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Vol. 16 (2024)

Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in Li–S Batteries

https://doi.org/10.1007/s40820-023-01319-8
Yu Du
Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Weijie Chen
Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Yu Wang
Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Yue Yu
Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Kai Guo
Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Gan Qu
Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, People’s Republic of China
Jianan Zhang
Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City, College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, People’s Republic of China

Corresponding Author: Jianan Zhang

zjn@zzu.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 100

Abstract

Spin-engineering with electrocatalysts have been exploited to suppress the “shuttle effect” in Li–S batteries. Spin selection, spin-dependent electron mobility and spin potentials in activation barriers can be optimized as quantum spin exchange interactions leading to a significant reduction of the electronic repulsions in the orbitals of catalysts. Herein, we anchor the MgPc molecules on fluorinated carbon nanotubes (MgPc@FCNT), which exhibits the single active Mg sites with axial displacement. According to the density functional theory calculations, the electronic spin polarization in MgPc@FCNT not only increases the adsorption energy toward LiPSs intermediates but also facilitates the tunneling process of electron in Li–S batteries. As a result, the MgPc@FCNT provides an initial capacity of 6.1 mAh cm−2 even when the high sulfur loading is 4.5 mg cm−2, and still maintains 5.1 mAh cm−2 after 100 cycles. This work provides a new perspective to extend the main group single-atom catalysts enabling high-performance Li–S batteries.


Highlights:
1 Compared with the traditional single-atom catalysts (SACs), the Mg SACs with axial displacement is accurately fabricated on the functional carbon nanotubes.
2 The electronic spin polarization modulates the spin density of MgPc, facilitating the LiPSs conversion kinetics in Li-S batteries.
3 The MgPc@FCNT achieves ultra-low capacity decay rate under the high sulfur loading.

Keywords

Metal phthalocyanines Spin polarization Electrocatalysis Li–S batteries
Du, Yu, Weijie Chen, Yu Wang, Yue Yu, Kai Guo, Gan Qu, and Jianan Zhang. 2024. “Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in Li–S Batteries”. Nano-Micro Letters 16 (January):100. https://doi.org/10.1007/s40820-023-01319-8.
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