Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation

Miguel, Álvaro; Jankowski, Piotr; Pablos, Jesús L.; Corrales, Teresa; López-Cudero, Ana; Bhowmik, Arghya; Carrasco‐Busturia, David; Ellis, Gary; García, Nuria; Garcı́a-Lastra, J. M.; Tiemblo, Pilar

doi:10.1016/j.polymer.2021.123707

Cited by 11 publications

(4 citation statements)

References 36 publications

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“…Figure 1d and Figure S3 (Supporting Information) show ionic conductivities of the polymer electrolytes as a function of SiO 2 and PEO content, ranging from 6.25 mS cm −1 (PE‐7‐0) to 15.3 mS cm −1 (PE‐6‐1). These values are in the same order of magnitude as the EMImCl‐AlCl 3 ionic liquid (≈19 mS cm −1 [ 37,38 ] ) and are comparatively higher than most other Al battery polymer electrolytes reported in the literature (0.25–6.61 mS cm −1 ), [ 10,11,18–20,27,28,39,40 ] owing to the high loading of ionic liquid within the electrolyte, at over 93 wt%. Similarly high ionic conductivities have been reported in polymer electrolytes with comparable ionic liquid loadings.…”

Section: Resultsmentioning

confidence: 78%

Solid Polymer Electrolytes with Enhanced Electrochemical Stability for High‐Capacity Aluminum Batteries

Leung,

Gordon,

Messinger

et al. 2024

Advanced Energy Materials

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Chloroaluminate ionic liquids are commonly used electrolytes in rechargeable aluminum batteries due to their ability to reversibly electrodeposit aluminum at room temperature. Progress in aluminum batteries is currently hindered by the limited electrochemical stability, corrosivity, and moisture sensitivity of these ionic liquids. Here, a solid polymer electrolyte based on 1‐ethyl‐3‐methylimidazolium chloride‐aluminum chloride, polyethylene oxide, and fumed silica is developed, exhibiting increased electrochemical stability over the ionic liquid while maintaining a high ionic conductivity of ≈13 mS cm−1. In aluminum–graphite cells, the solid polymer electrolytes enable charging to 2.8 V, achieving a maximum specific capacity of 194 mA h g−1 at 66 mA g−1. Long‐term cycling at 2.7 V showed a reversible capacity of 123 mA h g−1 at 360 mA g−1 and 98.4% coulombic efficiency after 1000 cycles. Solid‐state nuclear magnetic resonance spectroscopy measurements reveal the formation of five‐coordinate aluminum species that crosslink the polymer network to enable a high ionic liquid loading in the solid electrolyte. This study provides new insights into the molecular‐level design and understanding of polymer electrolytes for high‐capacity aluminum batteries with extended potential limits.

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Section: Resultsmentioning

confidence: 78%

Solid Polymer Electrolytes with Enhanced Electrochemical Stability for High‐Capacity Aluminum Batteries

Leung,

Gordon,

Messinger

et al. 2024

Advanced Energy Materials

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“…Chloride ions coordinate aluminum, forming different aluminum-chloride complexes, thus preventing an insulating aluminum oxide passivation film on the surface. [145] An electrochemical cell containing aluminum as the negative electrode, a chloride-based electrolyte, and a positive electrode of choice (graphite, organics, or sulfides [146,147] ) can be cycled up to high current densities without the formation of dendrites. [148] Although this is attractive, the use of highly corrosive and water-sensitive AlCl 3 hinders any possible practical application of this cell chemistry and calls for the development of less or completely non-corrosive electrolytes able to dissolve the passivation layer formed on aluminum to enable the plating/stripping process.…”

Section: Multivalent Anodesmentioning

confidence: 99%

Implications of the BATTERY 2030+ AI‐Assisted Toolkit on Future Low‐TRL Battery Discoveries and Chemistries

Bhowmik¹,

Berecibar

Casas‐Cabanas

et al. 2021

Advanced Energy Materials

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BATTERY 2030+ targets the development of a chemistry neutral platform for accelerating the development of new sustainable high-performance batteries.Here, a description is given of how the AI-assisted toolkits and methodologies developed in BATTERY 2030+ can be transferred and applied to representative examples of future battery chemistries, materials, and concepts. This perspective highlights some of the main scientific and technological challenges facing emerging low-technology readiness level (TRL) battery chemistries and concepts, and specifically how the AI-assisted toolkit developed within BIG-MAP and other BATTERY 2030+ projects can be applied to resolve these. The methodological perspectives and challenges in areas like predictive long time-and length-scale simulations of multi-species systems, dynamic processes at battery interfaces, deep learned multi-scaling and explainable AI, as well as AI-assisted materials characterization, self-driving labs, closed-loop optimization, and AI for advanced sensing and self-healing are introduced. A description is given of tools and modules can be transferred to be applied to a select set of emerging low-TRL battery chemistries and concepts covering multivalent anodes, metalsulfur/oxygen systems, non-crystalline, nano-structured and disordered systems, organic battery materials, and bulk vs. interface-limited batteries.

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“…However, the progress has been slow, with relatively few articles published on Al/S chemistry until recently. The discovery of an ionic liquid-based Al/S battery a few years ago opened a new direction in this battery chemistry, and more research results have been published in the last few years than all of the previous years combined. − In addition, significant recent work has focused on aluminum-ion batteries. − …”

Section: Introductionmentioning

confidence: 99%

Influence of Ionic Coordination on the Cathode Reaction Mechanisms of Al/S Batteries

et al. 2022

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The lack of knowledge on electrochemical reaction pathways for Al/S batteries prevents the development of practical approaches to mitigate the irreversibility and poor cycling performances of this appealing secondary battery system, which is, in theory, scalable, inexpensive, and energy-dense. Different from the Li/S system, Al/S batteries use ionic liquids (ILs) as electrolytes. The choice of the IL, i.e., whether the IL is based on a conventional EMImCl-based electrolyte or in a deep eutectic mixture of aluminum chloride with urea (or any of its derivatives), strongly affects the electrochemical energy-storage performance of the cell. To shed some light on the Al/S battery chemistry, here, we present the computational electrochemistry research work to determine the most favorable reaction pathways and thermodynamically stable reaction intermediates. We also discuss the effect of the coordination of ionic species (originated from aluminum-containing deep eutectic electrolytes) with polysulfide intermediates, which lead to alterations in the reaction pathway and electrochemical behavior of the Al/S system. The spectroscopic signatures from various reaction intermediates are also reported and validated via comparison with experimental observations.

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Polymers for aluminium secondary batteries: Solubility, ionogel formation and chloroaluminate speciation

Cited by 11 publications

References 36 publications

Solid Polymer Electrolytes with Enhanced Electrochemical Stability for High‐Capacity Aluminum Batteries

Solid Polymer Electrolytes with Enhanced Electrochemical Stability for High‐Capacity Aluminum Batteries

Implications of the BATTERY 2030+ AI‐Assisted Toolkit on Future Low‐TRL Battery Discoveries and Chemistries

Influence of Ionic Coordination on the Cathode Reaction Mechanisms of Al/S Batteries

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