Synthesis and Characterization of Polymer Electrolyte Membrane Based on Cellulose-Chitosan-Alginate as Li-Ion Battery Separator

Rahmadini Syafri (1), - Emriadi (2), - Zulhadjri (3), Mai Efdi (4), Delovita Ginting (5), - Chairil (6), Edy Saputra (7), Rika Taslim (8), Rusli Daik (9)
(1) Department of Chemistry, Universitas Muhammadiyah Riau, Pekanbaru, 28294, Indonesia
(2) Department of Chemistry, Faculty of Mathematics and Natural Science, Universitas Andalas, Padang, 25163, Indonesia
(3) Department of Chemistry, Faculty of Mathematics and Natural Science, Universitas Andalas, Padang, 25163, Indonesia
(4) Department of Chemistry, Faculty of Mathematics and Natural Science, Universitas Andalas, Padang, 25163, Indonesia
(5) Department of Physics, Universitas Muhammadiyah Riau, Pekanbaru, 28294, Indonesia
(6) Department of Nursing, Universitas Muhammadiyah Riau, Pekanbaru, 28294, Indonesia
(7) Department of Chemical Engineering, Riau University, Pekanbaru 28293, Indonesia
(8) Department of Industrial Engineering, State Islamic University of Sultan Syarif Kasim, Simpang Baru, Riau, 28293, Indonesia
(9) Department of Chemical Science, Faculty of Science and Technology, Universiti Kebangsaan Malaysia, 43600 Bangi, Selangor, Malaysia
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How to cite (IJASEIT) :
Syafri, Rahmadini, et al. “Synthesis and Characterization of Polymer Electrolyte Membrane Based on Cellulose-Chitosan-Alginate As Li-Ion Battery Separator”. International Journal on Advanced Science, Engineering and Information Technology, vol. 13, no. 2, Mar. 2023, pp. 585-91, doi:10.18517/ijaseit.13.2.16704.
The current commercial Gel Polymer Electrolyte (GPE) products are generally made of synthetic and non-biodegradable materials. In addition, some of these polymers require toxic reagents and complex synthesis processes. The purpose of this research is to manufacture GPE membrane products using biodegradable raw materials, a combination of Hydroxy Ethyl Cellulose (HEC), Carboxymethyl Chitosan (CMCs), and Sodium Alginate (SA) with lithium salt as the electrolyte source. The methods start from the fabrication/synthesis of biodegradable GPE membranes in various compositions, then LiOH is added as an electrolyte source and glutaraldehyde as a crosslinking agent using a solution casting technique. The mechanical membrane testing (tensile strength and elongation) and characterization were carried out using XRD, SEM, and FTIR. Based on mechanical tests carried out, variations in HEC 50%: SA 50% has the highest tensile strength value of 81.4255 MPa and the lowest elongation value of 11.68%. The results of XRD analysis in the presence of a typical peak in the HEC: SA variation was 11.56º, which could affect the strength of the electrolyte-polymer gel membrane (GPE). The results of SEM analysis proved that the HEC: SA variation has a porous morphology that can affect the ion absorption capacity in lithium-ion battery applications. The results of FTIR analysis proved that there are functional groups S=O, CH, CO, NH, OH, and COC in the three membranes (SA, CMCs, and HEC).

J. Yang, J. Yao, and S. Guan, “Enhanced electroresponsive and electrochemical properties of the biological gel artificial muscle prepared by sdium alginate and carboxylated chitosan,” Sensors Actuators, B Chem., vol. 322, no. March, p. 128526, 2020, doi: 10.1016/j.snb.2020.128526.

Y. G. Cho, C. Hwang, D. S. Cheong, Y. S. Kim, and H. K. Song, “Gel/Solid Polymer Electrolytes Characterized by In Situ Gelation or Polymerization for Electrochemical Energy Systems,” Adv. Mater., vol. 31, no. 20, pp. 1-12, 2019, doi: 10.1002/adma.201804909.

X. Zhang, S. Zhao, W. Fan, J. Wang, and C. Li, “Long cycling, thermal stable, dendrites free gel polymer electrolyte for flexible lithium metal batteries,” Electrochim. Acta, vol. 301, pp. 304-311, 2019, doi: 10.1016/j.electacta.2019.01.156.

N. Kassenova, S. Kalybekkyzy, M. V. Kahraman, A. Mentbayeva, and Z. Bakenov, “Photo and thermal crosslinked poly(vinyl alcohol)-based nanofiber membrane for flexible gel polymer electrolyte,” J. Power Sources, vol. 520, p. 230896, 2022, doi: 10.1016/j.jpowsour.2021.230896.

