PN-III-P1-1.1-TE-2019-1573
PROJECT CODE: PN-III-P1-1.1-TE-2019-1573, contract number TE 101 ⁄ 2020
PROJECT TITLE:
Green chemistry route for the enzymatic cascade synthesis of biodegradable oligoesters
Sinteza enzimatica unor oligoesteri biodegradabili printr-un procedeu verde de tip cascada
ACRONYM: GREEN_POLYGEL
PROJECT COORDINATOR: Politehnica University of Timişoara
PROJECT DIRECTOR: Ș.l dr. ing. Anamaria Todea - 2020 / Ș.l. dr. ing. Iulia Maria Păușescu - 2021

BUDGET: 431.900 RON (Public budget)
START TIME: 15/09/2020
END TIME: 14/09/2022


PROJECT LAYOUT

Cascade reactions catalyzed by multienzymatic systems strongly increased the researchers interest due to their unique potential for the environmentally benign production of chemicals and materials. In recent years considerable progress has been made for one pot systems and the synthetic power of several enzymes was demonstrated. Vegetable oils represent important bio-based raw-materials for polymer synthesis due to their universal availability, low price and biodegradability. The main objective of the project is to develop an efficient green and cost-effective route for the biocatalytic synthesis in one-pot system starting from castor oil and bio-based furan monomers using a combination of two enzymes. The proposed reaction system involves an innovative three cascade reaction system catalyzed by two enzymes of different classes: (i) hydrolysis of triglycerides, (ii) glycerol oxidation and (iii) synthesis of oligoesters. All the purposed reactions will be mediated by tailor-made immobilized enzymes that are non-toxic, recyclable and eco-friendly biocatalysts, by using green solvents or solventless systems. The resulted biodegradable oligoesters will present new functionalities and properties. The enzyme stabilization will be performed by covalent binding and the selectivity will be evaluated in terms of maximal catalytic efficiency, to increase the productivity of the process. The reaction products will be characterized in detail by several analytical techniques for structure confirmation and assessment of the physico-chemical properties and their biodegradability rate will be evaluated by two methods. The synthesized monomers and oligoesters will be used as starting materials for novel organogels preparation.

PROJECT TEAM:
Project leader: Ș.l. dr.ing. Anamaria Todea-2020 / Ș.l. dr. ing. Iulia Maria Păușescu - 2021
Postdoctoral researchers:
Ș.l. dr. ing. Iulia Maria Păușescu
Conf. dr. ing. Ionuț Valentin Ledeți
Asist. Dr. chim. Diana Maria Dreavă (Aparaschivei)
Ș.l. dr. ing. Ana Maria Pană
PhD Students:
Drd. Ing. Ioan Bîtcan
Drd. Ing. Ioana Cristina Benea
Drd. Ing. Ionuț Mihai Tănase
Students:
Andreea Petrovici

 OBJECTIVE:
The main objective of the project is to obtain new oligoesters in one-pot system starting from castor oil and bio-based furan monomers by a complete green route, using a combination of two enzymes. All the purposed reactions will be mediated by tailor-made immobilized enzymes that are non-toxic, recyclable and eco-friendly biocatalysts, by using green solvents or solventless systems. The resulted biodegradable oligoesters will present new functionalities and properties.

STAGES
Stage 1 (2020, 4 months)- Enzymatic synthesis and optimization of glycerol conversion in glyceric and tartronic acids

Stage 2 (2021, 12 months)- Increasing the stability of laccases by immobilization for the synthesis of hydroxy acids from glycerol. Biotransformation of triricinolein from castor oil and furan derivatives in oligoesters in a "one-pot" system using immobilized laccases and lipases.

Stage 3 (2022, 8 months)- Enzymatic and microbial degradation a new oligoesters. Preparation and characterization of some organogels with two or three components.

DELIVERABLES:
Stage 1
Experimental methodology for enzymatic synthesis of glycerin acids using laccases.
Protocol for immobilization of laccases by covalent bonding.
Stage 1 report.
Stage 2
Grams amounts of immobilized laccase.
Experimental methodology for conversion of triricinolein to oligoesters using immobilized enzymes
Optimized experimental methodology for biotransformation of vegetables oils using immobilized lipases and laccases.
Experimental design methodology for synthesis of oligo-esters in the one-pot system.
Grams of synthesized oligo-esters.
Stage 2 report.
Abstracts for two presentations at scientific conferences.
A scientific article submitted for publication / accepted in the journal with impact factor indexed in the Web of Science database.
Stage 3
Laboratory methodology for enzymatic and microbial biodegradation of oligoesters.
Laboratory methodology for preparation and characterization of organogels.
A scientific article submitted for publication /accepted in the journal with impact factor,indexed in the Web of Science database.
Abstracts for two presentations at scientific conferences.
Stage 3 report
Final report.

RESULTS 2021

Publications:

  1. D. Dreavă, I.-C. Benea, I. Bitcan, A. Todea, E. Sisu, M. Puiu, F. Peter , Biocatalytic Approach for Novel Functional Oligoesters of ε-Caprolactone and Malic Acid, Processes 2021, 9(2), 232.
  2. A. R. Buzatu, A.t E Frissen, L. AM van den Broek, A. Todea, M. Motoc, C. G. Boeriu, Chemoenzymatic synthesis of new aromatic esters of mono-and oligosaccharides, Processes, 2020, 8, 12, 1638.

Conferences:

  1. I. Bîtcan, A. Petrovici, A.Todea, D. Aparaschivei, I. Păușescu, F. Peter, Green Route Synthesis of Oligoesters from 5-Hydroxymethyl-2-Furan Carboxylic Acid and Ricinoleic Acid, The 6th International Conference on Biocatalysis in Non-Conventional Media (BNCM 2021), 6-8 May 2021, Milan, Italy.
  2. I. Bîtcan, A. Petrovici, A. Ștefan, A. Todea, Iulia Păușescu, F. Peter, Selective glycerol oxidation mediated by covalently immobilized laccases, International Forum on Industrial Biotechnology and Bioeconomy- IFIB 2021, 30 September 2021 - 1 October 2021, Trento, Italy.
  3. I. Bitcan, A. Petrovici, A. Ștefan, A. Todea, I. Păușescu, F. Peter, Laccasses stabilization by covalent immobilization onto functionalized magnetic and sepabeads suports, New trends and strategies in the Chemistry of advanced materiais with relevance in bioloqical systems, tehnique and environmental protection" 13th Edition, online, 7-8 October 2021, Timisoara, Romania.
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