Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study

Molecularly imprinted polymers (MIP) have garnered significant interest as drug delivery system (DDS) in recent years. The conventional thermal heating and one-variable-at-a-time method for synthesising MIP and rebinding capacity evaluation is resource- and time-consuming. Thus, this study focused o...

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Main Author:	Vannessa, Lawai
Format:	Thesis
Language:	English
Published:	2024
Subjects:	QD Chemistry
Online Access:	http://ir.unimas.my/id/eprint/45978/3/Thesis_PhD_Vannessa.pdf
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id	my-unimas-ir.45978
record_format	uketd_dc
institution	Universiti Malaysia Sarawak
collection	UNIMAS Institutional Repository
language	English
topic	QD Chemistry
spellingShingle	QD Chemistry Vannessa, Lawai Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study
description	Molecularly imprinted polymers (MIP) have garnered significant interest as drug delivery system (DDS) in recent years. The conventional thermal heating and one-variable-at-a-time method for synthesising MIP and rebinding capacity evaluation is resource- and time-consuming. Thus, this study focused on the response surface methodology (RSM) optimisation of the polymer synthesis using microwave (MW)-assisted and comparing with conventional thermal synthesis. The influence of two factors (methacrylic acid and divinylbenzene concentration) was studied on the response of the MIP rebinding capacity. Further optimisation on rebinding capacity were employed three factors including MIP dosage, initial drug concentration and contact time using Central Composite Design (CCD). In vitro drug release profiles were evaluated in pH 7.4 and pH 2.2 of dissolution media. The aspirin MIP showed spherical particles with smaller particle sizes (500 nm– 1.45 μm) and yields (0.5–1 g) via MW-assisted synthesis (sample id: ASDW) as compared to the conventional synthesis (sample id: ASD) (size 660 nm –3.65 μm, yield 0.5–1.15 g). The MW-MIP of paracetamol (sample id: PCMW) also showed similar findings with ASDW (size 1.07 – 1.64 μm, yield 0.5 - 0.9 g). The optimised formulation of MIP showed polymer P1 with T:FM:CL of 1:4:16 have shown high rebinding capacity in both polymerisation methods of conventional thermal heating (ASD-P1, 3.00±0.31mg/g)and MW-assisted synthesis (ASDW-P1, 7.05±0.08 mg/g; PCMW, 6.17±0.03 mg/g). The optimal rebinding conditions for ASD-P1, ASDW-P1 and PCMW-P1 to achieve high rebinding capacity are as follows: 240 min contact time, 300 mg/L initial concentration and 20 mg MIP dosage. Method validations were performed under optimised conditions and showed only 2-3% error compared with the predicted rebinding capacity. The drug release profile for ASD-P1, ASDW-P1 and PCMW-P1, has shown a sustained drug release with the highest cumulative release observed at pH 7.4 (64 – 78% for 24 h) than at pH 2.2 (44 – 76%, for 24 h). The release of aspirin and paracetamol at pH 2.2 was fitted in first-order kinetics, followed by the Higuchi model. Meanwhile, all MIP (ASD-P1, ASDW-P1 and PCMW-P1) at pH 7.4 were well-fitted with the Higuchi model. These results collectively demonstrated that the MIP performances are impacted by the choice of the MIP composition (i.e., functional monomer and crosslinker) and the polymerisation method (i.e., MW-assisted synthesis, conventional thermal heating). The optimised formulation ratio of MIP at ratio 1:4:16 can significantly enhance the efficacy, precision, and safety of drug delivery systems, making MIP a valuable component in modern pharmaceuticals. Furthermore, the optimised MIP can potentially reduce cost associated with drug formulation.
format	Thesis
qualification_name	Doctor of Philosophy (PhD.)
qualification_level	Doctorate
author	Vannessa, Lawai
author_facet	Vannessa, Lawai
author_sort	Vannessa, Lawai
title	Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study
title_short	Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study
title_full	Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study
title_fullStr	Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study
title_full_unstemmed	Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study
title_sort	microwave-assisted synthesis of molecularly imprinted polymer for sustained drug release: a chemometric approach on polymer synthesis and rebinding study
granting_institution	Universiti Malaysia Sarawak
granting_department	Faculty of Resource Science and Technology
publishDate	2024
url	http://ir.unimas.my/id/eprint/45978/3/Thesis_PhD_Vannessa.pdf
_version_	1811771583989022720
