Rough Endoplasmic Reticulum Inspired Polystyrene‐Brush‐Based Superhigh Sulfur Content Cathodes Enable Lithium–Sulfur Cells with High Mass and Capacity Loading

Abstract

The development of highly sophisticated biomimetic models is significant yet remains challenging in the electrochemical energy storage field. Lithium–sulfur (Li–S) cells with high sulfur content and high‐sulfur‐loading cathodes are urgently required to meet the fast‐growing demand for electronic devices. Nevertheless, such cathode materials generally suffer from large sulfur agglomeration, nonporous structure, and insufficient conductivity, leading to rapid capacity decay and low sulfur utilization. Herein, inspired by rough endoplasmic reticulum, a 2D polystyrene (PS)‐brush‐based (G‐g‐PS) superhigh‐sulfur‐content (96 wt%) composite(G‐g‐sPS@S) is fabricated via the vulcanization reaction. The vulcanized PS side‐chains and their S8 composites on the nanosheet surface can efficiently provide sulfur species, and the intersheet interstitial pores can provide rapid mass‐transfer channels for redox reactions of sulfur species. Furthermore, the highly sulfophilic vulcanized PS side‐chains are able to effectively inhibit the shuttle effect of polysulfides and regulate their redox process. With these merits, the cells with G‐g‐sPS@S cathodes exhibit an ultralow decay rate of 0.02% per cycle over 400 cycles at 2 C and deliver a superior areal capacity of 12.6 mAh cm−2 even with a high sulfur loading of 10.5 mg cm−2.

A Perspective of Bioinspired Interfaces Applied in Renewable Energy Storage and Conversion Devices

“…For G- g - s PS@S, the vulcanized PS side chains and their S8 composites on the nanosheet surface can efficiently provide sulfur species, and the intersheet interstitial pores can offer rapid mass transfer channels for the redox reactions of sulfur species. Reproduced with permission from ref . Copyright 2023, Wiley-Blackwell.…”

“…Inspired by the membranous morphology of rough endoplasmic reticulum (Figure 2a), a two-dimensional polystyrene-brush-like matrix was designed to boost sulfur content as high as 96% significantly by virtue of the plentiful membranaceous pores existing on cathode/electrolyte interfaces, probably promoting commercialization process of lithium−sulfur batteries. 13 By adjustment of the porous distribution and hierarchical architecture, a chemical environmental responsiveness characteristic can be achieved in the process of mass transfer. For example, a leaf-bioinspired cathode interface was exerted to control anisotropic nanofluidic flux spatially for the electrolytes of potassium-ion batteries (Figure 2b).…”

N‐Doping Induced Lattice Expansion of 1D Template Confined Ultrathin MoS2 Sheets to Significantly Enhance Lithium Polysulfides Redox Kinetics for Li–S Battery

“…Lithium-sulfur batteries (LSBs) owing to inexpensive cost, extraordinary theoretical capacity (1675 mAh g −1 ) and energy density (2600 Wh kg −1 ) are considered to be one of the most favorable energy storage solutions to meet the current energy crisis. [1,2] Unfortunately, despite years of research, many inherent factors of sulfur cathode, such as insulating nature of sulfur and discharge products (Li 2 S/Li 2 S 2 ), severe volume expansion (next to 80%), and the "shuttle effect" remain unsolved, thus resulting in low sulfur utilization, poor rate performance, and cycle life, which severely restrict the largescale application of LSBs. [3][4][5] To deal with the problems, numerous efforts have been devoted to design advanced sulfur hosting cathode such like porous carbon, [6] metal oxides, [7] sulfides, [8] and nitrides.…”

Three-Dimensional Carbon Networks Decorated with Co Nanocatalysts as Multifunctional Interlayers for a High-Performance Lithium–Sulfur Battery

“…For example, the presence of insulating S 8 substance (5 × 10 –30 S m –1 ) and Li 2 S (3 × 10 –7 S m –1 ) leads to low utilization of the active sulfur material and slow sulfur electrochemical reaction kinetics. − The shuttle effect of lithium polysulfide (LiPS) results in the loss of the active material. − In addition, the side reactions between the Li anode and the polysulfide also affect its cyclic stability . These problems seriously undermine the capacity and cycle performance of LSBs, especially at high sulfur loadings and high current rate operations. − …”