An all-biomaterials-based aqueous binder based on adsorption redox-mediated synergism for advanced lithium–sulfur batteries

• Published in: eScience (Beijing) 2024-06, Vol.4 (3), p.100203, Article 100203
• Main Authors: Jiang, Wanyuan, Zhang, Tianpeng, Mao, Runyue, Song, Zihui, Liu, Siyang, Song, Ce, Jian, Xigao, Hu, Fangyuan
• Format: Article
• Language: English
• Subjects: Adsorption redox-mediated synergism; Aqueous binder; Biomaterials; Hydrogen bonding; Li–S batteries
• ISSN: 2667-1417; 2667-1417
• DOI: 10.1016/j.esci.2023.100203

The complex multistep electrochemical reactions of lithium polysulfides and the solid–liquid–solid phase transformation involved in the S8 to Li2S reactions lead to slow redox kinetics in lithium–sulfur batteries (Li–S batteries). However, some targeted researches have proposed strategies requiring the introduction of significant additional inactive components, which can seriously affect the energy density. Whereas polymer binders, proven to be effective in suppressing shuttle effects and constraining electrode volume expansion, also have promising potential in enhancing Li–S batteries redox kinetics. Herein, a novel aqueous polymer binder is prepared by convenient amidation reaction of fully biomaterials, utilizing its inherent rich amide groups for chemisorption and redox mediating ability of thiol groups to achieve adsorption redox-mediated synergism for efficient conversion of polysulfides. Li–S batteries based on N-Acetyl-L-Cysteine-Chitosan (NACCTS) binder exhibit high initial discharge specific capacity (1260.1 ​mAh ​g−1 at 0.2 ​C) and excellent cycling performance over 400 cycles (capacity decay rate of 0.018% per cycle). In addition, the batteries exhibit great areal capacity and stable capacity retention of 83.6% over 80 cycles even under high sulfur loading of 8.4 ​mg ​cm−2. This work offers a novel perspective on the redox-mediated functional design and provides an environmentally friendly biomaterials-based aqueous binder for practical Li–S battery. [Display omitted] •An environmentally friendly aqueous polymer binder was prepared via fully biobased materials with low energy consumption.•The unique adsorption redox-mediated synergism of N-Acetyl-L-Cysteine-Chitosan confers significantly enhanced electrochemical reaction kinetics to lithium–sulfur batteries.•Abundant hydrogen bonding and modulation of Li2S deposition mode provide superior cathode structural stability.•A high initial capacity of 1298.2 ​mAh ​g−1 at 0.1 ​C and an ultra-low capacity decay rate of 0.018% per cycle over 400 cycles at 2 ​C.