Design of new nanocellulose-based gas-carrier systems
Project code: PN-III-P4-PCE-2021-0435
PCE 77/2.06.2022
Abstract
Severe oxygen deprivation can cause significant problems in chronic wounds, during organ preservation and implantation, or in cases of trauma, hemorrhagic shock, or viral pneumonia. Oxygen prevents wound infection, increases cell viability after implantation and could be an effective treatment in viral pneumonia. Currently, there is no viable solution to deliver oxygen to the grafts during the healing period and to administrate a large volume of oxygen to patients who suffered profound oxygen deprivation. The scope of the CELGAS project is to develop innovative oxygen-carrying systems capable of supplying oxygen in a controlled manner to injured tissue/implants or intravenously. The innovative oxygen-carrying systems will ensure controlled release of oxygen for long periods of time, will have a high stability, biodegradability, will not be cytotoxic and will have a nanometric size, essential for intravenous administration to avoid vascular obstruction. In CELGAS, the problem will be addressed using nanocellulose and nanocellulose/biopolymer to encapsulate oxygen-generating species or to obtain oxygen-containing nanobubbles.
Main objective: development of innovative oxygen carrier systems capable of delivering oxygen in a controlled manner to the injured tissue/implant or intravenously. The innovative oxygen carrier systems will ensure a controlled release of oxygen over longer periods of time, will have high stability, biodegradability, lack of toxicity and, in the case of intravenous administration, a nanometric size.
Specific objectives:
a. Designing new oxygen carrier systems by incorporating active elements in nanocellulose or nanocellulose/biopolymer carriers;
b. Designing gas containing carrier systems;
c. Optimizing the active elements incorporating processes and selection of the viable alternatives for scaling-up to a higher technological level.
Phase I:
During this phase, oxygen-carrying systems capable of providing oxygen in the case of chronic wounds, during conservation and in the case of organ implantation or other trauma cases were designed and realized. The developed solution is based on the encapsulation of oxygen-generating species in a porous substrate of nanocellulose or functionalized nanocellulose. For this purpose, the nanocellulose was modified by TEMPO oxidation, by grafting of alkylsilane with long aliphatic chain, by grafting of poly(ethylene glycol) methyl ether methacrylate and poly(3-hydroxybutyrate) oligomers. The functionalization of nanocellulose was aimed at modifying the surface properties and imprinting the amphiphilic character for more efficient incorporation of oxygen-generating species. The efficiency of the functionalization was demonstrated by the morpho-structural, thermal and surface properties characterization. The selected oxygen-generating species were incorporated into the porous nanocellulose and functionalized nanocellulose substrates and the methodology for obtaining oxygen-carrying systems was elaborated. The oxygen-carrying systems were characterized and their properties were correlated with the treatment applied to the nanocellulose substrate. The research work of this phase was disseminated by publishing two articles, one in the International Journal of Biological Macromolecules (FI 8,025, Q1) and the other in Polymers (FI 4,967, Q1) and by communicating two papers, a poster and a award-winning oral communication. All the activities expected for this stage have been carried out.
Phase II:
In the second stage of the CELGAS project, new oxygen-carrying systems were created by embedding natural peroxides into nanocellulose (NC) modified with aliphatic polyester oligomers. These systems, along with those made in the previous phase, were tested for oxygen release of at both room and body temperature. The obtained results showed that a higher degree of amphiphilicity of the nanocellulose is beneficial for the release of oxygen, which was demonstrated by the tests at the temperature of 37°. The morpho-structural characterization of the modified NC with the aim of improving the amphiphilic character of the NC indicated an increase in the form factor and a more advanced defibrillation without changes in the crystalline structure. The results of the EPR analysis of these samples correlated with the observations regarding the oxygen release and, in addition, helped to establish the mechanisms governing the time release of oxygen. Also at this stage, it was studied the influence of the surface modification of nanocellulose on the stabilization of air/water systems, the results indicating that cellulose nanofibers with increased surface hydrophobicity and a higher form factor are able to form gels and stabilize more efficient the air/water systems. In addition, it was observed that NC grafted with aliphatic polyester oligomers allows the stabilization of air bubbles, the percentage of nanobubbles being determined by the process used for their obtaining.
