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Soft, Small, and Smart: Design, Assembly, and Dynamics of Novel Nanoparticles for Novel Industrial
Applications

Final Report Summary - NANOS3 (Soft, Small, and Smart: Design, Assembly, and Dynamics of Novel Nanoparticles for Novel IndustrialApplications)

Project Coordinator: Dr. Imre Varga, Institute of Chemistry, Eötvös Loránd University, Budapest,
Hungary
Project webpage: http://www.nanos3.eu

Summary of The Project Objectives
NanoS3 is a multi-site Initial Training Network of 13 Early Stage Researchers (ESRs) at ten host organizations consisting of 8 academic and 2 industrial partners. The academic partners provided complementary expertise in synthesis, modelling and characterization techniques. They were joined by two industrial partners active either in the development of novel luminescent materials (LuminoChem), or in the home and personal care sectors (Procter and Gamble). In addition three associated partners helped the work of our ITN: an SME in the field of stem-cell research, a world-leading research institute from Sweden and a research group from from the Republic of Korea.

The main objective of NanoS3 was to train and promote qualified researchers in the field of soft matter nanoscience, capable to work in research or industry together with experts in different disciplines and in different countries. Since natural and synthetic macromolecules are among the most versatile building blocks in soft nanotechnology the main theme of our ITN was to develop hierarchical polymer nanoparticles, with tailored composition and functionalities. Furthermore, current understanding of polymer nanoparticles is mostly related to their equilibrium structures, whereas the kinetic aspects of the particle formation and the internal dynamics of the formed structures have been far less investigated. NanoS3 strived to study such structural dynamics.
NanoS3 aimed at reaching the following overall research objectives:
O1: Developing novel synthetic approaches for hierarchically structured, responsive nanoparticles.
O2: Elucidating the internal dynamics of domains of soft nanoparticles and to control the formation of specific products in non-equilibrium self-assembly processes.
O3: Clarifying the effect of adsorption at an interface and confinement between two surfaces on the structure and response dynamics of the hierarchical nanoparticles.

Description of the work performed during the project
TRAINING ACTIVITIES
All fellows have been enrolled in local PhD schools. These local trainings were complemented by the network-wide training activities coordinated and organized by NanoS3. Seven training events were organized during the lifetime of the ITN, which were planned to provide in depth fundamental understanding of soft materials as well as a theoretical and practical introduction to synthetic and characterization methods used in the field. The scientific trainings were accompanied by four Complementary trainings (e.g. on scientific project management, research integrity, writing and presentation skills) and a Workshop. ESRs also took part in secondments. Five ESRs have already obtained their Ph.D. and the others are expected to submit their Ph.D. thesis in the near future.

MAIN SCIENTIFIC RESULTS
Our main objectives were achieved by carrying out thirteen individual but strongly inter-related projects. Some of the main results are summarized below:
-A wide variety of diblock and triblock copolymers were synthetized.
-Novel responsive host-guest complexes were prepared.
-A novel single pot synthetic method was developed to prepare core/shell microgel particles.
-Polymers with tuned hydrophobicity were prepared.
-Polymer-DFT codes were implemented for the modelling of pH and temperature responsive polymer/polyelectrolyte solutions.
-Various block copolymers were used to create polymer nanoparticles, and complexes.
-Electrostatic and host/guest interactions as well as chemical coupling were used to create hierarchically organized responsive microgel particles and composite gels.
-Modelling tools were developed to investigate the self-assembly of responsive block coplymers.
-Novel approaches for the triggered self-assembly of soft nanoparticles and macrogels were developed.
-The effect of flow conditions on the non-equilibrium aggregate formation was studied.
-Structural and dynamic changes in soft nanoparticles were successfully coupled to release.
-The response kinetics of microgel particles adsorbed on PEI monolayer was investigated. A simple chemical coupling was developed to regain the fast response kinetics of the surface bound microgels.
-The effect of bulk nanostructure and charge density on the interfacial structure was investigated using polymersomes, worm-like and spherical micelles.
-Lipid mesophases were characterized and used for studying interfacial dynamics of water layers.
-Three different non-equilibrium mechanisms by which bulk aggregates directly modify the interfacial structure and morphology of an oppositely charged polyelectrolyte/surfactant (P/S) mixture were described. A novel approach to prepare fully elastic polyelectrolyte/surfactant films at the air/water interface by spreading aqueous dispersions of the P/S aggregates was developed.
-A wall-jet flow cell was interfaced with an evanescent wave Raman spectrometer to study the adsorption polymers at silica surfaces. The theory for analyzing the data was developed and applied to investigate the structural changes of polymer films and their interaction with cargo’ molecules.
-Two biomacromolecules, cartilage oligomeric matric protein (COMP) and lubricin are known to co-localize at the cartilage surface. It was demonstrated that COMP and lubricin self-assemble at interfaces, and the self-assembled layers show enhanced lubrication performance.
-A mathematical model was constructed and programmed to calculate Raman scattering peak intensities as a function of molecular orientation of the scattering moiety. It was applied to correlate structural changes in confined films to macroscopic modulations such as pressure and shear.
-The lubrication properties of self-assembly structures formed by biopolyelectrolytes and biosurfactants and host/guest nanocomplexes were studied. The combined action of load and shear was investigated and the results were correlated to the dynamic structure and self-healing.

DISSEMINATION
The results of the ITN were already published in 43 peer-reviewed papers and currently an additional 28 papers are in preparation or planned. Our results were also presented at numerous international conferences. 20 oral and 54 poster presentations were given by our ESRs. They also participated at various science fares, and gave popular science presentations.

Final Results and Their Potential Impact and Use
The NanoS3 network contributed substantially to the development of novel methods to create hierarchical nanostructures and to develop understanding how confinement between two surfaces affects the structure and response dynamics of soft nanostructures. Our results are related to fields such as nano-encapsulation, triggered release, creating complex dynamic soft nanostructures, which in turn are the foundation of developing e.g. drug delivery systems, regenerative medicine, intelligent household and personal care products or paints. Thus, it is expected that NanoS3 results will have a significant future impact in these fields benefitting the society and the environment. In addition thirteen well trained young scientists are joining academia and industry to find solutions for the burning questions in soft matter and biomedical research.