Q. Song et al., “Thermally stable, nano-porous and eco-friendly sodium alginate/attapulgite separator for lithium-ion batteries,” Energy Storage Mater., vol. 22, no. June, pp. 48-56, 2019, doi: 10.1016/j.ensm.2019.06.033.

X. Wang, J. He, L. Ma, B. Yan, L. Shi, and R. Ran, “Self-assembling graphene oxide/modified amphipathic hydroxyethyl cellulose hybrid stabilized Pickering emulsion polymerization for functional hydrogel,” Colloids Surfaces A Physicochem. Eng. Asp., vol. 610, no. October, p. 125742, 2021, doi: 10.1016/j.colsurfa.2020.125742.

S. S. Azahar, T. S. Hamidon, A. F. A. Latip, and M. H. Hussin, “Physicochemical and conductivity studies of chitosan-tapioca flour-LiBF4 gel polymer electrolytes,” Chem. Phys. Impact, vol. 3, no. November, p. 100055, 2021, doi: 10.1016/j.chphi.2021.100055.

D. Zhou, D. Shanmukaraj, A. Tkacheva, M. Armand, and G. Wang, “Polymer Electrolytes for Lithium-Based Batteries: Advances and Prospects,” Chem, vol. 5, no. 9, pp. 2326-2352, 2019, doi: 10.1016/j.chempr.2019.05.009.

X. Deng et al., “Gel polymer electrolyte with high performances based on biodegradable polymer polyvinyl alcohol composite lignocellulose,” Mater. Chem. Phys., vol. 229, pp. 232-241, 2019, doi: 10.1016/j.matchemphys.2019.03.014.

S. Liang et al., “Gel polymer electrolytes for lithium ion batteries: Fabrication, characterization and performance,” Solid State Ionics, vol. 318, no. August, pp. 2-18, 2018, doi: 10.1016/j.ssi.2017.12.023.

J. Zhang et al., “Composite electrolyte membranes incorporating viscous copolymers with cellulose for high performance lithium-ion batteries,” J. Memb. Sci., vol. 497, pp. 259-269, 2016, doi: 10.1016/j.memsci.2015.09.056.

J. Gou, W. Liu, A. Tang, and H. Xie, “A phosphorylated nanocellulose/hydroxypropyl methylcellulose composite matrix: A biodegradable, flame-retardant and self-standing gel polymer electrolyte towards eco-friendly and high safety lithium ion batteries,” Eur. Polym. J., vol. 158, no. June, p. 110703, 2021, doi: 10.1016/j.eurpolymj.2021.110703.

M. Y. Zhang et al., “A Sandwich PVDF/HEC/PVDF Gel Polymer Electrolyte for Lithium Ion Battery,” Electrochim. Acta, vol. 245, pp. 752-759, 2017, doi: 10.1016/j.electacta.2017.05.154.

L. Leng et al., “A novel stability-enhanced lithium-oxygen battery with cellulose-based composite polymer gel as the electrolyte,” Electrochim. Acta, vol. 176, pp. 1108-1115, 2015, doi: 10.1016/j.electacta.2015.07.111.

P. Lin et al., “Preparation and properties of carboxymethyl chitosan/oxidized hydroxyethyl cellulose hydrogel,” Int. J. Biol. Macromol., vol. 162, pp. 1692-1698, 2020, doi: 10.1016/j.ijbiomac.2020.07.282.

K. Soeda, M. Yamagata, and M. Ishikawa, “Outstanding features of alginate-based gel electrolyte with ionic liquid for electric double layer capacitors,” J. Power Sources, vol. 280, pp. 565-572, 2015, doi: 10.1016/j.jpowsour.2015.01.144.

Z. Du et al., “A mechanically robust, biodegradable and high performance cellulose gel membrane as gel polymer electrolyte of lithium-ion battery,” Electrochim. Acta, vol. 299, pp. 19-26, 2019, doi: 10.1016/j.electacta.2018.12.173.

J. Gou, W. Liu, and A. Tang, “A renewable gel polymer electrolyte based on the different sized carboxylated cellulose with satisfactory comprehensive performance for rechargeable lithium ion battery,” Polymer (Guildf)., vol. 208, no. August, p. 122943, 2020, doi: 10.1016/j.polymer.2020.122943.

O. Hu et al., “A facile preparation method for anti-freezing, tough, transparent, conductive and thermoplastic poly(vinyl alcohol)/sodium alginate/glycerol organohydrogel electrolyte,” Int. J. Biol. Macromol., vol. 164, pp. 2512-2523, 2020, doi: 10.1016/j.ijbiomac.2020.08.115.

K. Luo et al., “PVDF-HFP-modified gel polymer electrolyte for the stable cycling lithium metal batteries,” J. Electroanal. Chem., vol. 895, no. June, p. 115462, 2021, doi: 10.1016/j.jelechem.2021.115462.

