“IDEA” Project Cod: ID_1050

  
         
 
New class of nanobiomaterials obtained by tailoring organo-siloxanes interstitially imbedding lipid nanocapsules (LNC) with multifunctional properties
  
         
 
Project Manager:         

Prof. dr. Aurelia Meghea

   
Research Team:

Lecturer Dr. Nicoleta Badea
  Dr. Chem. Ioana Lacatusu
 

Ph.D. student Chem. Rodica Nita
  Ph.D. student Eng. Alina Murariu
   
   

Abstract
   

The aim of this project can be summarized as synthesis of new colloidal carriers able to offer not only a physical bio-encapsulating alternative for active biospecies, but also bioactive properties and enhanced electronic density by their interstitially imbedding in hybrid organo-siloxanic nanostructures. Taking into account the state-of-the-art in the field and prospective opened by this novel approach the project proposes the following objectives:
 
 
  • Evaluation of compatibility and of the specific interactions active biomolecule – template agent to be encapsulated into the siloxanic matrix.
  • Synthesis of nanosized colloidal bioencapsulated compounds (SLM and LNC) considering possible specific interaction between colloidal gel precursors and molecular structure of selected class of biomolecules.
  • Exhaustive characterization of prepared compounds during all the relevant synthetic steps by adequate techniques and also by some novel techniques for specific investigation at nanometric scale.
  • Obtaining and testing some novel photoprotective cosmetic formulations with enhanced antioxidant and anti-UV activity, of a siloxanic catalyst for pollution abatement.
  • Methodology set-up for kinetic and thermodynamic evaluation of selected bioencapsulated compounds with enhanced electronic density by Surface Plasmon Resonance and prospects for future research directions.
  
 

It can be concluded that the study of these highly organized systems and obtaining of nanostructures in some pre-defined spatial sites, both in structure and size, generically named as nanoreactors, offers actually unlimited possibilities for building new architectures, with unique character and specificity, resulting to new multi-functional composite materials, with pre-established properties and a vast applicative potential.

  
         
         
 

Project objectives (2007- 2010):

  
         
 
  • Documentary research with respect to controlled growing processes of nanoparticles;
  • Evaluation of interaction of couples active biomolecule – template agent/surfactant;
  • Synthesis of solid lipid microspheres  (SLM) and  solid lipid nanocapsules (LNC);
  • The selection of the most promising bioencapsulated colloidal nanocompounds;
  • Exhaustive characterization of organo-siloxanic nanostructured materials;
  • Obtaining and testing of some new sun protective cosmetic formulations with enhanced antioxidant and anti – UV activity;
  • Setting – up testing methodology by Surface Plasmon Resonance technique;
  • Obtaining and testing of a organo-siloxanic product with enhanced catalytic properties for pollution abatement;
  • The dissemination of results by scientific communications, articles published in impact reviews/journals. Publication of a scientific monograph.
  
     
 

Steps follwed to accomplish the objectives in the project plan:

  
     
 

1. Nano-structure synthesis
2. Surfactant - active biomolecule interaction
3. SLM, LNC synthesis
4. Modification of electronic properties of SLM and LNC
5. Exhaustive characterization    
6. Kinetics and thermodynamics evaluation of selected bioencapsulated compounds by Surface Plasmon Resonance
7. Products with different applications

  
     
 

Financial resources

  
     
 

Year

Amount [lei]

2007

55.000,0

2008

320.750,0

2009

250.750,5

2010

165.000,0

Total value

791.500,5
 
     
 

The involvement degree of young researchers

 
     
 

The degree of involvement of young scientists in research activity (2 PhD and 2 PhD students):

Dr. chem. Ioana Lacatusu

  • The compatibility evaluation of different classes of surfactants with various synthesis bio-molecules and vegetable provenience;
  • Self-asembling synthesis experiments by sol-gel tehnique and emulsification with high sher homogenisation;
  • DLS measurements (Nanosizer) in order to determine the size evolution of colloidal systems;
  • Exhaustive characterisation of silsesquioxane  nanostructures by microscopy (TEM, SEM, AFM);
  • Morphological evaluation of lipid nanoparticles by electronic transmission microscopy;
  • The obtining and testing of photoprotective cosmetic formulations with enhanced antioxidant and anti-UV properties.

Dr. eng. Nicoleta Badea

  • Characterisation by chemiluminescence method of antioxidant capacity of natural bioactive species and loaded bioactive species inside the lipid nanoparticles
  • The preparation of active vegetable extracts based on flavones and other polyphenolic compounds;
  • Exhaustive characterisation of organo-siloxanic nanostructures by UV-VIS-NIR, FT-IR and fluorescence;
  • Characterisation of lipid nanoparticles by UV-VIS and FT-IR spectroscopy;
  • The obtining and testing of some photoprotective cosmetic formulations with enhanced anti-UV and antioxidant properties by cuantification of Sun Protection Factor – SPF;
  • Thermal stability tests (by DSC analysis) and photochemical behaviour (controlled irradiation);

PhD students Rodica Nita

  • Literature study regarding the controlled growing of encapsulated compounds in different silica matrices;
  • Sol-gel experiments of silica and silsesquioxane matrices formation that involve competitive hydrolysis and polycondensation reactions;
  • Microsphere lipid synthesis with different organic compounds;
  • RPE spectra of organo-siloxan materials which contain paramagnetic species.

