Field‐assisted electrocatalysts spark sulfur redox kinetics: From fundamentals to applications

Li, Hongtai; Li, Yanguang; Zhang, Liang; Li, Gaoran; Sun, Xueliang

doi:10.1002/idm2.12087

Cited by 12 publications

(1 citation statement)

References 232 publications

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“…Lithium–sulfur (Li–S) batteries use abundant element S as the cathode material and lithium metal as anodes, which deliver high theoretic specific energy (2567 Wh kg –1 ) and are considered potential candidates for next-generation energy storage systems. However, Li–S batteries suffer from several issues, − such as the poor conductivity of active material sulfur , and discharge product of Li 2 S, large volume change upon cycling, , shuttling effect of polysulfides, , slow redox kinetics, − and so forth. Therefore, the practical applications of Li–S batteries must overcome these challenges.…”

Section: Introductionmentioning

confidence: 99%

V-Doped CoSe₂ Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

Li,

Wang

et al. 2024

ACS Appl. Mater. Interfaces

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Lithium−sulfur (Li−S) batteries have high theoretical energy density and are regarded as a promising candidate for next-generation energy storage systems. However, their practical applications are hindered by the slow kinetics of sulfur conversion and polysulfide shuttling. In particular, large-scale pouch cells show much poor cyclability. Here, we develop a high-efficiency catalyst of V-doped CoSe 2 by studying the binary CoSe 2 −VSe 2 system and confirming its effectiveness in accelerating polysulfide conversion. The coin cell tests reveal an initial capacity of 1414 mAh g −1 at 0.1 C and 1049 mAh g −1 at 1 C and demonstrate 1000 times cyclability with a decaying rate of 0.05% per cycle. Furthermore, the assembly and construction of pouch cells were optimized with monolithic three-dimensional (3D) electrodes and a multistacking strategy. Specifically, a 3D metallic scaffold (3MS) was developed to host V-doped CoSe 2 nanowires and sulfur. In addition, Janus microspheres of C@TiO 2 were synthesized to capture polar polysulfides with their polar part of TiO 2 and adsorb nonpolar sulfur with their nonpolar part of carbon. By integrating with 3MS, C@TiO 2 microspheres can block all ion channels of 3MS and only allow Li ions in and out. These integral designs and monolithic structures enable multistacking pouch cells with high cyclability. A high-loading pouch cell was demonstrated with a total capacity of 700 mAh. The cell can be cycled for 70 times with a capacity retention of 65.7%. In brief, this work provides an integral strategy of catalyst design and overall 3D assembly for practical Li−S batteries in a large pouch cell format.

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Section: Introductionmentioning

confidence: 99%

V-Doped CoSe₂ Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

Li,

Wang

et al. 2024

ACS Appl. Mater. Interfaces

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Challenges and Solutions for Lithium–Sulfur Batteries with Lean Electrolyte

Shi,

Sun,

Cao

et al. 2023

Adv Funct Materials

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Lithium–sulfur (Li–S) batteries have high theoretical energy density and are regarded as next‐generation batteries. However, their practical energy density is much lower than the theoretical value. In previous studies, the increase of the areal capacity of the cathode and the decrease of the negative/positive ratio can be well achieved, yet the energy density shows no corresponding increase. The main reason is the difficulty in decreasing electrolyte dosage because lean electrolyte inevitably causes the deterioration of reaction kinetics and sulfur utilization. Thus, the electrolyte/active material ratio in the reported works is usually higher than 10 µL mg−1, much higher than that in Li‐ion batteries (usually lower than ≈0.3 µL mg−1 for cathode). Although many works have focused on this topic, a systematic discussion is still rare. This review systematically discusses the key challenges and solutions for assembling high‐performance lean‐electrolyte Li–S batteries. First, the key challenges arising from lean‐electrolyte conditions are discussed in detail. Then, the approaches and the recent progress to reduce electrolyte usage, including optimization of electrode porosity and ion conduction, the introduction of electrocatalysis, exploration of new active materials, electrolyte regulation, and Li metal protection are reviewed. Finally, future research directions in lean‐electrolyte Li–S batteries are proposed.

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Xanthate‐Mediated Oxidation of Li₂S as the Lithium‐Containing Cathode in Lithium−Sulfur Batteries with Extremely Low Overpotential

Wu,

Ye,

et al. 2024

Advanced Materials

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Lithium−sulfide (Li2S) has long been pursued as a lithium‐containing cathode material for high‐energy‐density lithium‐sulfur (Li−S) batteries. Unfortunately, its direct oxidation generally has a large overpotential, giving rise to low energy efficiency. The use of redox mediators to accelerate the conversion of solid Li2S to polysulfides represents a possible solution to lower the initial oxidation overpotential. However, most reported redox mediators exhibit significantly higher redox potentials than the desirable value. Herein, it is serendipitously found that lithium ethyl xanthate (LiEX) formed from the reaction among Li2S, ethanol, and CS2 at room temperature is an efficient redox mediator. It has a redox potential (≈2.3 V vs Li+/Li) close to the electrochemical oxidation potential of Li2S (2.25 V vs Li+/Li), which enables fast Li2S oxidation reaction kinetics, and more importantly, lowers the Li2S oxidation potential from ≈3.6 to ≈2.3 V. When further integrated with an Ni–NC catalyst in a tandem catalysis scheme, a remarkable specific capacity of ≈1100 mAh g−1 at 0.2 mA cm−2 and long cycle life of 1400 cycles with ∼73% capacity retention is achieved, outperforming those of other Li2S‐based cathode materials from recent literature.

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Field‐assisted electrocatalysts spark sulfur redox kinetics: From fundamentals to applications

Cited by 12 publications

References 232 publications

V-Doped CoSe₂ Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

V-Doped CoSe₂ Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

Challenges and Solutions for Lithium–Sulfur Batteries with Lean Electrolyte

Xanthate‐Mediated Oxidation of Li₂S as the Lithium‐Containing Cathode in Lithium−Sulfur Batteries with Extremely Low Overpotential

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Field‐assisted electrocatalysts spark sulfur redox kinetics: From fundamentals to applications

Cited by 12 publications

References 232 publications

V-Doped CoSe2 Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

V-Doped CoSe2 Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

Challenges and Solutions for Lithium–Sulfur Batteries with Lean Electrolyte

Xanthate‐Mediated Oxidation of Li2S as the Lithium‐Containing Cathode in Lithium−Sulfur Batteries with Extremely Low Overpotential

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V-Doped CoSe₂ Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

V-Doped CoSe₂ Nanowire Catalysts in a 3D-Structured Electrode for Durable Li–S Pouch Cells

Xanthate‐Mediated Oxidation of Li₂S as the Lithium‐Containing Cathode in Lithium−Sulfur Batteries with Extremely Low Overpotential