Sustainable Lithium‐Ion Battery Separator Membranes Based on Carrageenan Biopolymer

Abstract

Aiming to improve the sustainability of materials for lithium‐ion batteries (LIBs), this work reports on the development of novel membranes based on iota‐carrageenan biopolymer and their suitability as separator in LIBs applications. The membranes are prepared by freeze‐drying and its morphology, thermal, mechanical, and electrochemical properties are evaluated as a function of polymer concentration in the solution. Porous membranes with a degree of porosity above 90% and different interconnected pore sizes between 50 and 70 µm for both polymer concentrations are obtained. The electrochemical parameters of the membranes are influenced by the carrageenan polymer concentration, being 1.34 mS cm‐1, 3, 7, and 0.48 for ionic conductivity, tortuosity, MacMullin number, and lithium transference number, respectively, for the membrane prepared from the 4 wt% carrageenan content solution. The half‐cells cathodic prepared with the developed membranes show good cyclability and rate capability. The discharge capacity values obtained with the membrane prepared from 4 wt% carrageenan content are 145 and 25 mAh g‐1 at C/10‐ and 1C‐rates, respectively, demonstrating excellent battery cycling performance and long‐term stability. Thus, this work demonstrates that iota‐carrageenan biopolymer membranes developed by freeze‐drying can be used as separators for a next generation of more sustainable batteries.

Progress of Carrageenan‐Based Films and Coatings for Food Packaging Applications

“…For example, as the mean molecular weight increases from 10 000 to 250 000, the strength of the gel gradually increases. However, the rate of increase in gel strength decreases when the mean molecular weight exceeds 250 000 [46]. This is because the molecular weight of carrageenan is positively correlated with the length of the double helix chain.…”

Overview on Theoretical Simulations of Lithium‐Ion Batteries and Their Application to Battery Separators

“…Additionally, to improve the thermal and mechanical properties and wettability of the conventional separators based on PE and PP, new separators based on covalent organic framework (COF) into poly(arylene ether benzimidazole) (OPBI), [93] polyacrylonitrile (PAN) composite separators with cellulose acetate and nano-hydroxyapatite, [94] PAN with aluminum diethylphosphinate (ADEP), [95] polyimide (PI) polymer, [96] PI with polyethylene oxide (PEO) processed by electrospinning technique, [97] PI with zirconia (ZrO 2 ), [98] PI with graphene, [99] PI with hexagonal boron nitride, [100] PI with nano-tiO 2 , [101] PI with organic montmorillonite (OMMT), [102] PEO with para-aramid nanofibers (ANFs), [103] PVDF/SiO 2 , [104] poly(ethylene glycol) diacrylate (PEGDA), [105] polyurethane separator coated Al 2 O 3 particles, [89a] and poly(vinyl alcohol) with nano architecture halloysite nanotubes (NHNTs) composite separator (OPVA/NHNTs separator, [106] and new coatings of boehmite (γ-AlO(OH)) nanofibers, [107] inorganic oxide solid electrolyte layers (Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 , LATP), [108] SiO 2 with acrylamide (AM), [81a] Ca 3 (PO 4 ) 2 inorganic layer, [91] polyimide microsphere, [109] and plasma treatment plus zwitterion grafting [110] were developed. Further, it has been also explored the replacement of these synthetic polymers by natural polymers such as, natural wood, [111] cellulose, [96,112] silk fibroin, [113] silk fibroin with sericin, [114] poly(vinyl alcohol) (PVA), [115] lignin, [116] carrageenan, [117] among others.…”

Tailoring the Function of Battery Separators via the Design of MOF Coatings

“…Traditional separators are mainly composed of porous DOI: 10.1002/adfm.202314246 polyolefin films like polpropylene (PP) and polyethylene (PE), which suffer from poor electrolyte wettability and flammability, potentially leading to safety risks. [2] In recent years, various approaches have been explored to tackle these critical challenges, including the development of new polymers, [3][4][5] surface coating, [6][7][8] and filling modification. [9][10][11] Among these strategies, surface coating has garnered extensive attention due to its straightforward processes and the potential for industrial scalability.…”