PhD students Alina Murariu

  • Documentary study on bioactive species selection to be encapsulated in different organo-siloxane matrices;
  • Encapsulation experiments of UV absorbents and vegetable extracts in lipid nanoparticles by high shear homogenisation technique;
  • Measurements of z potential elctrocinetic (using the DLS technique);
  • Preparation of thin films, based on organo-siloxane materials with different bioactive compounds, through dip and spin- coating.

 The reflection of the experience researches and those in training in staff expenses:

  
     
   
 

In this project two researchers have been engaged, from which one with experience (PhD Ioana Lacatusu) and one in training (PhD student Alina Murariu).

  
     
 

Objectivs, activities and achievement degree of the project

 
     
 

Year

Stage

Objective

Activities

Achievement degree

 

2007

Unique  I

1. Documentary study for  growing proceses of  nanoparticles

1.1. Literature study regarding the controlled growing of encapsulated compounds in different silica matrices

100 %

1.2. Selection of materials for organic-siloxane nanophases synthesis

2. Active biomolecule – surfactant interactions

2.1. Documentary study on bioactive species selection to be encapsulated in different organo-siloxane matrices;

100 %

2.2. The compatibility evaluation of different classes of surfactants with various synthesis bio-molecules

Total stage: 55.000

 

 

 

 

2008

Unique  II

1. Nanostructures synthesis with controlled sizes

1.1. Sol-gel experiments of silica and silsesquioxane matrices formation that involve competitive hydrolysis and polycondensation reactions

100 %

1.2. Dynamic Light Scattering measurements (Nanosizer) for evaluation of the size evolution of colloidal systems

1.3. Phototochemiluminometer aquisition

1.4. Information/documentation stage (1 week, Angers University, France)

1.5. RPE spectra of organo-siloxan materials which contain paramagnetic species

2. Solid lipid microsphere synthesis (SLM) and solid lipid nanocarriers (LNC)

 

 

2.1. Lipid microspheres synthesis with organic synthesis compounds

100 %

2.2. Amplificarea  proprietatilor electronice ale SLM si rearanjarea structurala, utilizand tehnica microemulsionarii

2.3. Prepararation of active vegetable extracts based on flavones and other polyphenols

2.4. Characterisation by chemiluminescence method of antioxidant capacity of natural bioactive species and surfactants couples

2.5. Encapsulation processes  – synthesis of lipid nanoparticles interstitial loaded

2.7. Results disseminations by Master and PhD cources, scientific communications, published papers in ISI journals; registration of a national patent demand

Total stage: 320.750

 

 

 

 

2009

 

 

Unique  III

1. The selection of the most promising nanometer bioencapsulated compounds

1.1. Evaluation and selection of materials by corroboration of the chemico-structural and toxicological characteristics

100 %

2. The characterisation of the intermediate encapsulation of SLM and NLC

2.1. Measurements of z potential elctrocinetic (using the DLS technique)

100 %

2.2. UV-VIS-NIR, FT-IR, Raman and  fluorescence analysis

2.3. Morphologic evaluation of powders (SEM, TEM)

3. Exhaustive characterisation of  nanostructurated organic-siloxane materials

3.1. Spectroscopic analysis (FT-IR, UV-VIS, Raman, fluorescence)

100 %

3.2. Microscopy: SEM, TEM, AFM

3.3. Results disseminations by published papers in ISI journals
Scientific monography publication

4. The obtining and testing of photoprotective cosmetic formulations with enhanced anti-UV activity

4.1. Thermal stability tests (by DSC analysis) and photochemical behaviour

100 %

4.2. Cuantification of Sun Protection Factor – SPF

Total stage: 250.750,5
 
     
 

Obtained results

 
     
 

I.Synthesis and characterisation of organo-siloxane nanostructures with controlled sizes (objectiv carried on 2008/2009 period):

  • Conceptual and experimental expertise in use of the soft-nanotechnologies for obtaining the self-organizing systems at nanometer scale by using different structural direction agents (agents template):
    • glucidic derivates (e.g. D-glucose, D-fructose, n-dodecyl-b-D-maltoside;
    • alkyl derivates of succinic anhydride;
    • conventional surfactants: amonium cuaternary salts, polyethylenglicol derivate.
  • The obtaining of new hybrid nanostructures with enhanced specific properties (fluorescence, antioxidant activity) containing various active natural extracts: Begonia flowers extract; orange peel extracts; ornamental bush extracts; green tea extracts.