Published articles:
1. D. M. Panaitescu, S. Stoian, A. N. Frone, G. M. Vlăsceanu, D. D. Baciu, A. R. Gabor, C. A. Nicolae, V. Radiţoiu, E. Alexandrescu, A. Căşărică, C.
Damian, P. Stanescu, Nanofibrous scaffolds based on bacterial cellulose crosslinked with oxidized sucrose, International Journal of Biological Macromolecules, 221, 2022, 381-397, https://doi.org/10.1016/j.ijbiomac.2022.08.189.
2. I. Chiulan, D. M. Panaitescu, A. Serafim, E. R. Radu, G. Ioniţă, V. Rădiţoiu, A. R. Gabor, C. A. Nicolae, M. Ghiurea, D. D. Baciu, Sponges from plasma treated cellulose nanofibers grafted with poly(ethylene glycol)methyl ether methacrylate. Polymers 14, 2022, 4720, https://doi.org/10.3390/polym14214720.
3. D. M. Panaitescu, A. N. Frone, C-A. Nicolae, A. R. Gabor, D. M. Miu, M-G. Soare, B. S. Vasile, I. Lupescu, Poly(3-hydroxybutyrate) nanocomposites modified with even and odd chain length polyhydroxyalkanoates, International Journal of Biological Macromolecules, 2023, 244, 125324.
4. G. M. Oprică, D. M. Panaitescu, B. E. Lixandru, C. D. Uşurelu, A. R. Gabor, C-A. Nicolae, R. C. Fierascu, A. N. Frone, Plant-derived nanocellulose with antibacterial activity for wound healing dressing, Pharmaceutics 2023, 15(12), 2672.
5. C-D. Uşurelu, A. N. Frone, G-M. Oprică, M. F. Raduly, M. Ghiurea, E. I. Neblea, C-A. Nicolae, M. Teodorescu, D. M. Panaitescu, Preparation and functionalization of cellulose nanofibers using a naturally occurring acid and their application in stabilizing linseed oil/water Pickering emulsions, submitted to International Journal of Biological Macromolecules.
6. D. M. Panaitescu, M. Oprea, B. Trica, I. Popa-Tudor, M. Ghiurea, C-A. Nicolae, A. R. Gabor, A. N. Frone, G. M. Oprica, C. D. Usurelu, D. Constantinescu-Aruxandei, F. Oancea, Poly(lactic acid) reinforced with cellulose nanofibers extracted from spent lignocellulosic substrate of Pleurotus, submitted to International Journal of Biological Macromolecules
Communications
1. C-D. Uşurelu, D. M. Panaitescu, S. Stoian, A. N. Frone, A. R. Gabor, C. A. Nicolae, E. Alexandrescu, Bacterial cellulose sponges obtained using a green crosslinker, Conferința Națională de Chimie, ediția a XXXVI-a, Calimaneşti, October 4-7, 2022 (poster)
2. C-D. Uşurelu, D. M. Panaitescu, A. N. Frone, A. R. Gabor, C. A. Nicolae, M. F. Raduly, M. Teodorescu, Obtaining poly(3-hydroxybutyrate) oligomers via the controlled thermal degradation of poly(3-hydroxybutyrate) in the presence of metal compounds, XVIII-th International Symposium PRIOCHEM “Priorities of Chemistry for a Sustainable Development” October 26-28, 2022 (award-winning oral communication).
3. C-D. Uşurelu, D. M. Panaitescu, A. N. Frone, A. R. Gabor, C-A. Nicolae, M. F. Raduly, M. Teodorescu, PHB oligomers obtained by controlled thermal degradation of PHB, Advanced Nano Materials Conference, University of Aveiro, Portugal, July 26-28, 2023 (virtual oral presentation)
4. C-D. Uşurelu, G-M. Oprica, E. I. Neblea, M. F. Raduly, C-A. Nicolae, A. R. Gabor, A. N. Frone, M. Teodorescu, D. M. Panaitescu, Throughout thermal characterization of ester-grafted nanocellulose, 7-th Central and Eastern European Conference on Thermal Analysis and Calorimetry, CEEC-TAC7, Brno, Cehia, August 28-31, 2023 (poster).
