Semi-Immobilized Molecular Electrocatalysts for High-Performance Lithium–Sulfur Batteries,Journal of the American Chemical Society

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Semi-Immobilized Molecular Electrocatalysts for High-Performance Lithium–Sulfur Batteries
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-11-11 , DOI: 10.1021/jacs.1c09107
Chang-Xin Zhao ₁ , Xi-Yao Li ₁ , Meng Zhao _{2,

3} , Zi-Xian Chen _{2,

3} , Yun-Wei Song ₁ , Wei-Jing Chen ₁ , Jia-Ning Liu ₁ , Bin Wang ₄ , Xue-Qiang Zhang _{2,

3,

5} , Cheng-Meng Chen ₆ , Bo-Quan Li _{2,

3} , Jia-Qi Huang _{2,

3} , Qiang Zhang ₁

Affiliation

Lithium–sulfur (Li–S) batteries constitute promising next-generation energy storage devices due to the ultrahigh theoretical energy density of 2600 Wh kg^–1. However, the multiphase sulfur redox reactions with sophisticated homogeneous and heterogeneous electrochemical processes are sluggish in kinetics, thus requiring targeted and high-efficient electrocatalysts. Herein, a semi-immobilized molecular electrocatalyst is designed to tailor the characters of the sulfur redox reactions in working Li–S batteries. Specifically, porphyrin active sites are covalently grafted onto conductive and flexible polypyrrole linkers on graphene current collectors. The electrocatalyst with the semi-immobilized active sites exhibits homogeneous and heterogeneous functions simultaneously, performing enhanced redox kinetics and a regulated phase transition mode. The efficiency of the semi-immobilizing strategy is further verified in practical Li–S batteries that realize superior rate performances and long lifespan as well as a 343 Wh kg^–1 high-energy-density Li–S pouch cell. This contribution not only proposes an efficient semi-immobilizing electrocatalyst design strategy to promote the Li–S battery performances but also inspires electrocatalyst development facing analogous multiphase electrochemical energy processes.

中文翻译：

用于高性能锂硫电池的半固定化分子电催化剂

锂硫 (Li-S) 电池由于具有 2600 Wh kg ^–1的超高理论能量密度而成为很有前景的下一代储能装置. 然而，具有复杂的均相和非均相电化学过程的多相硫氧化还原反应动力学缓慢，因此需要有针对性的高效电催化剂。在此，设计了一种半固定化分子电催化剂来调整锂硫电池中硫氧化还原反应的特征。具体而言，卟啉活性位点共价接枝到石墨烯集流体上的导电和柔性聚吡咯连接体上。具有半固定化活性位点的电催化剂同时表现出均相和非均相功能，增强氧化还原动力学和调节相变模式。^–1高能量密度锂硫软包电池。这一贡献不仅提出了一种有效的半固定化电催化剂设计策略来提高 Li-S 电池的性能，而且还激发了面临类似多相电化学能量过程的电催化剂的发展。

更新日期：2021-12-01

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