Design of new nanocellulose-based gas-carrier systems

Project code: PN-III-P4-PCE-2021-0435

PCE 77/2.06.2022

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. Uşurelu, C.D.; Panaitescu, D.M.; Oprică, G.M.; Nicolae, C.-A.; Gabor, A.R.; Damian, C.M.; Ianchiş, R.; Teodorescu, M.; Frone, A.N. Effect of Medium-Chain-Length Alkyl Silane Modified Nanocellulose in Poly(3-hydroxybutyrate) Nanocomposites. Polymers 2024, 16, 3069. https://doi.org/10.3390/polym16213069

6. Uşurelu, C.D.; Frone, A.N. Oprică, G.M.; Raduly, M.F.; Ghiurea, M.; Neblea, E.I.; Nicolae, C.-A.; Filip, X.; Teodorescu, M.S.; Panaitescu, D.M. Preparation and functionalization of cellulose nanofibers using a naturally occurring acid and their application in stabilizing linseed oil/water Pickering emulsions. International Journal of Biological Macromolecules 2024, 262, Part 1, 129884, ISSN 0141-8130, https://doi.org/10.1016/j.ijbiomac.2024.129884.

7. Panaitescu, D.M., Oprea, M., Frone, A.N. et al. Valorization of Spent Lignocellulosic Substrate of Edible Mushrooms into Cellulose Nanofibers for Bionanocomposites Production. J Polym Environ 2024, 32, 6618–6635. https://doi.org/10.1007/s10924-024-03378-3.

8.  Frone, A.N.; Panaitescu, D.M.; Gabor, A.R.; Nicolae, C.A.; Bradu, C. Poly(3-hydroxybutyrate) modified with thermoplastic polyurethane and microfibrillated cellulose: hydrolytic degradation, thermal and mechanical properties. Polymers 2024, under review


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).

12. C.D. Usurelu, A.N. Frone, D.M. Panaitescu, G.M. Oprica, C.A. Nicolae, G. Ionita, I. Caras, M.S. Teoodrescu, Nanocellulose-based oxygen-generating

systems, The 7th International Conference New Trends in Sensing – Monitoring – Telediagnosis for Life Sciences NT-SMT-LS 2024, September 20 – 22 , 2024 Brașov, Romania, online (award-winning young research oral communication)

13. G.M. Oprica, C.D. Usurelu, A.N. Frone, C. Firinca, C.A. Nicolae, R.C. Fierascu, D.M. Panaitescu, The effect of cellulose nanofibers’ concentration on the behavior of nanoemulsions, Applications of Chemistry in Nanosciences and Biomaterials Engineering (NanoBioMat), November 27-29, Bucharest, (online – oral communication)

14. A.N. Frone, C.D. Usurelu, G.M. Oprica, M.F, Raduly, C.A. Nicolae, M. Ghiurea, B. Trica, D.M. Panaitescu. Nanocellulose isolated from agro-industrial residue for biopolymers reinforcement, Polymers 2024—Polymers for a Safe and Sustainable Future, May 28-31, Athens, Greece (poster)

15.    G.M. Oprica, C.D. Usurelu, C.A. Nicolae, I.E. Neblea, R.C. Fierăscu, D.M. Panaitescu, A.N. Frone, Pickering emulsions stabilized using curcumin-loaded TEMPO-oxidized nanocellulose, Polymers 2024—Polymers for a Safe and Sustainable Future, May 28-31, Athens, Greece (poster)

16. C.D. Usurelu, G.M. Oprica, A.N. Frone, V. Raditoiu, C.A. Nicolae, C. Stavarache, M.S. Teodorescu, D.M. Panaitescu, Nanocellulose functionalized with oligomers of aliphatic polyesters for increased compatibility with biopolymeric matrices. Polymers 2024—Polymers for a Safe and Sustainable Future, May 28-31, Athens, Greece (poster)

17.    D.M. Panaitescu, A.N. Frone, G.M. Oprica, C.D. Usurelu, A.R. Gabor, C.A. Nicolae, B.E. Lixandru, V. Satulu, S. Vizireanu, Layered dressings from biopolymers and natural antibacterial products, Polymers 2024—Polymers for a Safe and Sustainable Future, May 28-31, Athens, Greece (poster)

18. C.D. Usurelu, D.M. Panaitescu, M.S. Teodorescu, G.M. Oprica, G. Ionita, C.A. Nicolae, I. Caras, V. Raditoiu, A.N. Frone. Surface-modified cellulose nanofibers as a carrier for oxygen generating compounds, The International Symposium “Priorities of chemistry for a sustainable development” PRIOCHEM, XXth edition 16-18 October 2024, Bucharest, Romania, Book of Abstracts no. 20/2024, pag. 53, ISSN 2601 – 4203 and ISSN-L 2601 – 4181 – poster

Workshop

1. Round table New oxygen-carrying systems based on nanocellulose for wound healing organized within The International Symposium “Priorities of chemistry for a sustainable development” PRIOCHEM, XXth edition 16-18 October 2024, Bucharest, Romania, Book of Abstracts no. 20/2024, pag. 78, ISSN 2601 – 4203 and ISSN-L 2601 – 4181

Patents

1. D.M. Panaitescu, F. Oancea, G.M. Oprica, A.N. Frone, D. Constantinescu Aruxandei, B. Trică, C.A. Nicolae, A.R. Gabor, Process for obtaining cellulose nanofibers from lignocellulosic waste and method of using them to obtain bionanocomposites – patent application no. A 2024 -00186/17.04.2024.

