Control of Polymer Brush Morphology, Rheology, and Protein Repulsion by Hydrogen Bond Complexation
Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert toward biomolecular adsorption. Neutral hydrophilic brushes are normally considered to have static properties at a given temperature. As an...
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| Published in | Langmuir Vol. 37; no. 16; pp. 4943 - 4952 |
|---|---|
| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
27.04.2021
|
| Subjects | |
| Online Access | Get full text |
| ISSN | 0743-7463 1520-5827 1520-5827 |
| DOI | 10.1021/acs.langmuir.1c00271 |
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| Abstract | Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert toward biomolecular adsorption. Neutral hydrophilic brushes are normally considered to have static properties at a given temperature. As an example, PEG is not responsive to pH or ionic strength. Here we show that, by simply introducing a polymeric acid such as poly(methacrylic acid) (PMAA), the highly hydrated brush barrier can change its properties entirely. This is caused by multivalent hydrogen bonds in an extremely pH-sensitive process. Remarkably, it is sufficient to reduce the pH to 5 for complexation to occur at the interface, which is two units higher than in the corresponding bulk systems. Below this critical pH, PMAA starts to bind to PEG in large amounts (comparable to the PEG amount), causing the brush to gradually compact and dehydrate. The brush also undergoes major rheology changes, from viscoelastic to rigid. Furthermore, the protein repelling ability of PEG is lost after reaching a threshold in the amount of PMAA bound. The changes in brush properties are tunable and become more pronounced when more PMAA is bound. The initial brush state is fully recovered when releasing PMAA by returning to physiological pH. Our findings are relevant for many applications involving functional interfaces, such as capture–release of biomolecules. |
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| AbstractList | Polymer brushes are widely used to alter the properties of interfaces.
In particular, poly(ethylene glycol) (PEG) and similar polymers can
make surfaces inert toward biomolecular adsorption. Neutral hydrophilic
brushes are normally considered to have static properties at a given
temperature. As an example, PEG is not responsive to pH or ionic strength.
Here we show that, by simply introducing a polymeric acid such as
poly(methacrylic acid) (PMAA), the highly hydrated brush barrier can
change its properties entirely. This is caused by multivalent hydrogen
bonds in an extremely pH-sensitive process. Remarkably, it is sufficient
to reduce the pH to 5 for complexation to occur at the interface,
which is two units higher than in the corresponding bulk systems.
Below this critical pH, PMAA starts to bind to PEG in large amounts
(comparable to the PEG amount), causing the brush to gradually compact
and dehydrate. The brush also undergoes major rheology changes, from
viscoelastic to rigid. Furthermore, the protein repelling ability
of PEG is lost after reaching a threshold in the amount of PMAA bound.
The changes in brush properties are tunable and become more pronounced
when more PMAA is bound. The initial brush state is fully recovered
when releasing PMAA by returning to physiological pH. Our findings
are relevant for many applications involving functional interfaces,
such as capture–release of biomolecules. Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert toward biomolecular adsorption. Neutral hydrophilic brushes are normally considered to have static properties at a given temperature. As an example, PEG is not responsive to pH or ionic strength. Here we show that, by simply introducing a polymeric acid such as poly(methacrylic acid) (PMAA), the highly hydrated brush barrier can change its properties entirely. This is caused by multivalent hydrogen bonds in an extremely pH-sensitive process. Remarkably, it is sufficient to reduce the pH to 5 for complexation to occur at the interface, which is two units higher than in the corresponding bulk systems. Below this critical pH, PMAA starts to bind to PEG in large amounts (comparable to the PEG amount), causing the brush to gradually compact and dehydrate. The brush also undergoes major rheology changes, from viscoelastic to rigid. Furthermore, the protein repelling ability of PEG is lost after reaching a threshold in the amount of PMAA bound. The changes in brush properties are tunable and become more pronounced when more PMAA is bound. The initial brush state is fully recovered when releasing PMAA by returning to physiological pH. Our findings are relevant for many applications involving functional interfaces, such as capture-release of biomolecules.Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert toward biomolecular adsorption. Neutral hydrophilic brushes are normally considered to have static properties at a given temperature. As an example, PEG is not responsive to pH or ionic strength. Here we show that, by simply introducing a polymeric acid such as poly(methacrylic acid) (PMAA), the highly hydrated brush barrier can change its properties entirely. This is caused by multivalent hydrogen bonds in an extremely pH-sensitive process. Remarkably, it is sufficient to reduce the pH to 5 for complexation to occur at the interface, which is two units higher than in the corresponding bulk systems. Below this critical pH, PMAA starts to bind to PEG in large amounts (comparable to the PEG amount), causing the brush to gradually compact and dehydrate. The brush also undergoes major rheology changes, from viscoelastic to rigid. Furthermore, the protein repelling ability of PEG is lost after reaching a threshold in the amount of PMAA bound. The changes in brush properties are tunable and become more pronounced when more PMAA is bound. The initial brush state is fully recovered when releasing PMAA by returning to physiological pH. Our findings are relevant for many applications involving functional interfaces, such as capture-release of biomolecules. Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert toward biomolecular adsorption. Neutral hydrophilic brushes are normally considered to have static properties at a given temperature. As an example, PEG is not responsive to pH or ionic strength. Here we show that, by simply introducing a polymeric acid such as poly(methacrylic acid) (PMAA), the highly hydrated brush barrier can change its properties entirely. This is caused by multivalent hydrogen bonds in an extremely pH-sensitive process. Remarkably, it is sufficient to reduce the pH to 5 for complexation to occur at the interface, which is two units higher than in the corresponding bulk systems. Below this critical pH, PMAA starts to bind to PEG in large amounts (comparable to the PEG amount), causing the brush to gradually compact and dehydrate. The brush also undergoes major rheology changes, from viscoelastic to rigid. Furthermore, the protein repelling ability of PEG is lost after reaching a threshold in the amount of PMAA bound. The changes in brush properties are tunable and become more pronounced when more PMAA is bound. The initial brush state is fully recovered when releasing PMAA by returning to physiological pH. Our findings are relevant for many applications involving functional interfaces, such as capture–release of biomolecules. Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert toward biomolecular adsorption. Neutral hydrophilic brushes are normally considered to have static properties at a given temperature. As an example, PEG is not responsive to pH or ionic strength. Here we show that, by simply introducing a polymeric acid such as poly(methacrylic acid) (PMAA), the highly hydrated brush barrier can change its properties entirely. This is caused by multivalent hydrogen bonds in an extremely pH-sensitive process. Remarkably, it is sufficient to reduce the pH to 5 for complexation to occur at the interface, which is two units higher than in the corresponding bulk systems. Below this critical pH, PMAA starts to bind to PEG in large amounts (comparable to the PEG amount), causing the brush to gradually compact and dehydrate. The brush also undergoes major rheology changes, from viscoelastic to rigid. Furthermore, the protein repelling ability of PEG is lost after reaching a threshold in the amount of PMAA bound. The changes in brush properties are tunable and become more pronounced when more PMAA is bound. The initial brush state is fully recovered when releasing PMAA by returning to physiological pH. Our findings are relevant for many applications involving functional interfaces, such as capture-release of biomolecules. |
| Author | Bilotto, Pierluigi Valtiner, Markus Dahlin, Andreas Höök, Fredrik Andersson, John Ferrand-Drake del Castillo, Gustav |
| AuthorAffiliation | Department of Chemistry and Chemical Engineering Institute of Applied Physics, Group of Applied Interface Physics Department of Physics |
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| Author_xml | – sequence: 1 givenname: John orcidid: 0000-0002-2977-8305 surname: Andersson fullname: Andersson, John organization: Department of Chemistry and Chemical Engineering – sequence: 2 givenname: Gustav surname: Ferrand-Drake del Castillo fullname: Ferrand-Drake del Castillo, Gustav organization: Department of Chemistry and Chemical Engineering – sequence: 3 givenname: Pierluigi orcidid: 0000-0001-6531-8528 surname: Bilotto fullname: Bilotto, Pierluigi organization: Institute of Applied Physics, Group of Applied Interface Physics – sequence: 4 givenname: Fredrik orcidid: 0000-0003-1994-5015 surname: Höök fullname: Höök, Fredrik organization: Department of Physics – sequence: 5 givenname: Markus orcidid: 0000-0001-5410-1067 surname: Valtiner fullname: Valtiner, Markus organization: Institute of Applied Physics, Group of Applied Interface Physics – sequence: 6 givenname: Andreas orcidid: 0000-0003-1545-5860 surname: Dahlin fullname: Dahlin, Andreas email: adahlin@chalmers.se organization: Department of Chemistry and Chemical Engineering |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/33851532$$D View this record in MEDLINE/PubMed https://research.chalmers.se/publication/523882$$DView record from Swedish Publication Index |
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| Snippet | Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert... Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert... Polymer brushes are widely used to alter the properties of interfaces. In particular, poly(ethylene glycol) (PEG) and similar polymers can make surfaces inert... |
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| SubjectTerms | adsorption biochemical compounds hydrogen hydrogen bonding hydrophilicity ionic strength rheology temperature viscoelasticity |
| Title | Control of Polymer Brush Morphology, Rheology, and Protein Repulsion by Hydrogen Bond Complexation |
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