W. Bao, Z. Zhang, Y. Gan, X. Wang, and J. Lia, “Enhanced cyclability of sulfur cathodes in lithium-sulfur batteries with Na-alginate as a binder,” J. Energy Chem., vol. 22, no. 5, pp. 790-794, 2013, doi: 10.1016/S2095-4956(13)60105-9.

S. Wichai, P. Chuysinuan, S. Chaiarwut, P. Ekabutr, and P. Supaphol, “Development of bacterial cellulose/alginate/chitosan composites incorporating copper (II) sulfate as an antibacterial wound dressing,” J. Drug Deliv. Sci. Technol., vol. 51, no. Ii, pp. 662-671, 2019, doi: 10.1016/j.jddst.2019.03.043.

M. Karzar Jeddi and M. Mahkam, “Magnetic nano carboxymethyl cellulose-alginate/chitosan hydrogel beads as biodegradable devices for controlled drug delivery,” Int. J. Biol. Macromol., vol. 135, pp. 829-838, 2019, doi: 10.1016/j.ijbiomac.2019.05.210.

K. Nowacki, M. GaliÅ„ski, and I. StÄ™pniak, “Synthesis and characterization of modified chitosan membranes for applications in electrochemical capacitor,” Electrochim. Acta, vol. 320, 2019, doi: 10.1016/j.electacta.2019.134632.

H. Kang, Y. Rho, S. Bhade, S. Hegde, A. Ferrese, and J. Newman, “Recent Development of Polyvinylidene Fluoride / Cellulose Membranes Electrolyte Separator for Lithium Ion Batteries Recent Development of Polyvinylidene Fluoride / Cellulose Membranes Electrolyte Separator for Lithium Ion Batteries,” 2021, doi: 10.1088/1757-899X/1096/1/012144.

Z. Li, Q. Ding, and W. Han, “PVA-based high carboxyl group substituted modified cellulose nanofiber composite hydrogel for flexible new air battery PVA-based high carboxyl group substituted modified cellulose nanofiber composite hydrogel for flexible new air battery,” 2021, doi: 10.1088/1755-1315/639/1/012044.

R. Chitra, P. Sathya, S. Selvasekarapandian, and S. Meyvel, “Investigation of seaweed derivative iota- carrageenan based biopolymer electrolytes with lithium trifluoromethanesulfonate Investigation of seaweed derivative iota-carrageenan based biopolymer electrolytes with lithium tri fl uoromethanesulfonate.” Mater. Res. Express, vol. 7 no.1 2020, doi: 10.1088/2053-1591/ab5d79

S. Abdullah et al., “Characterization of Solid Polymer Electrolyte Membrane made of Methylcellulose and Ammonium Nitrate,” J. Phys. Conf. Ser., vol. 1532, no. 1, pp. 6-11, 2020, doi: 10.1088/1742-6596/1532/1/012017.

M. R. Asghar, M. T. Anwar, T. Rasheed, A. Naveed, X. Yan, and J. Zhang, “Lithium Salt Doped Poly(Vinylidene Fluoride)/Cellulose Acetate Composite Gel Electrolyte Membrane for Lithium Ion Battery,” IOP Conf. Ser. Mater. Sci. Eng., vol. 654, no. 1, 2019, doi: 10.1088/1757-899X/654/1/012017.

N. F. Mazuki, A. P. P. Abdul Majeed, Y. Nagao, and A. S. Samsudin, “Studies on ionics conduction properties of modification CMC-PVA based polymer blend electrolytes via impedance approach,” Polym. Test., vol. 81, no. November 2019, p. 106234, 2020, doi: 10.1016/j.polymertesting.2019.106234.

M. A. Saadiah, D. Zhang, Y. Nagao, S. K. Muzakir, and A. S. Samsudin, “Reducing crystallinity on thin film based CMC/PVA hybrid polymer for application as a host in polymer electrolytes,” J. Non. Cryst. Solids, vol. 511, no. November 2018, pp. 201-211, 2019, doi: 10.1016/j.jnoncrysol.2018.11.032.

S. B. Aziz et al., “Impedance, circuit simulation, transport properties and energy storage behavior of plasticized lithium ion conducting chitosan based polymer electrolytes,” Polym. Test., vol. 101, no. June, p. 107286, 2021, doi: 10.1016/j.polymertesting.2021.107286.

P. Perumal, P. Christopher Selvin, S. Selvasekarapandian, and P. Sivaraj, “Structural and electrical properties of bio-polymer pectin with LiClO4 solid electrolytes for lithium ion polymer batteries,” Mater. Today Proc., vol. 8, pp. 196-202, 2019, doi: 10.1016/j.matpr.2019.02.100.

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