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: Low-Concentration Electrolyte Design for Wide-Temperature Operation in Sodium Metal Batteries
Sodium metal batteries (SMBs) are cost-effective and environmentally sustainable alternative to lithium batteries. However, at present, limitations such as poor compatibility, low coulombic efficiency (CE), and high electrolyte cost hinder their widespread application. Herein, we propose a non-flammable, low-concentration electrolyte composed of 0.3 M NaPF6in propylene carbonate (PC), fluoroethylene carbonate (FEC), and 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE). This low-concentration electrolyte not only reduces cost but also delivers rapid ion diffusion and superior wetting properties. While the Na||FePO4system with this electrolyte demonstrates slightly reduced performance at room temperature compared to standard-concentration formulations (S-PFT), it excels at both high (55 °C) and low (−20 °C) temperatures, showcasing its balanced performance. At 0.5 C (charge)/1 C (discharge), capacity retention reaches 92.8% at room temperature and 98.5% at elevated temperature, with CE values surpassing 99% and 99.63%, respectively, and significant performance sustained at −20 °C at 0.2 C. This electrolyte development thus offers a well-rounded, economically viable path to high-performance SMBs for diverse environmental applications.  more » « less
Award ID(s):
2208840
PAR ID:
10655904
Author(s) / Creator(s):
; ; ;
Publisher / Repository:
The Electrochemical Society
Date Published:
Journal Name:
Journal of The Electrochemical Society
Volume:
172
Issue:
1
ISSN:
0013-4651
Page Range / eLocation ID:
010501
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; (, Advanced Functional Materials)
    Abstract Aqueous zinc‐ion batteries are promising alternatives to lithium‐ion batteries due to their cost‐effectiveness and improved safety. However, several challenges, including corrosion, dendrites, and water decomposition at the Zn anode, hinder their performance. Herein, an approach is proposed, that deviates from the conventional design by adding water into a propylene carbonate‐based organic electrolyte to prepare a non‐flammable “water‐in‐organic” electrolyte. The chaotropic salt Zn(ClO4)2exploits the Hofmeister effect to promote the miscibility of immiscible liquid phases. Interactions between propylene carbonate and water restrict water activity and mitigate unfavorable reactions. This electrolyte facilitates preferential Zn (002) deposition and the formation of solid electrolyte interphase. Consequently, the “water‐in‐organic” electrolyte achieves a 99.5% Coulombic efficiency at 1 mA cm−2over 1000 cycles in Zn/Cu cells, and constant cycling over 1000 h in Zn/Zn symmetric cells. A Na0.33V2O5/Zn battery exhibits impressive cycling stability with a capacity of 175 mAh g−1for 800 cycles at 2 A g−1. Additionally, this electrolyte enables sustainable cycling across a wide temperature range from −20 to 50 °C. The design of a “water‐in‐organic” electrolyte employing a chaotropic salt presents a potential strategy for high‐performance electrolytes in zinc‐ion batteries with a large stability window and a wide temperature range. 
    more » « less
  2. ; ; ; ; ; (, Journal of The Electrochemical Society)
    An investigation of alternative lithium salts, lithium tetrafluoroborate (LiBF 4 ), lithium difluoro(oxalato)borate (LiDFOB) and lithium hexafluorophosphate (LiPF 6 ), in novel ester-based (methyl acetate/fluoroethylene carbonate- MA/FEC or methyl propionate/fluoroethylene carbonate- MP/FEC) electrolyte formulations has been conducted in LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622)/graphite cells to improve low temperature cycling performance of lithium ion batteries at −20 °C. Improved low temperature performance was observed with all the lithium salts in MA/FEC electrolyte while comparable room temperature (25 °C) capacities were observed with LiPF 6 salt only. Detailed ex-situ analysis of surface films generated with LiBF 4 , LiDFOB and LiPF 6 in ester-based electrolytes reveals that the solid electrolyte interphase (SEI) is predominately composed of lithium salt decompaction products and addition of 10% FEC (by volume%) may not be sufficient at forming a protective SEI. 
    more » « less
  3. ; ; ; ; ; ; (, 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
  4. ; ; ; ; ; ; ; ; (, Journal of The Electrochemical Society)
    The thermal stability of ∼420 mAh Na0.97Ca0.03[Mn0.39Fe0.31Ni0.22Zn0.08]O2(NCMFNZO)/hard carbon (HC) pouch cells was investigated using accelerating rate calorimetry (ARC) at elevated temperatures. 1 m NaPF6in propylene carbonate (PC):ethyl methyl carbonate (EMC) (1:1 by volume) was used as a control electrolyte. Adding 2 wt% fluoroethylene carbonate to the electrolyte improves the cell’s thermal stability by decreasing the self-heating rate (SHR) across the whole testing temperature range. The selected states-of-charge (SoC), including 70%, 84%, and 100%, exhibit minimal impact on the exothermic behavior, except for a slight decrease in SHR after ∼275 °C at 70% SoC. When compared to traditional lithium-ion batteries operating at 100% SoC, NCMFNZO/HC pouch cells demonstrate inferior thermal stability compared to LiFePO4(LFP)/graphite pouch cells, displaying a higher SHR from 220 to 300 °C. LiNi0.8Mn0.1Co0.1O2/graphite + SiOxpouch cells exhibit the worst safety performance, with an early onset temperature of ∼100 °C and the highest SHR across the entire temperature range. These results offer a direct comparison of the impact of SoC and electrolyte compositions on the thermal stability of SIBs at elevated temperatures, highlighting that there is still room for improvement in SIBs safety performance compared to LFP/graphite chemistry. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; ; et al (, Advanced Materials)
    Abstract Iron is a promising candidate for a cost‐effective anode for large‐scale energy storage systems due to its natural abundance and well‐established mass production. Recently, Fe‐ion batteries (FeIBs) that use ferrous ions as the charge carrier have emerged as a potential storage solution. The electrolytes in FeIBs are necessarily acidic to render the ferrous ions more anodically stable, allowing a wide operation voltage window. However, the iron anode suffers severe hydrogen evolution reaction with a low Coulombic efficiency (CE) in an acidic environment, shortening the battery cycle life. Herein, a hybrid aqueous electrolyte that forms a solid‐electrolyte interphase (SEI) layer on the Fe anode surface is introduced. The electrolyte mainly comprises FeCl2and ZnCl2as cosalts, where the Zn‐Cl anionic complex species of the concentrated ZnCl2allows dimethyl carbonate (DMC) to be miscible with the aqueous ferrous electrolyte. SEI derived from DMC's decomposition passivates the iron surface, which leads to an average CE of 98.3% and much‐improved cycling stability. This advancement shows the promise of efficient and durable FeIBs. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Text Encoded Conversion
  • XML
  • Save / Share this Record
  • Send to Email