Unleashing the potential of sulfur-incorporated polymer framework composite for enhanced performance and stability of lithium-organosulfur batteries

Sulfur-containing polymer have emerged as a promising cathode material due to their high theoretical capacity, energy density and low cost. However, their commercial development is hindered by the shuttle effect and slow lithium-ion transport efficiency. Here, a novel sulfur-containing polymer framework material (1,4-NDC@S@PAA) was synthesized by using a solid-phase reaction method. The carbon skeleton of polyacrylic acid (PAA) is functionalized with both 1,4-naphthalenedicarboxylic acid (1,4-NDC) and sulfur molecular clusters. By incorporating small molecules into the carbon skeleton, the lithium-ion transport channels within the electrode material are increased, resulting in improved performance. Compared to traditional vulcanized sulfur chain-type polymers, employing PAA as the main chain enhances stability during charge/discharge process. After 500 cycles at 1.0 C, the material demonstrates a modest average decay rate of 0.091% per cycle. Additionally, the introduction of 1,4-NDC constructs a molecular framework that facilitates rapid Li ⁺ ions diffusion, leading to a two-order of magnitude increase of Li ⁺ ions diffusion coefficient as high as 3.58×10 ⁻⁸ cm ² s ⁻¹ and excellent rate performance with a 721 mAh g ⁻¹ specific capacity at 5.0 C. This high-performance sulfur-containing polymer framework material holds great promise for advancing lithium-sulfur battery technology and addressing the limitations faced by traditional lithium-ion batteries.