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1.
Adv Mater ; 34(39): e2204810, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35953449

RESUMEN

Designing efficient electrocatalysts with high electroconductivity, strong chemisorption, and superior catalytical efficiency to realize rapid kinetics of the lithium polysulfides (LiPSs) conversion process is crucial for practical lithium-sulfur (Li-S) battery applications. Unfortunately, most current electrocatalysts cannot maintain long-term stability due to the possible failure of catalytic sites. Herein, a novel dynamic electrocatalytic strategy with the liquid metal (i.e., gallium-tin, EGaSn) to facilitate LiPSs redox reaction is reported. The combined theoretical simulations and microstructure experiment analysis reveal that Sn atoms dynamically distributed in the liquid Ga matrix act as the main active catalytic center. Meanwhile, Ga provides a uniquely dynamic environment to maintain the long-term integrity of the catalytic system. With the participation of EGaSn, a tailor-made 2 Ah Li-S pouch cell with a specific energy density of 307.7 Wh kg-1 is realized. This work opens up new opportunities for liquid-phase binary alloys as electrocatalysts for high-specific-energy Li-S batteries.

2.
Nat Commun ; 13(1): 5, 2022 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-35013151

RESUMEN

Extra-terrestrial explorations require electrochemical energy storage devices able to operate in gravity conditions different from those of planet earth. In this context, lithium (Li)-based batteries have not been fully investigated, especially cell formation and cycling performances under supergravity (i.e., gravity > 9.8 m s-2) conditions. To shed some light on these aspects, here, we investigate the behavior of non-aqueous Li metal cells under supergravity conditions. The physicochemical and electrochemical characterizations reveal that, distinctly from earth gravity conditions, smooth and dense Li metal depositions are obtained under supergravity during Li metal deposition on a Cu substrate. Moreover, supergravity allows the formation of an inorganic-rich solid electrolyte interphase (SEI) due to the strong interactions between Li+ and salt anions, which promote significant decomposition of the anions on the negative electrode surface. Tests in full Li metal pouch cell configuration (using LiNi0.8Co0.1Mn0.1O2-based positive electrode and LiFSI-based electrolyte solution) also demonstrate the favorable effect of the supergravity in terms of deposition morphology and SEI composition and ability to carry out 200 cycles at 2 C (400 mA g-1) rate with a capacity retention of 96%.

3.
ACS Appl Mater Interfaces ; 11(28): 25147-25154, 2019 Jul 17.
Artículo en Inglés | MEDLINE | ID: mdl-31199107

RESUMEN

Lithium-sulfur (Li-S) batteries are strong contenders among lithium batteries due to superior capacity and energy density, but the polysulfide shuttling effect limits the cycle life and reduces energy efficiency due to a voltage gap between charge and discharge. Here, we demonstrate that graphene foam impregnated with single-atom catalysts (SACs) can be coated on a commercial polypropylene separator to catalyze polysulfide conversion, leading to a reduced voltage gap and a much improved cycle life. Also, among Fe/Co/Ni SACs, Fe SACs may be a better option to be used in Li-S systems. By deploying SACs in the battery separator, cycling stability improves hugely, especially considering relatively high sulfur loading and ultralow SAC contents. Even at a metal loading of ∼2 µg in the whole cell, an Fe SAC-modified separator delivers superior Li-S battery performance even at high sulfur loading (891.6 mAh g-1, 83.7% retention after 750 cycles at 0.5C). Our work further enriches and expands the application of SACs catalyzing polysulfide blocking and conversion and improving round trip efficiencies in batteries, without side effects such as electrolyte and electrode decomposition.

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