Towards practical cells: combined use of titanium black as a cathode additive and sparingly solvating electrolyte for high-energy-density lithium–sulfur batteries

Liu, Jiali; Li, Shanglin; Marium, Mayeesha; Wang, Binshen; Ueno, Kazuhide; Dokko, Kaoru; Watanabe, Masayoshi

doi:10.1039/d1se00042j

Cited by 18 publications

(31 citation statements)

References 60 publications

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“…Consequently, Cuisinier et al [100] , Lee et al [101] , Shyamsunder et al [102] proposed new different concepts of "sparingly solvating electrolytes", which consists of a low donor number solvent as a co-solvent or as a solo solvent when a low ion-pairing Li salt is used. Following this concept, other research groups, such as Nakanishi et al in Japan and Piwko et al in Germany, also actively contributed to this regard [103][104][105][106][107] . It is noteworthy that with the change from electrolytes with high PS solubility to such "sparingly solvating electrolytes", the whole cell chemistry is changed simultaneously.…”

Section: Qsspe Systemsmentioning

confidence: 98%

Perspective of polymer-based solid-state Li-S batteries

Castillo¹,

Qiao²,

Santiago³

et al. 2022

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Li-S batteries, as the most promising post Li-ion technology, have been intensively investigated for more than a decade. Although most previous studies have focused on liquid systems, solid electrolytes, particularly all-solidstate polymer electrolytes (ASSPEs) and quasi-solid-state polymer electrolyte (QSSPEs), are appealing for Li-S cells due to their excellent flexibility and mechanical stability. Such Li-S batteries not only provide significantly improved safety but are also expected to augment the all-inclusive energy density compared to liquid systems. Therefore, this perspective briefly summarizes the recent progress on polymer-based solid-state Li-S batteries, with a special focus on electrolytes, including ASSPEs and QSSPEs. Furthermore, future work is proposed based on the existing development and current challenges.

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Section: Qsspe Systemsmentioning

confidence: 98%

Perspective of polymer-based solid-state Li-S batteries

Castillo¹,

Qiao²,

Santiago³

et al. 2022

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“…In addition, the homogeneously distributed TiB contributes to the uniform growth of Li 2 S, thereby affecting the porosity of the discharged cathode. Our previous study [36] also demonstrated that sulfur cathodes show substantially different morphologies following the addition of TiB, especially after long‐term cycling. The porosity loss of the sulfur cathode was extremely severe in the case of TiB‐free cathodes, whereas it was maintained to a certain degree for the TiB‐added electrodes.…”

Section: Resultsmentioning

confidence: 85%

“…The poor wettability of the TiB‐free electrode to the electrolyte may also hinder the Li‐ion transport capability. In contrast, TiB included as a multifunctional sulfur cathode additive enabled the fabrication of crack‐free highly S‐loaded porous electrodes with a high wettability to the electrolyte [36] . To evaluate how these features affect the mass transport occurring within the sulfur cathode, we also examined the performance of the TiB‐added electrode under the same lean conditions using the G4 electrolyte.…”

Section: Resultsmentioning

confidence: 99%

“…In addition, Tables S2 and S3 show the electrode and separator conditions, respectively. In this study, we focused on the difference in the wettabilities of the cathodes [36] to evaluate the effect of TiB. Considering that the porous electrode containing TiB was reported to have high wettability, [36] it was assumed that the effect of TiB can be represented as an effective ion transfer network through the electrolyte phase in the porous electrode.…”

Section: Resultsmentioning

confidence: 99%

“…[34 ] However, to date, there have been very few reports on the usage of sparingly solvating electrolytes along with a relatively high sulfur loading in the cathode to achieve a low E/S ratio, and thus realise a high energy density at the practical cell level [32,35] . Our previous study proposed a commercially available black pigment, titanium black (TiB), as a multifunctional additive for sulfur cathodes [36] . The amphipathic nature of TiB enabled a homogeneous and thick coating of the electrode on a current collector (>4 mg cm −2 ), and led to improved electrode wettability by the electrolyte [36] .…”

