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Atomistic mechanisms and predictive modeling of biomolecular adsorption on nanomaterial surfaces
Stockholm University, Faculty of Science, Department of Chemistry.ORCID iD: 0009-0004-0000-3962
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Molecular simulations provide detailed insight into how biomolecules interact with nanomaterial surfaces. However, quantitative adsorption calculations are computationally demanding, and experimental measurements alone rarely reveal the molecular mechanism of binding. This type of molecular-level understanding is often essential for guiding the design of nanomaterials with improved safety and performance in technological and medical applications. This thesis combines atomistic molecular dynamics, enhanced sampling methods, machine learning, and quartz crystal microbalance with dissipation monitoring to develop a mechanistic and predictive description of adsorption at nano-bio interfaces. Adsorption free energies were computed for a broad set of biomolecular building blocks on flat and curved ZnS nanostructures, both pristine and polymer-coated, showing how curvature, hydration structure, and polymer layers affect adsorption affinities. Building on this and on the results of previous studies, a consistently generated dataset of adsorption free energies for biomolecular fragments on various nanomaterial surfaces was analyzed using statistical machine-learning tools, revealing that biomolecules and nanomaterials cluster into a few chemically significant classes and that adsorption behavior can be reproduced using a reduced set of representative fragments in simple linear models. The thesis then shifts attention from individual fragments to short peptides, examining how the order of amino acids in a peptide sequence collectively governs adsorption behavior onto TiO2. Extensive MD simulations of sequence permutations of the titanium-binding peptide (min-TBP-1) show how the spatial arrangement of charged and polar residues, together with ion-mediated interactions, determines adsorption affinity, conformational adaptation, and preferred sequence motifs. Finally, a subset of these peptides was studied using enhanced sampling and QCM-D experiments, providing quantitative adsorption free energies and complementary information on adsorption kinetics. The comparison between computed free energies and experimentally derived binding offers a more complete picture of sequence-specific peptide adsorption. Together, these studies advance the molecular understanding of nano-bio interfaces and outline practical strategies for predicting and tailoring biomolecular adsorption on nanomaterials.

Place, publisher, year, edition, pages
Stockholm: Department of Chemistry, Stockholm University , 2026. , p. 78
Keywords [en]
Nanomaterials, ZnS, TiO2, Adsorption free energy, Molecular dynamics simulations, QCM-D
National Category
Physical Chemistry Theoretical Chemistry
Research subject
Physical Chemistry
Identifiers
URN: urn:nbn:se:su:diva-250844ISBN: 978-91-8107-486-4 (print)ISBN: 978-91-8107-487-1 (electronic)OAI: oai:DiVA.org:su-250844DiVA, id: diva2:2025539
Public defence
2026-02-20, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B and online via Zoom, public link is available at the department website, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2026-01-28 Created: 2026-01-07 Last updated: 2026-01-28Bibliographically approved
List of papers
1. Biomolecular Adsorprion at ZnS Nanomaterials: A Molecular Dynamics Simulation Study of the Adsorption Preferences, Effects of the Surface Curvature and Coating
Open this publication in new window or tab >>Biomolecular Adsorprion at ZnS Nanomaterials: A Molecular Dynamics Simulation Study of the Adsorption Preferences, Effects of the Surface Curvature and Coating
2023 (English)In: Nanomaterials, E-ISSN 2079-4991, Vol. 13, no 15, article id 2239Article in journal (Refereed) Published
Abstract [en]

The understanding of interactions between nanomaterials and biological molecules is of primary importance for biomedical applications of nanomaterials, as well as for the evaluation of their possible toxic effects. Here, we carried out extensive molecular dynamics simulations of the adsorption properties of about 30 small molecules representing biomolecular fragments at ZnS surfaces in aqueous media. We computed adsorption free energies and potentials of mean force of amino acid side chain analogs, lipids, and sugar fragments to ZnS (110) crystal surface and to a spherical ZnS nanoparticle. Furthermore, we investigated the effect of poly-methylmethacrylate (PMMA) coating on the adsorption preferences of biomolecules to ZnS. We found that only a few anionic molecules: aspartic and glutamic acids side chains, as well as the anionic form of cysteine show significant binding to pristine ZnS surface, while other molecules show weak or no binding. Spherical ZnS nanoparticles show stronger binding of these molecules due to binding at the edges between different surface facets. Coating of ZnS by PMMA changes binding preferences drastically: the molecules that adsorb to a pristine ZnS surface do not adsorb on PMMA-coated surfaces, while some others, particularly hydrophobic or aromatic amino-acids, show high binding affinity due to binding to the coating. We investigate further the hydration properties of the ZnS surface and relate them to the binding preferences of biomolecules.

