primary as well as higher ordered architectures. To mimic the folding found in Nature, we herein demonstrate the design and characterization of single-chain nanoparticles that are formed by the folding of sequence-defined macromolecules with metal ions. The study showcases the influence of the loop size of such precision macromolecules on their relative hydrodynamic radius. The sequence-defined structures are fabricated using thiolactone chemistry, where two picolyl moieties are installed forming a valuable ligand system for subsequent metal complexation. Next, metal ions such as Ni(ii) and Cu(ii) ions are introduced to fold the unimers into sequence-defined single-chain nanoparticles (SD-SCNPs). After proving the successful complexation using a trimer, a systematic study is conducted altering the distance between the respective ligands by incorporating variable numbers of non-functionalized spacer units. Finally, the loop size formation of the SD-SCNPs is evidenced by DOSY measurements. The result indicates that the positioning of the ligands plays a crucial role on the compaction process and, more specifically, on the final size of the SD-SCNP. In addition, molecular dynamics (MD) simulations show the effects of the sequence and Ni(ii) complexation on the structure and compaction of the SD-SCNPs, and highlight the differences of the nanoparticles' shape when varying the number of spacer units. Finally, the system is further expanded to a dodecamer and even a heptadecamer with drastically decreased hydrodynamic radii after compaction.}},
author = {{Reith, Melissa and Kardas, Sinan and Mertens, Chiel and Fossepre, Mathieu and Surin, Mathieu and Steinkoenig, Jan and Du Prez, Filip}},
issn = {{1759-9954}},
journal = {{POLYMER CHEMISTRY}},
keywords = {{SEQUENCE-DEFINED MACROMOLECULES,POLYMERIC NANOPARTICLES,CROSS-LINKING,DATA-STORAGE,OLIGOMERS,MONODISPERSE,STRATEGY,AFFINITY,DELIVERY,MONOMER}},
language = {{eng}},
number = {{34}},
pages = {{4924--4933}},
title = {{Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles}},
url = {{http://doi.org/10.1039/d1py00229e}},
volume = {{12}},
year = {{2021}},
}
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