Review—Polymer Electrolytes for Magnesium Batteries: Forging Away from Analogs of Lithium Polymer Electrolytes and Towards the Rechargeable Magnesium Metal Polymer Battery
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Solid inorganic and polymeric electrolytes have the potential to enable rechargeable batteries with higher energy densities, compared to current lithium-ion technology, which uses liquid electrolyte. Inorganic materials such as ceramics and glasses conduct lithium ions well, but they are brittle, which makes incorporation into a battery difficult. Polymers have the flexibility for facile use in a battery, but their transport properties tend to be inferior to inorganics. Thus, there is growing interest in composite electrolytes with inorganic and organic phases in intimate contact. This article begins with a discussion of ion transport in single-phase electrolytes. A dimensionless number (the Newman number) is presented for quantifying the efficacy of electrolytes. An effective medium framework for predicting transport properties of composite electrolytes containing only one conducting phase is then presented. The opportunities and challenges presented by composite electrolytes containing two conducting phases are addressed. Finally, the importance and status of reaction kinetics at the interfaces between solid electrolytes and electrodes are covered, using a lithium-metal electrode as an example.more » « less
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Nanoparticle organic hybrid materials (NOHMs) have been proposed as excellent electrolytes for combined CO2capture and electrochemical conversion due to their conductive nature and chemical tunability. However, CO2capture behavior and transport properties of these electrolytes after CO2capture have not yet been studied. Here, we use a variety of nuclear magnetic resonance (NMR) techniques to explore the carbon speciation and transport properties of branched polyethylenimine (PEI) and PEI-grafted silica nanoparticles (denoted as NOHM-I-PEI) after CO2capture. Quantitative13C NMR spectra collected at variable temperatures reveal that absorbed CO2exists as carbamates (RHNCOO−or RR′NCOO−) and carbonate/bicarbonate (CO32−/HCO3−). The transport properties of PEI and NOHM-I-PEI studied using1H pulsed-field-gradient NMR, combined with molecular dynamics simulations, demonstrate that coulombic interactions between negatively and positively charged chains dominate in PEI, while the self-diffusion in NOHM-I-PEI is dominated by silica nanoparticles. These results provide strategies for selecting adsorbed forms of carbon for electrochemical reduction.more » « less
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