Origin of shuttle-free sulfurized polyacrylonitrile in lithium-sulfur batteries

Huang, Chen‐Jui; Cheng, Ju‐Hsiang; Su, Wei‐Nien; Partovi–Azar, Pouya; Kuo, Liang-Yin; Tsai, Meng‐Che; Lin, Ming‐Hsien; Jand, Sara Panahian; Chan, Ting‐Shan; Wu, Nae‐Lih; Kaghazchi, Payam; Dai, Hongjie; Bieker, Peter

doi:10.1016/j.jpowsour.2021.229508

Cited by 39 publications

(61 citation statements)

References 66 publications

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“…[3,6,7] In this regard, polymeric materials have been widely proposed and investigated as alternative cathodes for LiÀ S batteries. [8][9][10][11][12][13][14][15] In particular, sulfur/carbon co-polymers, usually synthesized through an inverse vulcanization process, have recently attracted much attention. [9,16] As sulfur cathode materials, they are not only able to withstand the volumetric expansion of the cathode during discharge, thanks to their structural flexibility, but they also have demonstrated a promising performance in improving the cycle life of LiÀ S batteries.…”

Section: Introductionmentioning

confidence: 99%

On the Structure of Sulfur/1,3‐Diisopropenylbenzene Co‐Polymer Cathodes for Li‐S Batteries: Insights from Density‐Functional Theory Calculations

2021

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Sulfur co-polymers have recently drawn considerable attention as alternative cathode materials for lithium-sulfur batteries, thanks to their flexible atomic structure and the ability to provide high reversible capacity. Here, we report on the atomic structure of sulfur/1,3-diisopropenylbenzene co-polymers (poly (S-co-DIB)) based on the insights obtained from density-functional theory calculations. The focus is set on studying the local structural properties, namely the favorable sulfur chain length (S n with n ¼ 1 � � � 8) connecting two DIBs. In order to investigate the effects of the organic groups and sulfur chains separately, we perform series of atomic structure optimizations. We start from simple organic groups connected via sulfur chains and gradually change the structure of the organic groups until we reach a structure in which two DIB molecules are attached via sulfur chains. Additionally, to increase the structural sampling, we perform temperature-assisted minimum-energy structure search on slightly simpler model systems. We find that in DIB-S n -DIB co-polymers, shorter sulfur chains with n � 4 are preferred, where the stabilization is mostly brought about by the sulfur chains rather than the organic groups. The presented results, corresponding to the fully charged state of the cathode in the thermodynamic limit, have direct applications in the field of lithium-sulfur batteries with sulfur-polymer cathodes.

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Section: Introductionmentioning

confidence: 99%

On the Structure of Sulfur/1,3‐Diisopropenylbenzene Co‐Polymer Cathodes for Li‐S Batteries: Insights from Density‐Functional Theory Calculations

2021

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“…[179] In addition, sulfurized poly acrylonitrile (SPAN) is one of the most successful examples of side-chain type DSPs. [181][182][183] SPAN has a single discharge platform, high CE, and high reversible capacity (≈1651 mAh g −1 ). [182,184] The possible reasons for the excellent electrochemical performance were discussed.…”

Section: Disulfide-based Polymersmentioning

confidence: 99%

“…[185] However, the practical application of SPAN is limited by the low sulfur content (≈33-44.7%) and high voltage hysteresis during the initial discharge process. [183,186] Fanous et al [186] reported that the sulfur content of SPAN was affected by the vulcanization temperature. The sulfur content increased from 33% to 41% as the temperature dropped from 550 to 330 °C.…”

Section: Disulfide-based Polymersmentioning

confidence: 99%

Polymer Electrode Materials for Lithium‐Ion Batteries

et al. 2022

Adv Funct Materials

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Polymer electrode materials (PEMs) have become a hot research topic for lithium-ion batteries (LIBs) owing to their high energy density, tunable structure, and flexibility. They are regarded as a category of promising alternatives to conventional inorganic materials because of their abundant and green resources. Currently, conducting polymers, carbonyl polymers, radical polymers, sulfide polymers, and imine polymers as five kinds of PEMs are studied extensively. This review introduces the latest research progress of PEMs for LIBs from the perspectives of molecular structure, redox mechanism, and electrochemical performance. The synthesis mechanisms and methods are outlined to guide the future design of PEMs. However, the practical application of PEMs is limited by their insufficient conductivity, structural instability, and high solubility. Aiming at these obstacles, reasonable optimization strategies are discussed, including the modification of molecular structure, the control of micromorphology, and the composite of carbon materials. Finally, the development trends and prospects of PEMs are put forward.

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“…Recently, Huang et al. [ 89,90 ] proposed another probable molecular structure of S‐cPAN with the coexistence of pyridinic and pyrrolic nitrogen (NPD and NPL) (Figure 5c). They first unraveled the presence of a significant amount of NPL in S‐cPAN, which is different from the predominant NPD in most previous reports.…”

Section: Polymer‐based Cathodesmentioning

confidence: 99%

Polymers in Lithium–Sulfur Batteries

et al. 2021

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Lithium–sulfur batteries (LSBs) hold great promise as one of the next‐generation power supplies for portable electronics and electric vehicles due to their ultrahigh energy density, cost effectiveness, and environmental benignity. However, their practical application has been impeded owing to the electronic insulation of sulfur and its intermediates, serious shuttle effect, large volume variation, and uncontrollable formation of lithium dendrites. Over the past decades, many pioneering strategies have been developed to address these issues via improving electrodes, electrolytes, separators and binders. Remarkably, polymers can be readily applied to all these aspects due to their structural designability, functional versatility, superior chemical stability and processability. Moreover, their lightweight and rich resource characteristics enable the production of LSBs with high‐volume energy density at low cost. Surprisingly, there have been few reviews on development of polymers in LSBs. Herein, breakthroughs and future perspectives of emerging polymers in LSBs are scrutinized. Significant attention is centered on recent implementation of polymers in each component of LSBs with an emphasis on intrinsic mechanisms underlying their specific functions. The review offers a comprehensive overview of state‐of‐the‐art polymers for LSBs, provides in‐depth insights into addressing key challenges, and affords important resources for researchers working on electrochemical energy systems.

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Origin of shuttle-free sulfurized polyacrylonitrile in lithium-sulfur batteries

Cited by 39 publications

References 66 publications

On the Structure of Sulfur/1,3‐Diisopropenylbenzene Co‐Polymer Cathodes for Li‐S Batteries: Insights from Density‐Functional Theory Calculations

On the Structure of Sulfur/1,3‐Diisopropenylbenzene Co‐Polymer Cathodes for Li‐S Batteries: Insights from Density‐Functional Theory Calculations

Polymer Electrode Materials for Lithium‐Ion Batteries

Polymers in Lithium–Sulfur Batteries

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