skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Interfaces in rechargeable magnesium batteries
This minireview provides a concise overview on the development of electrolytes for rechargeable magnesium (Mg) batteries. It elucidates the intrinsic driving force of the evolution from Grignard-based electrolytes to electrolytes based on simple Mg salts. Additional discussion includes the key electrochemical processes at the interfaces in Mg electrolytes, with a focus on unaddressed issues and future research directions.  more » « less
Award ID(s):
2004497
PAR ID:
10287261
Author(s) / Creator(s):
; ; ;
Date Published:
Journal Name:
Nanoscale Horizons
Volume:
5
Issue:
11
ISSN:
2055-6756
Page Range / eLocation ID:
1467 to 1475
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; (, Energy & Environmental Science)
    null (Ed.)
    Due to its high theoretical energy density and relative abundancy of active materials, the magnesium–sulfur battery has attracted research attention in recent years. A closely related system, the lithium-sulfur battery, can suffer from serious self-discharge behavior. Until now, the self-discharge of Mg–S has been rarely addressed. Herein, we demonstrate for a wide variety of Mg–S electrolytes and conditions that Mg–S batteries also suffer from serious self-discharge. For a common Mg–S electrolyte, we identify a multi-step self-discharge pathway. Covalent S 8 diffuses to the metal Mg anode and is converted to ionic Mg polysulfide in a non-faradaic reaction. Mg polysulfides in solution are found to be meta-stable, continuing to react and precipitate as solid magnesium polysulfide species during both storage and active use. Mg–S electrolytes from the early, middle, and state-of-the-art stages of the Mg–S literature are all found to enable the self-discharge. The self-discharge behavior is found to decrease first cycle discharge capacity by at least 32%, and in some cases up to 96%, indicating this is a phenomenon of the Mg–S chemistry that deserves focused attention. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; ; et al (, Materials Horizons)
    The utilization of metallic anodes holds promise for unlocking high gravimetric and volumetric energy densities and is pivotal to the adoption of ‘beyond Li’ battery chemistries. Much of the promise of magnesium batteries stems from claims regarding their lower predilection for dendrite growth. Whilst considerable effort has been invested in the design of novel electrolytes and cathodes, detailed studies of Mg plating are scarce. Using galvanostatic electrodeposition of metallic Mg from Grignard reagents in symmetric Mg–Mg cells, we establish a phase map characterized by disparate morphologies spanning the range from fractal aggregates of 2D nanoplatelets to highly anisotropic dendrites with singular growth fronts and nanowires entangled in the form of mats. The effects of electrolyte concentration, applied current density, and coordinating ligands have been explored. The study demonstrates a complex range of electrodeposited morphologies including canonical dendrites with shear moduli conducive to penetration through typical polymeric separators. We further demonstrate a strategy for mitigating Mg dendrite formation based on the addition of molecular Lewis bases that promote nanowire growth through selective surface coordination. 
    more » « less
  3. ; ; ; ; ; ; ; ; ; (, Angewandte Chemie International Edition)
    Abstract Oxidative anion insertion into graphite in an aqueous environment represents a significant challenge in the construction of aqueous dual‐ion batteries. In dilute aqueous electrolytes, the oxygen evolution reaction (OER) dominates the anodic current before anions can be inserted into the graphite gallery. Herein, we report that the reversible insertion of Mg‐Cl superhalides in graphite delivers a record‐high reversible capacity of 150 mAh g−1from an aqueous deep eutectic solvent comprising magnesium chloride and choline chloride. The insertion of Mg‐Cl superhalides in graphite does not form staged graphite intercalation compounds; instead, the insertion of Mg‐Cl superhalides makes the graphite partially turbostratic. 
    more » « less
  4. ; ; (, ChemPhysChem)
    Abstract Metal‐sulfur batteries are a promising next‐generation energy storage technology, offering high theoretical energy densities with low cost and good sustainability. An active area of research is the development of electrolytes that address unwanted migration of sulfur and intermediate species known as polysulfides during operation of metal‐sulfur batteries, a phenomenon that leads to low energy efficiency and short life‐spans. A particular class of electrolytes, gel polymer electrolytes, are especially attractive for their ability to repel polysulfides on the basis of structure, electrostatics, and other polymer properties. Herein, within the context of magnesium‐ and lithium‐sulfur batteries, we investigate the impact of gel polymer electrolyte cation solvation capacity, a property related to network dielectric constant and chemistry, on sulfur/polysulfide‐polymer interactions, an understudied property‐performance relationship. Polymers with lower cation solvation capacity are found to permanently absorb less polysulfide active material, which increases sulfur utilization for Li−S batteries and significantly increases charge efficiency and life‐span for Li−S and Mg−S batteries. 
    more » « less
  5. ; ; ; ; ; ; (, ChemSusChem)
    Abstract All‐solid‐state batteries have the potential for enhanced safety and capacity over conventional lithium ion batteries, and are anticipated to dominate the energy storage industry. As such, strategies to enable recycling of the individual components are crucial to minimize waste and prevent health and environmental harm. Here, we use cold sintering to reprocess solid‐state composite electrolytes, specifically Mg and Sr doped Li7La3Zr2O12with polypropylene carbonate (PPC) and lithium perchlorate (LLZO−PPC−LiClO4). The low sintering temperature allows co‐sintering of ceramics, polymers and lithium salts, leading to re‐densification of the composite structures with reprocessing. Reprocessed LLZO−PPC−LiClO4exhibits densified microstructures with ionic conductivities exceeding 10−4 S/cm at room temperature after 5 recycling cycles. All‐solid‐state lithium batteries fabricated with reprocessed electrolytes exhibit a high discharge capacity of 168 mA h g−1at 0.1 C, and retention of performance at 0.2 C for over 100 cycles. Life cycle assessment (LCA) suggests that recycled electrolytes outperforms the pristine electrolyte process in all environmental impact categories, highlighting cold sintering as a promising technology for recycling electrolytes. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email