Citation: Yan Wang, Huixin Chen, Fuda Yu, Shanyue Wei, Jinhui Song, Qianfeng He, Yiming Xie, Miaoliang Huang, Canzhong Lu. Oxygen self-doping pyrolyzed polyacrylic acid as sulfur host with physical/chemical adsorption dual function for lithium-sulfur batteries[J]. Chinese Chemical Letters, ;2024, 35(7): 109001. doi: 10.1016/j.cclet.2023.109001 shu

Oxygen self-doping pyrolyzed polyacrylic acid as sulfur host with physical/chemical adsorption dual function for lithium-sulfur batteries

Yan Wang ^{a, c, 1} ,
Huixin Chen ^{b, c, 1} ,
Fuda Yu ^a ,
Shanyue Wei ^{a, c} ,
Jinhui Song ^c ,
Qianfeng He ^c ,
Yiming Xie ^{a, *,} ,
Miaoliang Huang ^{a, *,} ,
Canzhong Lu ^{b, c, *,}

a.
Engineering Research Center of Environment-Friendly Functional Materials, Ministry of Education, Institute of Materials Physical Chemistry, Huaqiao University, Xiamen 361021, China
b.
CAS Key Laboratory of Design and Assembly of Functional Nanostructures, and Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
c.
Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare Earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen 361021, China

ymxie@hqu.edu.cn

huangml@hqu.edu.cn

czlu@fjirsm.ac.cn

Received Date: 27 June 2023
Revised Date: 9 August 2023
Accepted Date: 28 August 2023
Available Online: 1 September 2023

Figures(5)

Lithium-sulfur (Li-S) batteries with high theoretical capacity and energy density need to solve problems such as the high decomposition energy barrier of Li₂S and large volume change of sulfur in the charging process caused by the shuttle effect before practical application. Herein, a green synthesis method is used to prepare polyacrylic acid (PAA) superabsorbent material, and then the pyrolyzed PAA (P/PAA) material is obtained as the positive electrode of Li-S battery. Density functional calculation reveals that the oxygen self-doping pyrolyzed polyacrylic acid (P/PAA) delivered stronger binding energy toward Li₂S species in carbonyl C=O than that of graphite powder (GP) which are −1.58 eV and −1.02 eV, respectively. Coupled with the distribution of relaxation time analysis and the in-situ electrochemical impedance approach, it is further demonstrated that the designed P/PAA as sulfur host plays a physical/chemical adsorption dual function in maintaining the stability and rate performance of batteries. With an initial discharge capacity of 1258 mAh/g at 0.1 C and a minimal capacity decline of 0.05% per cycle even after 800 cycles at 0.5 C, the produced cathode demonstrated outstanding electrochemical performance. The average Coulombic efficiency is nearly 100%. The P/PAA electrodes may typically retain 96% of their capacity while declining on average only 0.033% per cycle after 130 cycles at 3 C. This effort provides a new method for the future development of heteroatomic self-doping superabsorbent with promising adsorption properties for polysulfides as cathode materials of Li-S batteries.
- Polyacrylic acid,
- Oxygen self-doping,
- Green synthetic,
- Pore mesh polymer cathodes,
- Lithium-sulfur batteries
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