II. Synthesis and characterisation of microsphere/solid lipid nanoparticles (SLM/SLN) and solid lipid nanocarriers (NLC) (objective carried on in 2009)

  • The efficiency of complex mixtures of surfactants and biocompatibile lipids in two types of lipid nanostructures (SLN and NLC):
    • Surfactants mixture: polyethylenglicol derivates, bloc copolimers, lechitin, polyglicoside derivates etc.)
    • Lipid mixture: glyceril stearate, cetyl palmitate, olive oil;
    • Compounds/liophile mixtures: sunscreen (e.g. octylmetoxycinamate, octocrylen and bemotrisinol); systems with antioxidant activity (e.g. Rosmarin extract obtined from Rosmarinus officinalis L.).
  • Development of cosmetic formulation by introduction of lipid nanoparticles loaded with UV absorbers in a model base cream provided by S.C. Elmiplant.

The obtained results have led to achieve all objectives and activities proposed in the implementation plan of the project. These results have provided a real perspective towards hybrid silica nanostructures and lipid nanoparticles synthesis with amplified properties that contain in their composition organic compounds molecules with active principles and UV absorbers (compounds with fluorescent, antioxidant and anti UV properties) loaded in biocompatibile host matrices. The obtained products may open new directions for applying in biomedical field.

  
     
 

Published papers:

 
     
 
  • Lacatusu I., Badea N., Nita R., Murariu A., Miculescu F., Iosub I., Meghea A., “Encapsulation of fluorescence vegetable extracts within a templated sol – gel matrix”, Optical Materials, Elsevier, 2010, 32, 711-718, www.elsevier.com/locate/optmat;
  • Lacatusu I., Badea N., Bojin D., Iosub I., Meghea A., “Silica polymeric networks templated with D-fructose – as host matrices for natural extracts immobilization”, Molecular Crystals and Liquid Crystals, acceptat spre publicare, 2010, http://www.tandf.co.uk/journals/titles/1058725x.html;
  • Lacatusu I., Badea N., Bojin D., Iosub S., Meghea A., “Novel fluorescence nanostructured materials obtained by entrapment of an ornamental bush extract in hybrid silica glass”, Journal of Sol-Gel Science and Technology, 2009, 51(1), 84-91, http://www.springer.com/materials/special+types/journal;
  • Lacatusu I., Badea N., Nita R., Giurginca M., Bojin D., Iosub I., Meghea A., “Synthesis of high fluorescent silica hybrid materials by immobilization of orange peel extract in silica-silsesquioxane matrix”, Journal of Organic-Physics Chemistry, 2009, 22, 1015-1021, http://www..interscience.wiley.com;
  • Lacatusu I., Badea N., Giurginca M., Garcia C.V., Sahraoui B., Meghea A., “Synthesis and properties of hybrid glass nanomaterials prepared by entrapping of green tea extract in sol-gel templated matrices”, Journal of Optoelectonics and Advanced Materials-Symposia, 1(6), 2009, p. 1040-1046, http://www.infim.ro/~roam/index.php;
  • Bărbinţă Pătraşcu M.E., Badea N., Ţugulea L., Meghea A., “Photo-Oxidative Stress on Model Membranes – Studies by Optical Methods” Key Engineering Materials, 2009, 415, 29-32, http://www.scientific.net/KEM.415;
  • Lacatusu I., Nita R., Badea N., Bojin D., Meghea A., “The role of silsesquioxane compounds used as „building blocks” in sol – gel nanoencapsulation of retinyl palmitate”, Materials Research Innovations, 2009, 13(3), 330-333, http://www.ingentaconnect.com/content/maney/mri/2009;
  • Lacatusu I., Badea N., Meghea A. “Effect of surfactants on stability of colloidal sols as precursors in sol-gel encapsulation”, Key Engineering Materials, 2009, 415, 57-60, http://www.scientific.net/KEM.415;
  • Bărbînţă-Pătraşcu M.E., Badea N., Ţugulea L.G., Giurginca M., Meghea A.  ,,Oxidative stress simulation on artificial membranes – chemiluminescent studies”, Rev. Chem.,2008, 59, 8, 834-837, http://www.revistadechimie.ro.
 
     
 

Other results

 
     
 
  • Scientific monography. A. Meghea, I. Lacatusu, N. Badea, R.Nita, A. Murariu, Controlled synthesis of nanostructures for materials with multifunctional properties. Vol. 1. Nanostructured self-assembled systems. Ed. Politehnica Press, 2009, 514 p., ISBN 978-606-515-048-5;
  • A chapter contribution (80 pg.) in an international book “Biocompatible Nanomaterials: Synthesis, Characterization and Application in Analytical Chemistry”, edited by Sea-Fue Wang, Nova Publisher, in press, 2010; “Nanoencapsulation of natural products with multifunctional properties in silica and hybrid organic – silica host matrices" authors: I. Lacatusu, N. Badea and A. Meghea, https://www.novapublishers.com/catalog/product_info.php?products_id=14962&osCsid=f69911d1aa871dbc0a657a31e6462684;
  • National Patent. „Immobilisation procedure of orange peel extract in silica-silsesquioxane hybrid host matrices”, authors: A. Meghea, I. Lacatusu, M. N. Badea, M.R. Nita, I. Iosub, registered demand at 16.09.2008, A/00719.