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Beyond lithium-ion technologies, lithium−sulfur batteries stand out because of their multielectron redox reactions and high theoretical specific energy (2500 Wh kg−1). However, the intrinsic irreversible transformation of soluble lithium polysulfides to solid short-chain sulfur species (Li2S2 and Li2S) and the associated large volume change of electrode materials significantly impair the long-term stability of the battery. Here we present a liquid sulfur electrode consisting of lithium thiophosphate complexes dissolved in organic solvents that enable the bonding and storage of discharge reaction products without precipitation. Insights garnered from coupled spectroscopic and density functional theory studies guide the complex molecular design, complexation mechanism, and associated electrochemical reaction mechanism. With the novel complexes as cathode materials, high specific capacity (1425 mAh g−1 at 0.2 C) and excellent cycling stability (80% retention after 400 cycles at 0.5 C) are achieved at room temperature. Moreover, the highly reversible all-liquid electrochemical conversion enables excellent low temperature battery operability (>400 mAh g−1 at −40 °C and >200 mAh g−1 at −60 °C). This work opens new avenues to design and tailor the sulfur electrode for enhanced electrochemical performance across a wide operating temperature range.
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A comparative study on the production of Ni1/3Co1/3Mn1/3C2O4 cathode precursor material for lithium-ion batteries using batch and slug-flow reactors
The intermittent nature of the renewable energy sources drifts research interest towards various electrochemical energy storage devices, such as the lithium ion battery, which offers consistent power supply. The manufacturing cost and electrochemical performance of a battery pack largely depends on the quality of the cathode material, which further depends on the production method and its parameters. However, the traditional stirred tank-based co-precipitation manufacturing process for precursors of lithium nickel manganese cobalt oxide (NCM111) cathode suffers from inhomogeneity in the reaction environment, which leads to non-uniform morphology and particle size distribution (PSD). In this work, slug-flow-based manufacturing platform, which offers a homogeneous reaction environment, is used for the continuous production of NCM111 oxalate precursors. One of the novel features of this work is the comparative study between the quality of batch and slug-flow-derived products. The slug-flow-derived product is found to be better in terms of having bigger particle size, narrower PSD and higher tap density. The study on the single and dual-element precipitation in similar conditions to understand the co-precipitation behavior in the slug-flow manufacturing platform is also a unique feature of this work. Furthermore, the effect of NH4OH concentration and residence time (RT) on the electrochemical performance of cathode were also studied and it is found that the cathode precursors synthesized at a NH4OH concentration of 0.08 M and a RT of 2 minutes followed by lithiation shows a better electrochemical performance of 128 mAh g−1 at 0.1 C with cycling stability of more than 80% both at 0.5 C and 1 C.
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- Award ID(s):
- 1940948
- PAR ID:
- 10565594
- Publisher / Repository:
- Elsevier
- Date Published:
- Journal Name:
- Journal of Alloys and Compounds
- Volume:
- 994
- Issue:
- C
- ISSN:
- 0925-8388
- Page Range / eLocation ID:
- 174720
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1016/j.jallcom.2024.174720
