Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion

Bai, Zhe; Wang, Zhenhua; Li, Ruilong; Wu, Zeyu; Feng, Pingli; Zhao, Lina; Wang, Tan; Hou, Wenshuo; Bai, Yu; Wang, Guoxiu; Mao, Yuqiong

doi:10.1021/acs.nanolett.3c00566

Cited by 12 publications

(2 citation statements)

References 52 publications

(58 reference statements)

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“…Co-N/G indicated a lower ∆G than N/G for the Li 2 S 2 reduction, implying a more favorable reaction pathway. Based on the ∆G calculations, various catalyst materials have been predicted, such as single atoms [77], metal oxides [78][79][80], sulfides [81], nitrides [82,83], and heterostructures [84,85], which present accelerated conversion kinetics for Li-S batteries.…”

Section: Gibbs Free Energymentioning

confidence: 99%

Theoretical Calculations Facilitating Catalysis for Advanced Lithium-Sulfur Batteries

Fang,

Zhou,

Chen

et al. 2023

Molecules

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Lithium-sulfur (Li-S) batteries have emerged as one of the most hopeful alternatives for energy storage systems. However, the commercialization of Li-S batteries is still confronted with enormous hurdles. The poor conductivity of sulfur cathodes induces sluggish redox kinetics. The shuttling of polysulfides incurs the heavy failure of electroactive substances. Tremendous efforts in experiments to seek efficient catalysts have achieved significant success. Unfortunately, the understanding of the underlying catalytic mechanisms is not very detailed due to the complicated multistep conversion reactions in Li-S batteries. In this review, we aim to give valuable insights into the connection between the catalyst activities and the structures based on theoretical calculations, which will lead the catalyst design towards high-performance Li-S batteries. This review first introduces the current advances and issues of Li-S batteries. Then we discuss the electronic structure calculations of catalysts. Besides, the relevant calculations of binding energies and Gibbs free energies are presented. Moreover, we discuss lithium-ion diffusion energy barriers and Li2S decomposition energy barriers. Finally, a Conclusions and Outlook section is provided in this review. It is found that calculations facilitate the understanding of the catalytic conversion mechanisms of sulfur species, accelerating the development of advanced catalysts for Li-S batteries.

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Section: Gibbs Free Energymentioning

confidence: 99%

Theoretical Calculations Facilitating Catalysis for Advanced Lithium-Sulfur Batteries

Fang,

Zhou,

Chen

et al. 2023

Molecules

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“…Due to its high ionic conductivity, LLTO accelerated the transformation of LiPSs and inhibited the shuttling of LiPSs. Although ionic conductor catalytic materials have shown higher-than-expected cycling performance in LSBs, few researchers have studied the mechanism of the triple-phase interface formed by ionic conductor catalytic electrode on LSBs, which is critical for the application of ionic conductor materials in LSBs. − …”

Section: Introductionmentioning

confidence: 99%

Ion/Electron Co-Conductive Triple-Phase Interface Enabling Fast Redox Reaction Kinetics in Lithium–Sulfur Batteries

Wang,

Li,

Shen

et al. 2024

ACS Appl. Mater. Interfaces

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Lithium−sulfur batteries (LSBs) are promising nextgeneration energy storage systems because of their high energy densities and high theoretical specific capacities. However, most catalysts in the LSBs are based on carbon materials, which can only improve the conductivity and are unable to accelerate lithium-ion transport. Therefore, it would be worthwhile to develop a catalytic electrode exhibiting both ion and electron conductivity. Herein, a triple-phase interface using lithium lanthanum titanate/carbon (LLTO/C) nanofibers to construct ion/electron co-conductive materials was used to afford enhanced adsorption of lithium polysulfides (LiPSs), high conductivity, and fast ion transport in working LSBs. The triple-phase interface accelerates the kinetics of the soluble LiPSs and promotes uniform Li 2 S precipitation/ dissolution. Additionally, the LLTO/C nanofibers decrease the reaction barrier of the LiPSs, significantly improving the conversion of LiPSs to Li 2 S and promoting rapid conversion. Specifically, the LLTO promotes ion transport owing to its high ionic conductivity, and the carbon enhances the conductivity to improve the utilization rate of sulfur. Therefore, the LSBs with LLTO/C functional separators deliver stable life cycles, high rates, and good electrocatalytic activities. This strategy is greatly important for designing ion/electron conductivity and interface engineering, providing novel insight for the development of the LSBs.

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Promoting Li₂S Nucleation/Dissolution Kinetics via Multiple Active Sites over TiVCrMoC₃T_x Interface

Zou,

Liang,

Zhou

et al. 2024

Small

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Lithium–sulfur batteries (LSBs) are still limited by some issues such as polysulfides shuttle and lithium dendrites. Recently, the concept “high‐entropy” has been considered as the research hotspot and international frontier. Herein, a high entropy MXene (TiVCrMoC3Tx, HE‐MXene) doped graphene is designed as the modified coating on commercial separators for LSBs. The HE‐MXene affords multiple metal active sites, fast Li+ diffusion rate, and efficient adsorption toward polysulfide intermediates. Furthermore, strong lithophilic property is favorable for uniform Li+ deposition. The combination of in situ characterizations confirms TiVCrMoC3Tx effectively promotes the Li2S nucleation/dissolution kinetics, reduces the Li+ diffusion barrier, and exhibits favorable lithium uniform deposition behavior. This TiVCrMoC3Tx/G@PP provides a high‐capacity retention rate after 1000 cycles at 1 C and 2 C, with a capacity decay rate of merely 0.021% and 0.022% per cycle. Surprisingly, the cell operates at a low potential of 48 mV while maintaining at 5 mA cm−2/5 mAh cm−2 for 4000 h. Furthermore, it still maintains a high‐capacity retention rate under a high sulfur loading of 4.8/6.4 mg cm−2 and a low E/S ratio of 8.6/7.5 µg mL−1. This work reveals a technical roadmap for simultaneously addressing the cathode and anode challenge, thus achieving potential commercially viable LSBs.

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Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion

Cited by 12 publications

References 52 publications

Theoretical Calculations Facilitating Catalysis for Advanced Lithium-Sulfur Batteries

Theoretical Calculations Facilitating Catalysis for Advanced Lithium-Sulfur Batteries

Ion/Electron Co-Conductive Triple-Phase Interface Enabling Fast Redox Reaction Kinetics in Lithium–Sulfur Batteries

Promoting Li₂S Nucleation/Dissolution Kinetics via Multiple Active Sites over TiVCrMoC₃T_x Interface

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Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion

Cited by 12 publications

References 52 publications

Theoretical Calculations Facilitating Catalysis for Advanced Lithium-Sulfur Batteries

Theoretical Calculations Facilitating Catalysis for Advanced Lithium-Sulfur Batteries

Ion/Electron Co-Conductive Triple-Phase Interface Enabling Fast Redox Reaction Kinetics in Lithium–Sulfur Batteries

Promoting Li2S Nucleation/Dissolution Kinetics via Multiple Active Sites over TiVCrMoC3Tx Interface

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Product

Resources

About

Promoting Li₂S Nucleation/Dissolution Kinetics via Multiple Active Sites over TiVCrMoC₃T_x Interface