Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation
This work deals with the search of polymers apt for the preparation of solid-like chloroaluminate-based electrolytes. To accomplish this, the solubility and gelling ability of a large set of polymers in the deep eutectic solvent AlCl3:urea (uralumina) are studied, followed by the characterization of...
| Autores: | , , , , , , , , , , |
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| Formato: | artículo |
| Estado: | Versión publicada |
| Fecha de publicación: | 2021 |
| País: | España |
| Recursos: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositorio: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/237786 |
| Acesso em linha: | http://hdl.handle.net/10261/237786 |
| Access Level: | acceso abierto |
| Palavra-chave: | Polymer gel electrolyte Chloroaluminate ionogel Aluminium secondary battery |
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Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciationMiguel, ÁlvaroJankowski, PiotrPablos, Jesús L.Corrales, TeresaLópez-Cudero, AnaBhowmik, ArghyaCarrasco-Busturia, DavidEllis, Gary JamesGarcía, NuriaGarcía-Lastra, J. M.Tiemblo, PilarPolymer gel electrolyteChloroaluminate ionogelAluminium secondary batteryThis work deals with the search of polymers apt for the preparation of solid-like chloroaluminate-based electrolytes. To accomplish this, the solubility and gelling ability of a large set of polymers in the deep eutectic solvent AlCl3:urea (uralumina) are studied, followed by the characterization of the electrochemical activity of the gels. The polymers are directly dissolved in urea:AlCl3 without auxiliary solvents following a fast and scalable gel preparation methodology previously reported for ultra-high molecular weight (UHMW) polyethylene oxide (PEO). The list of polymers studied includes diverse chemical structures, different thermal properties and different aggregation states at the mixing temperature of 70 ◦C, defined by the thermal stability of AlCl3:urea. To avoid a molecular weight influence on the ionogel rheological properties, polymers with molecular weight close to 100,000 g mol 1 have been chosen. The polymers considered include poly(ε-caprolactone) (PCL), poly (dimethyl siloxane) (PDMS), poly(vinyl pyrrolidone) (PVP), polyformal, thermoplastic polyurethanes, polymethacrylates, polyacetates and the elastomer SEBS. It was found that together with polyethylene oxide, only poly(ε-caprolactone) and poly(dimethyl siloxane) are soluble and produce gel electrolytes with AlCl3:urea. The solubility rules of polymers in chloroaluminates are discussed. The stripping/plating of Al and the ionic conductivity of PEO, PDMS and PCL ionogels are studied by cyclic voltammetry and impedance spectroscopy. PDMS proves to be as efficient as PEO to produce ionogels at low polymer concentration, that are also self-standing and electroactive, whereas a higher concentration of PCL is required to produce self-standing gels. The molecular structure of the ionogels and the modification of the chloroaluminate speciation is studied by vibrational spectroscopies, and supported by DFT calculations.The authors acknowledge financial support from project European Union H2020-FETOPEN-1-2016-2017 call (G A. No. 766581, SALBAGE project). All calculations were carried out at the Wrocław Center for Networking and Supercomputing, Grant 346.Peer reviewedElsevierEuropean CommissionWroclaw Centre for Networking and SupercomputingMiguel, Álvaro [0000-0003-3981-5699]Pablos, Jesús L. [0000-0001-8504-8836]Corrales,Teresa [0000-0002-0171-2283]López-Cudero, Ana [0000-0001-8330-3805]Gary Ellis [0000-0003-4851-6092]Nuria García [0000-0002-4330-3883]Tiemblo, Pilar [0000-0002-3917-0504]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202120212021info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/237786reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/H2020/766581Miguel, Alvaro; Jankowski, Piotr; Pablos, Jesús L.; Corrales, Teresa ; López-Cudero, Ana; Bhowmik, Arghya; Carrasco-Busturia, David; Ellis, Gary James ; García, Nuria ; García-Lastra, J. M.; Tiemblo, Pilar; 2021; Polymer gel electrolytes for secondary aluminium batteries, prepared with the deep eutectic solvent uralumina (urea:AlCl3) and poly(ethylene oxide) of different molecular weight and at different concentrations; DIGITAL.CSIC; http://dx.doi.org/10.20350/digitalCSIC/13856https://doi.org/10.1016/j.polymer.2021.123707Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2377862026-05-22T06:33:51Z |
| dc.title.none.fl_str_mv |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation |
| title |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation |
| spellingShingle |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation Miguel, Álvaro Polymer gel electrolyte Chloroaluminate ionogel Aluminium secondary battery |
| title_short |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation |
| title_full |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation |
| title_fullStr |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation |
| title_full_unstemmed |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation |
| title_sort |
Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation |
| dc.creator.none.fl_str_mv |
Miguel, Álvaro Jankowski, Piotr Pablos, Jesús L. Corrales, Teresa López-Cudero, Ana Bhowmik, Arghya Carrasco-Busturia, David Ellis, Gary James García, Nuria García-Lastra, J. M. Tiemblo, Pilar |
| author |
Miguel, Álvaro |
| author_facet |
Miguel, Álvaro Jankowski, Piotr Pablos, Jesús L. Corrales, Teresa López-Cudero, Ana Bhowmik, Arghya Carrasco-Busturia, David Ellis, Gary James García, Nuria García-Lastra, J. M. Tiemblo, Pilar |
| author_role |
author |
| author2 |
Jankowski, Piotr Pablos, Jesús L. Corrales, Teresa López-Cudero, Ana Bhowmik, Arghya Carrasco-Busturia, David Ellis, Gary James García, Nuria García-Lastra, J. M. Tiemblo, Pilar |
| author2_role |
author author author author author author author author author author |
| dc.contributor.none.fl_str_mv |
European Commission Wroclaw Centre for Networking and Supercomputing Miguel, Álvaro [0000-0003-3981-5699] Pablos, Jesús L. [0000-0001-8504-8836] Corrales,Teresa [0000-0002-0171-2283] López-Cudero, Ana [0000-0001-8330-3805] Gary Ellis [0000-0003-4851-6092] Nuria García [0000-0002-4330-3883] Tiemblo, Pilar [0000-0002-3917-0504] Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72] |
| dc.subject.none.fl_str_mv |
Polymer gel electrolyte Chloroaluminate ionogel Aluminium secondary battery |
| topic |
Polymer gel electrolyte Chloroaluminate ionogel Aluminium secondary battery |
| description |
This work deals with the search of polymers apt for the preparation of solid-like chloroaluminate-based electrolytes. To accomplish this, the solubility and gelling ability of a large set of polymers in the deep eutectic solvent AlCl3:urea (uralumina) are studied, followed by the characterization of the electrochemical activity of the gels. The polymers are directly dissolved in urea:AlCl3 without auxiliary solvents following a fast and scalable gel preparation methodology previously reported for ultra-high molecular weight (UHMW) polyethylene oxide (PEO). The list of polymers studied includes diverse chemical structures, different thermal properties and different aggregation states at the mixing temperature of 70 ◦C, defined by the thermal stability of AlCl3:urea. To avoid a molecular weight influence on the ionogel rheological properties, polymers with molecular weight close to 100,000 g mol 1 have been chosen. The polymers considered include poly(ε-caprolactone) (PCL), poly (dimethyl siloxane) (PDMS), poly(vinyl pyrrolidone) (PVP), polyformal, thermoplastic polyurethanes, polymethacrylates, polyacetates and the elastomer SEBS. It was found that together with polyethylene oxide, only poly(ε-caprolactone) and poly(dimethyl siloxane) are soluble and produce gel electrolytes with AlCl3:urea. The solubility rules of polymers in chloroaluminates are discussed. The stripping/plating of Al and the ionic conductivity of PEO, PDMS and PCL ionogels are studied by cyclic voltammetry and impedance spectroscopy. PDMS proves to be as efficient as PEO to produce ionogels at low polymer concentration, that are also self-standing and electroactive, whereas a higher concentration of PCL is required to produce self-standing gels. The molecular structure of the ionogels and the modification of the chloroaluminate speciation is studied by vibrational spectroscopies, and supported by DFT calculations. |
| publishDate |
2021 |
| dc.date.none.fl_str_mv |
2021 2021 2021 |
| dc.type.none.fl_str_mv |
info:eu-repo/semantics/article http://purl.org/coar/resource_type/c_6501 Publisher's version info:eu-repo/semantics/publishedVersion |
| format |
article |
| status_str |
publishedVersion |
| dc.identifier.none.fl_str_mv |
http://hdl.handle.net/10261/237786 |
| url |
http://hdl.handle.net/10261/237786 |
| dc.language.none.fl_str_mv |
Inglés |
| language_invalid_str_mv |
Inglés |
| dc.relation.none.fl_str_mv |
#PLACEHOLDER_PARENT_METADATA_VALUE# info:eu-repo/grantAgreement/EC/H2020/766581 Miguel, Alvaro; Jankowski, Piotr; Pablos, Jesús L.; Corrales, Teresa ; López-Cudero, Ana; Bhowmik, Arghya; Carrasco-Busturia, David; Ellis, Gary James ; García, Nuria ; García-Lastra, J. M.; Tiemblo, Pilar; 2021; Polymer gel electrolytes for secondary aluminium batteries, prepared with the deep eutectic solvent uralumina (urea:AlCl3) and poly(ethylene oxide) of different molecular weight and at different concentrations; DIGITAL.CSIC; http://dx.doi.org/10.20350/digitalCSIC/13856 https://doi.org/10.1016/j.polymer.2021.123707 Sí |
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info:eu-repo/semantics/openAccess |
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openAccess |
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Elsevier |
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Elsevier |
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reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC instname:Consejo Superior de Investigaciones Científicas (CSIC) |
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DIGITAL.CSIC. Repositorio Institucional del CSIC |
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15,228081 |