5. G. M. Oprica, C. D. Usurelu, A. N. Frone, R. Ianchis, D. M. Panaitescu, Nanofibrillated cellulose as a stabilizer of Pickering emulsions, 21st International Balkan Workshop on Applied Physics, Constanţa, Romania, July 11-14, 2023 (poster)
6. C-D. Uşurelu, G-M. Oprica, A. N. Frone, A. R. Gabor, C-A. Nicolae, D. M. Panaitescu, Effect of surface treated nanocellulose on the crystallization behavior of poly(3-hydroxybutyrate), 21st International Balkan Workshop on Applied Physics, Constanţa, Romania, July 11-14, 2023 (oral presentation)
7. C-D. Uşurelu, G-M. Oprica, A. N. Frone, C-A. Nicolae, D. M. Panaitescu, M. Teodorescu, Modification of nanocellulose’s surface by oxidation and silylation, NeXT-Chem V, Tehnologii inovatoare trans-sectoriale, May 22-23, 2023, Bucharest, Romania (oral presentation)
8. C-D. Uşurelu, G-M. Oprica, A. N. Frone, V. Raditoiu, A. R. Gabor, C-A. Nicolae, M. Teodorescu, D. M. Panaitescu, Nanocellulose grafted with oligomers obtained through the controlled thermal degradation of poly(3-hydroxybutyrate), POLY-K 2023 „Advances in polymer composites and nanocomposites”, Terni, Italy, September 13-15, 2023 (poster)
9. A. N. Frone, C. D. Usurelu, G. M. Oprica, A. R. Gabor, G. M. Teodorescu, C-A. Nicolae, D. Panaitescu, Tuning the properties of poly(3-hydroxybutyrate)/nanocellulose composites with bio-based polymeric lubricants, POLY-K 2023 „Advances in polymer composites and nanocomposites”, Terni, Italy, September 13-15, 2023 (poster)
10. C-D. Uşurelu, G-M. Oprica, M. F. Raduly, A. R. Gabor, C-A. Nicolae, A. N. Frone, M. Teodorescu, D. M. Panaitescu, Chemically modified nanocellulose for Pickering emulsions stabilization, POLY-K 2023 „Advances in polymer composites and nanocomposites”, Terni, Italy, September 13-15, 2023 (oral presentation)
11. C-D. Uşurelu, G-M. Oprică, A. N. Frone, E-I. Neblea, M. F. Raduly, A. R. Gabor, C-A. Nicolae, M. Teodorescu, D. M. Panaitescu, Preparation and functionalization of nanocellulose using lactic acid: morphostructural characterization and emulsifying capacity, “PRIORITIES OF CHEMISTRY FOR A SUSTAINABLE DEVELOPMENT” PRIOCHEM – XIXth Edition, Bucharest, Romania, October 11-13, 2023 (award-winning oral communication).
Diplomas/Awards
1. Diploma of excellence for the concept of the project “Design of new nanocellulose-based gas-carrier systems” – CELGA awarded within the 15th edition of the European Exhibition of Creativity and Innovation – Euroinvent 2023, Iași, Romania, 11-12 May
2. Silver medal for the concept of the project “Design of new nanocellulose-based gas-carrier systems” – CELGAS and Special Prize awarded by the Politehnica University of Timisoara in the 9th edition of the International Salon of Inventions and Innovations” Traian Vuia , Timisoara, Romania, June 15-17, 2023
- Dr. eng. Denis Mihaela Panaitescu
- Prof. dr. eng. Teodorescu Mircea
- Prof. dr. eng. Elena Gabriela Ionita
- Dr. eng. Adriana Nicoleta Frone
- Dr. eng. Valentin Rădițoiu
- Dr. eng. Zina Vuluga
- Dr. biochim. Iuliana Caras
- Dr. eng. Raluca Ianchis
- Dr. eng. Ioana Catalina Gîfu
- Drd. eng. George-Mihail Teodorescu
- Drd. eng. Andreea Afilipoaei
- Drd. eng. Catalina-Diana Usurelu
- Eng. Madalina Oprică
Dr. eng. Denis Mihaela Panaitescu
National Institute for Research & Development in Chemistry and Petrochemistry