Section: Introductionmentioning

confidence: 99%

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Importance of Mass Transport in High Energy Density Lithium‐Sulfur Batteries Under Lean Electrolyte Conditions

Ishikawa

Liu

et al. 2022

Batteries & Supercaps

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The operation of a lithium‐sulfur (Li−S) battery under lean electrolyte conditions is essential for enhancing the energy density to a practical level. It is rather challenging to reduce the amount of electrolyte in Li−S cells because the discharge reactions of sulfur (Li2Sx formation: x=8−1) occur via a fully dissolution/precipitation conversion mechanism in conventional electrolyte solutions. Therefore, the use of sparingly solvating electrolytes has been reported as an effective method to reduce the electrolyte content in Li−S cells. However, the majority of related research to date has been based on the use of an excess amount of electrolyte and low S loading. In this study, we investigated the performance of Li−S cells using cathodes with a relatively high S loading (>4 mg cm−2) under lean electrolyte conditions of sparingly solvating electrolytes. The products of inhomogeneous discharge reactions occurring at the separator side in the Li−S cell cathodes blocked the void spaces of the cathode, and the porosity of the cathode decreased due to the expansion of the active material. In addition, the ion pathway toward the interior parts of the electrode (close to the current collector) was hindered, and further discharge reactions were inhibited. The inhomogeneous discharge reactions could be alleviated by enhancing the transport properties of the electrolyte and adequately maintaining the porous structure of the cathode by incorporating an additive in it. The effects of these changes on the Li−S cell performance were also further confirmed by numerical simulations.

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Influence of Primary Particle Morphology and Hydrophilicity of Carbon Matrix on Electrode Coating Quality and Performance of Practical High‐Energy‐Density Li–S Batteries

Li,

Chen,

Yamamoto

et al. 2024

Adv Materials Inter

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Li–S batteries have attracted attention as the next‐generation secondary batteries. While substantial progress is made in understanding Li–S chemistry at a fundamental level, only a limited number of studies are dedicated to achieving high energy density at the practical pouch cell level. The challenge lies in attaining high‐energy‐density Li–S batteries under harsh conditions, which involve a minimal amount of electrolyte and a relatively high areal S‐loading cathode. This discrepancy creates a substantial gap between fundamental material research and comprehensive cell‐level investigations. In this study, it is investigated how the morphology and properties of two carbon materials, namely Ketjen black (KB) and mesoporous carbon nano‐dendrites (MCND), influence the composite cathode architecture and determine the performance of Li–S batteries. Unlike KB, MCND allows for a higher sulfur‐loading cathode without evident cracks in the composite cathode. This achievement can be attributed to the high porosity, excellent wettability, and high conductivity exhibited during an identical electrode preparation procedure. Furthermore, large‐format Li–S pouch cells incorporating MCND/S cathodes are successfully fabricated. These cells demonstrate an energy density surpassing 250 Wh kg−1 and an initial discharge capacity of 3.7 Ah under challenging conditions (S‐loading > 5 mg cm−2 and E/S < 3.5 µL mg−1).

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Towards practical cells: combined use of titanium black as a cathode additive and sparingly solvating electrolyte for high-energy-density lithium–sulfur batteries

Abstract: The lithium–sulfur (Li–S) battery is considered one of the most promising technologies for next-generation energy storage. To realise its practical applications, electrodes with high areal sulfur loading, low-cost raw materials,...

Cited by 18 publications

References 60 publications

Perspective of polymer-based solid-state Li-S batteries

Perspective of polymer-based solid-state Li-S batteries

Importance of Mass Transport in High Energy Density Lithium‐Sulfur Batteries Under Lean Electrolyte Conditions

Influence of Primary Particle Morphology and Hydrophilicity of Carbon Matrix on Electrode Coating Quality and Performance of Practical High‐Energy‐Density Li–S Batteries

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