2.     D.M. Panaitescu, A.N. Frone, A.R. Gabor, C-D. Uşurelu, G.M. Oprica, C. A. Nicolae, D. Radu. Natural endoperoxides nanocarriers and process to obtain them Nanopurtători cu endoperoxid natural şi procedeu de obţinere a acestora



Diplomas/Awards

1. Diploma of excellence for the concept of the project “Design of new nanocellulose-based gas-carrier systems” – CELGAS 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

3. Silver medal for “Design of new nanocellulose-based gas-carrier systems” – CELGS awarded within Inova 2024 – 48th International Invention Show, October 16-19, Zagreb, Croatia

4.    Silver medal for “Process for obtaining cellulose nanofibers from lignocellulosic waste and method of using them to obtain bionanocomposites – patent application no. A 202 – 00186/17.04.2024 awarded within Inova 2024 – 48th International Invention Show, October 16-19, Zagreb, Croatia

5.  Gold medal for “Process for obtaining cellulose nanofibers from lignocellulosic waste and method of using them to obtain bionanocomposites – patent application no. A 202 – 00186/17.04.2024 awarded within 16th edition of the European Exhibition of Creativity and Innovation – EUROINVENT 2024, May 6-8 , Iași, Romania.

6.    Silver medal for “Process for obtaining cellulose nanofibers from lignocellulosic waste and method of using them to obtain bionanocomposites – patent application no. A 202 – 00186/17.04.2024 awarded within America Invention Innovation Expo, August 26-28 2024, U.S.A.

7.     Gold medal for “Process for obtaining cellulose nanofibers from lignocellulosic waste and method of using them to obtain bionanocomposites – patent application no. A 202 – 00186/17.04.2024 awarded within ITE 2024 – International Invention & Trade Expo, September 24-25 2024, London  

8. Silver medal for the concept of the project “Design of new nanocellulose-based gas-carrier systems” – CELGAS awarded within Saudi Global Inventions and Innovations Expo – SGiE 2024, November 5 – 8, Jeddah, Saudi Arabia

9.    Gold medal for “Process for obtaining cellulose nanofibers from lignocellulosic waste and method of using them to obtain bionanocomposites – patent application no. A 202 – 00186/17.04.2024 awarded within Saudi Global Inventions and Innovations Expo – SGiE 2024, November 5 – 8, Jeddah, Saudi Arabia

10.   “Process for obtaining cellulose nanofibers from lignocellulosic waste and method of using them to obtain bionanocomposites – patent application no. A 202 – 00186/17.04.202 KAOHSIUNG INTERNATIONAL INVENTION and Design EXPO – KIDE 2024, December 5-7, Kaohsiung, Taiwan

11. Gold medal for the “Design of new nanocellulose-based gas-carrier systems” – CELGAS awarded within ITE 2024 – International Invention & Trade Expo, September 24-25 2024, London



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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.

Objectives

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.

Results

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.

Phase III

During the third stage of the project, oxygen-carrying systems based on biopolymers and a natural endoperoxide capable of releasing both reactive oxygen species and molecular oxygen were developed.  These systems have applications in treating many conditions, especially chronic wounds that often suffer from insufficient oxygen supply and have an increased risk of infections. The innovative solution consisted in the design and manufacture of carrier nanospheres that would encapsulate air or oxygen inside, with potential in treating hypoxia, and in the outer shell, of biopolymeric nature, a natural endoperoxide, which decomposes with the release of reactive oxygen species with antibacterial, antiviral, antifungal, anti-inflammatory and anticancer action. The newly obtained systems are particularly important in the ongoing problems related to the increased antibiotic and antiviral resistance of bacteria and viruses. The emulsification solvent-evaporation technique was used as a method for manufacturing the nanospheres, and various homogenization methods (such as mechanical agitation, ultrasonication, intensive homogenization, and/or microfluidization) were used individually or in combination to obtain the emulsions. The efficiency of the prepared systems in the gradual and controlled release of molecular oxygen was demonstrated using an optical oxygen sensor, which quantified the amount of oxygen dissolved in water over time. In vivo tests performed by spraying the selected systems directly onto the wound site infected with methicillin-resistant Staphylococcus aureus demonstrated the ability of the materials obtained in this project to rapidly heal infected wounds.


Publications
Project Team
  • 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
Contact

Dr. eng. Denis Mihaela Panaitescu

National Institute for Research & Development in Chemistry and Petrochemistry