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Review Challenges in Solvent-Free Methods for Manufacturing Electrodes and Electrolytes for Lithium-Based Batteries Nina Verdier 1, Gabrielle Foran 1, David Lepage 1, Arnaud Prébé 1, David Aymé-Perrot 2 and Mickaël Dollé 1,* Citation: Verdier, N.; Foran, G.; Lepage, D.; Prébé, A.; Aymé-Perrot, D.; Dollé, M. Challenges in Solvent- Free Methods for Manufacturing Electrodes and Electrolytes for Lithium-Based Batteries. Polymers 2021, 13, 323. https://doi.org/10.3390/ polym13030323 Received: 10 December 2020 Accepted: 15 January 2021 Published: 20 January 2021 Publisher’s Note: MDPI stays neu- tral with regard to jurisdictional claims in published maps and insti- tutional affiliations. Copyright: © 2021 by the authors. Li- censee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and con- ditions of the Creative Commons At- tribution (CC BY) license (http://crea- tivecommons.org/licenses/by/4.0/). 1 Département de Chimie, Université de Montréal, CP6128 Succursale Centre-Ville, Montréal, QC H3T 1J4, Canada; nina.verdier@umontreal.ca (N.V.); gabrielle.foran@umontreal.ca (G.F.); david.lepage.3@umontreal.ca (D.L.); arnaud.prebe@umontreal.ca (A.P.) 2 Total SA, 2 Pl. Millier, 92069 Paris La Défense, France; david.aymeperrot@total.com * Correspondence: mickael.dolle@umontreal.ca; Tel.: 1-514-343-7054 Abstract: With the ever-growing energy storage notably due to the electric vehicle market expansion and stationary applications, one of the challenges of lithium batteries lies in the cost and environ- mental impacts of their manufacture. The main process employed is the solvent-casting method, based on a slurry casted onto a current collector. The disadvantages of this technique include the use of toxic and costly solvents as well as significant quantity of energy required for solvent evapo- ration and recycling. A solvent-free manufacturing method would represent significant progress in the development of cost-effective and environmentally friendly lithium-ion and lithium metal bat- teries. This review provides an overview of solvent-free processes used to make solid polymer elec- trolytes and composite electrodes. Two methods can be described: heat-based (hot-pressing, melt processing, dissolution into melted polymer, the incorporation of melted polymer into particles) and spray-based (electrospray deposition or high-pressure deposition). Heat-based processes are used for solid electrolyte and electrode manufacturing, while spray-based processes are only used for electrode processing. Amongst these techniques, hot-pressing and melt processing were re- vealed to be the most used alternatives for both polymer-based electrolytes and electrodes. These two techniques are versatile and can be used in the processing of fillers with a wide range of mor- phologies and loadings. Keywords: solvent-free processes; solid polymer electrolyte; electrodes; polymer binder; melt-pro- cessing; hot-pressing; Li-ion batteries; Li metal batteries 1. Introduction Li-ion batteries are a well-established and mature technology that has spread to al- most, if not all, of our portable devices. Li-ion batteries are composed of a positive and a negative electrode as well as an electrolyte to ensure the transfer of lithium ions through the cell. If the electrolyte is liquid, a membrane called separator is used to avoid contact between the two electrodes. Electrodes are then connected thanks to an external circuit allowing electrons to go from one electrode to the other. Li-ion batteries are based on the insertion/deintercalation of lithium ions inside the electrode, more specifically into inor- ganic materials commonly called active materials due to their role inside electrodes. Such batteries have conquered the battery market as they present several advantages compared to other battery types like alkaline or lead-acid batteries. Li-ion batteries have higher spe- cific power and specific energy and show an increased cycle life [1]. For these reasons, this technology is one of the most promising for use in the developing electric vehicle (EV) market. Mostly due to the high demand in the automotive industry for EVs, the fabrica- tion of Li-ion batteries has drastically increased and is predicted to rise even more in com- ing years. The creation of batteries requires the formulation and manufacturing of an elec- Polymers 2021, 13, 323. https://doi.org/10.3390/polym13030323 www.mdpi.com/journal/polymersPDF Image | Electrodes and Electrolytes for Lithium-Based Batteries
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