Abstract
Nanoceria, typically used for “clean-air” catalytic converter technologies because of its ability to capture, store, and release oxygen, is the same material that has the potential to be used in nanomedicine. Specifically, nanoceria can be used to control oxygen content in cellular environments; as a “nanozyme”, nanoceria mimics enzymes by acting as an antioxidant agent. The computational design procedures for predicting active materials for catalytic converters can therefore be used to design active ceria nanozymes. Crucially, the ceria nanomedicine is not a molecule; rather, it is a crystal and exploits its unique crystal properties. Here, we use ab initio and classical computer modeling, together with the experiment, to design structures for nanoceria that maximize its nanozymetic activity. We predict that the optimum nanoparticle shape is either a (truncated) polyhedral or a nanocube to expose (active) CeO2{100} surfaces. It should also contain oxygen vacancies and surface hydroxyl species. We also show that the surface structures strongly affect the biological activity of nanoceria. Analogous to catalyst poisoning, phosphorus “poisoning”, the interaction of nanoceria with phosphate, a common bodily electrolyte, emanates from phosphate ions binding strongly to CeO2{100} surfaces, inhibiting oxygen capture and release and hence its ability to act as a nanozyme. Conversely, the phosphate interaction with {111} surfaces is weak, and therefore, these surfaces protect the nanozyme against poisoning. The atom-level understanding presented here also illuminates catalytic processes and poisoning in “clean-air” or fuel-cell technologies because the mechanism underpinning and exploited in each technology, oxygen capture, storage, and release, is identical.
Original language | English |
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Pages (from-to) | 1098-1106 |
Number of pages | 9 |
Journal | ACS Applied Bio Materials |
Volume | 2 |
Issue number | 3 |
Early online date | 23 Jan 2019 |
DOIs | |
Publication status | Published - 18 Mar 2019 |
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Marco Molinari
- Department of Physical and Life Sciences - Reader
- School of Applied Sciences
- Centre for Functional Materials - Member
- Pharmaceutics and Drug Delivery Centre - Associate Member
- Structural, Molecular and Dynamic Modelling Centre - Associate Member
Person: Academic
Datasets
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Computer-Aided Design of Nanoceria Structures as Enzyme Mimetic Agents: The Role of Bodily Electrolytes on Maximising Their Activity
Molinari, M. (Creator), University of Huddersfield, 2019
DOI: 10.34696/yqqc-xw77, https://huddersfield.box.com/s/lyvzmh0q2xnhfgm5cytxnum43gf7mtr6 and one more link, https://huddersfield.box.com/s/3ud0ikhrgowu4j6d1n6py1yfwwzlmqjd (show fewer)
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