Keywords
zinc sulfide, surface properties, biomolecular adsorption, molecular dynamics
National Category
Nano Technology Materials Engineering Physical Sciences Physical Chemistry
Identifiers
urn:nbn:se:su:diva-221114 (URN)10.3390/nano13152239 (DOI)001046278000001 ()37570556 (PubMedID)2-s2.0-85167657281 (Scopus ID)
Available from: 2023-09-19 Created: 2023-09-19 Last updated: 2026-01-07Bibliographically approved
2. Biomolecular Adsorption on Nanomaterials: Combining Molecular Simulations with Machine Learning
Open this publication in new window or tab >>Biomolecular Adsorption on Nanomaterials: Combining Molecular Simulations with Machine Learning
2024 (English)In: Journal of Chemical Information and Modeling, ISSN 1549-9596, E-ISSN 1549-960X, Vol. 64, no 9, p. 3799-3811Article in journal (Refereed) Published
Abstract [en]

Adsorption free energies of 32 small biomolecules (amino acids side chains, fragments of lipids, and sugar molecules) on 33 different nanomaterials, computed by the molecular dynamics - metadynamics methodology, have been analyzed using statistical machine learning approaches. Multiple unsupervised learning algorithms (principal component analysis, agglomerative clustering, and K-means) as well as supervised linear and nonlinear regression algorithms (linear regression, AdaBoost ensemble learning, artificial neural network) have been applied. As a result, a small set of biomolecules has been identified, knowledge of adsorption free energies of which to a specific nanomaterial can be used to predict, within the developed machine learning model, adsorption free energies of other biomolecules. Furthermore, the methodology of grouping of nanomaterials according to their interactions with biomolecules has been presented.

National Category
Biophysics Theoretical Chemistry Physical Chemistry
Identifiers
urn:nbn:se:su:diva-229076 (URN)10.1021/acs.jcim.3c01606 (DOI)001203614700001 ()38623916 (PubMedID)2-s2.0-85190749149 (Scopus ID)
Available from: 2024-05-07 Created: 2024-05-07 Last updated: 2026-01-07Bibliographically approved
3. Uncovering sequence effects in Titanium binding peptides adsorption on TiO2: A molecular dynamics study
Open this publication in new window or tab >>Uncovering sequence effects in Titanium binding peptides adsorption on TiO2: A molecular dynamics study
2025 (English)In: Scientific Reports, E-ISSN 2045-2322, Vol. 15, article id 26885Article in journal (Refereed) Published
Abstract [en]

Titanium binding peptides are useful tools for material functionalization in both biomedical and nanotechnology applications because of their ability to attach selectively to titanium surfaces. In this work, we investigate the adsorption behavior of a series of 360 six amino acids long peptides obtained by permutations of titanium binding peptide residues, RKLPDA, on hydroxylated anatase TiO2 (101) surfaces using extensive atomistic molecular dynamics (MD) simulations, with the purpose identifying sequences with stronger adsorption affinity to titanium. Our results show that small changes in amino acid order can significantly affect both binding strength and structural conformations. Peptides with arginine at the N-terminus and lysine or aspartic acid near the C-terminus tended to exhibit more stable adsorption. The clustering and radial distribution function (RDF) analyzes revealed different binding modes and key atomic interactions, with nitrogen-containing groups and, in some cases, Na+ ions playing a significant role in the anchoring of peptides to the surface. These findings suggest a detailed sequence-level understanding of peptide-TiO2 interactions and can guide the design of improved peptides for titanium functionalization.

Keywords
Adsorption, Molecular dynamics, Peptides, Titanium dioxide
National Category
Physical Chemistry
Identifiers
urn:nbn:se:su:diva-245445 (URN)10.1038/s41598-025-10966-3 (DOI)001537443500019 ()40707617 (PubMedID)2-s2.0-105011494628 (Scopus ID)
Available from: 2025-08-14 Created: 2025-08-14 Last updated: 2026-01-07Bibliographically approved
4. Adsorption of titanium binding peptides on TiO2: Quartz crystal microbalance and molecular dynamics simulations studies
Open this publication in new window or tab >>Adsorption of titanium binding peptides on TiO2: Quartz crystal microbalance and molecular dynamics simulations studies
(English)Manuscript (preprint) (Other academic)
National Category
Physical Chemistry Theoretical Chemistry Analytical Chemistry Materials Chemistry
Research subject
Physical Chemistry; Analytical Chemistry; Materials Chemistry
Identifiers
urn:nbn:se:su:diva-251293 (URN)
Available from: 2026-01-16 Created: 2026-01-16 Last updated: 2026-01-19

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