spelling	my-unimas-ir.459782024-09-10T01:32:23Z Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study 2024-09-06 Vannessa, Lawai QD Chemistry Molecularly imprinted polymers (MIP) have garnered significant interest as drug delivery system (DDS) in recent years. The conventional thermal heating and one-variable-at-a-time method for synthesising MIP and rebinding capacity evaluation is resource- and time-consuming. Thus, this study focused on the response surface methodology (RSM) optimisation of the polymer synthesis using microwave (MW)-assisted and comparing with conventional thermal synthesis. The influence of two factors (methacrylic acid and divinylbenzene concentration) was studied on the response of the MIP rebinding capacity. Further optimisation on rebinding capacity were employed three factors including MIP dosage, initial drug concentration and contact time using Central Composite Design (CCD). In vitro drug release profiles were evaluated in pH 7.4 and pH 2.2 of dissolution media. The aspirin MIP showed spherical particles with smaller particle sizes (500 nm– 1.45 μm) and yields (0.5–1 g) via MW-assisted synthesis (sample id: ASDW) as compared to the conventional synthesis (sample id: ASD) (size 660 nm –3.65 μm, yield 0.5–1.15 g). The MW-MIP of paracetamol (sample id: PCMW) also showed similar findings with ASDW (size 1.07 – 1.64 μm, yield 0.5 - 0.9 g). The optimised formulation of MIP showed polymer P1 with T:FM:CL of 1:4:16 have shown high rebinding capacity in both polymerisation methods of conventional thermal heating (ASD-P1, 3.00±0.31mg/g)and MW-assisted synthesis (ASDW-P1, 7.05±0.08 mg/g; PCMW, 6.17±0.03 mg/g). The optimal rebinding conditions for ASD-P1, ASDW-P1 and PCMW-P1 to achieve high rebinding capacity are as follows: 240 min contact time, 300 mg/L initial concentration and 20 mg MIP dosage. Method validations were performed under optimised conditions and showed only 2-3% error compared with the predicted rebinding capacity. The drug release profile for ASD-P1, ASDW-P1 and PCMW-P1, has shown a sustained drug release with the highest cumulative release observed at pH 7.4 (64 – 78% for 24 h) than at pH 2.2 (44 – 76%, for 24 h). The release of aspirin and paracetamol at pH 2.2 was fitted in first-order kinetics, followed by the Higuchi model. Meanwhile, all MIP (ASD-P1, ASDW-P1 and PCMW-P1) at pH 7.4 were well-fitted with the Higuchi model. These results collectively demonstrated that the MIP performances are impacted by the choice of the MIP composition (i.e., functional monomer and crosslinker) and the polymerisation method (i.e., MW-assisted synthesis, conventional thermal heating). The optimised formulation ratio of MIP at ratio 1:4:16 can significantly enhance the efficacy, precision, and safety of drug delivery systems, making MIP a valuable component in modern pharmaceuticals. Furthermore, the optimised MIP can potentially reduce cost associated with drug formulation. Vannessa Lawai 2024-09 Thesis http://ir.unimas.my/id/eprint/45978/ http://ir.unimas.my/id/eprint/45978/3/Thesis_PhD_Vannessa.pdf text en public phd doctoral Universiti Malaysia Sarawak Faculty of Resource Science and Technology Abbasi, S., Haeri, S. A., & Sajjadifar, S. (2019). Bio-dispersive liquid liquid microextraction based on nano rhamnolipid aggregates combined with molecularly imprinted-solid phase extraction for selective determination of paracetamol in human urine samples followed by HPLC. Microchemical Journal, 146, 106–114. https://doi.org/10.1016/j.microc.2018.12.065 Abd, F. N., Al-Bayati, Y. K., & Joda, B. A. (2019). Synthesis of molecularly imprinted polymers for estimation of aspirin by using different functional monomers. International Journal of Drug Delivery Technology, 9(04), 660–665. https://doi.org/10.25258/ijddt.9.4.24 Abdollahi, E., Khalafi-Nezhad, A., Mohammadi, A., Abdouss, M., & Salami-Kalajahi, M. (2018). Synthesis of new molecularly imprinted polymer via reversible addition fragmentation transfer polymerisation as a drug delivery system. Polymer, 143, 245–257. https://doi.org/10.1016/j.polymer.2018.03.058 Adepu, S., & Ramakrishna, S. (2021). Controlled drug delivery systems: Current status and future directions. Molecules, 26(19). https://doi.org/10.3390/molecules26195905 Aghoutane, Y., Diouf, A., Österlund, L., Bouchikhi, B., & El Bari, N. (2020). Development of a molecularly imprinted polymer electrochemical sensor and its application for sensitive detection and determination of malathion in olive fruits and oils. Bioelectrochemistry, 132, 107404. https://doi.org/10.1016/j.bioelechem.2019.107404 Agrawal, P. (2015). Significance of Polymers in Drug Delivery System. Journal of Pharmacovigilance, 03(01), 1–2. https://doi.org/10.4172/2329-6887.1000e127 Alanazi, K., Garcia Cruz, A., Di Masi, S., Voorhaar, A., Ahmad, O. S., Cowen, T., Piletska, E., Langford, N., Coats, T., Sims, M. R., & Piletsky, S. A. (2021). Disposable paracetamol sensor based on electroactive molecularly imprinted polymer nanoparticles for plasma monitoring. Sensors and Actuators, B: Chemical, 329, 129128. https://doi.org/10.1016/j.snb.2020.129128 Ali, F., Shah, Z., Khan, A., Saadia, M., Alothman, Z. A., & Cheong, W. J. (2022a). Synthesis, column packing and liquid chromatography of molecularly imprinted polymers for the acid black 1, acid black 210 and acid brown 703 dyes. RSC Advances, 12, 19611–19623. https://doi.org/10.1039/d2ra02357a

Microwave-assisted Synthesis of Molecularly Imprinted Polymer for Sustained Drug Release: A Chemometric Approach on Polymer Synthesis and Rebinding Study

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