Investigating the Influence of Diverse Functionalized Carbon Nanotubes as Conductive Fibers on Paper-Based Sulfur Cathodes in Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries are expected to be one of the next generations of high-energy-density battery systems due to their high theoretical energy density of 2600 Wh kg−1. Embracing the trends toward flexibility, lightweight design, and cost-effectiveness, paper-based electrodes offer a promising alternative to traditional coated cathodes in Li–S batteries. Within paper-based electrodes, conductive fibers such as carbon nanotubes (CNTs) play a crucial role. They help to form a three-dimensional network within the paper matrix to ensure structural integrity over extended cycling while mitigating the shuttle effect by confining sulfur within the cathode. Herein, we explore how variously functionalized CNTs, serving as conductive fibers, impact the physical and electrochemical characteristics of paper-based sulfur cathodes in Li–S batteries. Specifically, graphitized hydroxylated carbon nanotubes (G-CNTs) exhibit remarkable capacity at low currents owing to their excellent conductivity and interaction with lithium polysulfide (LiPS), achieving the highest initial specific capacity of 1033 mAh g−1 at 0.25 C (1.1 mA cm−2). Aminated multi-walled carbon nanotubes (NH2-CNTs) demonstrate an enhanced affinity for LiPS due to the -NH2 groups. However, the uneven distribution of these fibers may induce electrode surface passivation during charge–discharge cycles. Notably, hydroxylated multi-walled carbon nanotubes (OH-CNTs) can establish a uniform and stable 3D network with plant fibers, showcasing superior mechanical properties and helping to mitigate Li2S agglomeration while preserving the electrode porosity. The paper-based electrode integrated with OH-CNTs even retains a specific capacity of approximately 800 mAh g−1 at about 1.25 C (5 mA cm−2), demonstrating good sulfur utilization and rate capacity compared to other CNT variants.