Details

Autor(en) / Beteiligte

• Feng, Shuai
• Fu, Zhong‐Heng
• Chen, Xiang
• Li, Bo‐Quan
• Peng, Hong‐Jie
• Yao, Nan
• Shen, Xin
• Yu, Legeng
• Gao, Yu‐Chen
• Zhang, Rui
• Zhang, Qiang

Titel

An Electrocatalytic Model of the Sulfur Reduction Reaction in Lithium–Sulfur Batteries

Ist Teil von

• Angewandte Chemie International Edition, 2022-12, Vol.61 (52), p.e202211448-n/a

Auflage

International ed. in English

Ort / Verlag

Germany: Wiley Subscription Services, Inc

Erscheinungsjahr

2022

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Lithium–sulfur (Li–S) battery is strongly considered as one of the most promising energy storage systems due to its high theoretical energy density and low cost. However, the sluggish reduction kinetics from Li2S4 to Li2S during discharge hinders the practical application of Li–S batteries. Although various electrocatalysts have been proposed to improve the reaction kinetics, the electrocatalytic mechanism is unclear due to the complexity of sulfur reduction reactions (SRR). It is crucial to understand the electrocatalytic mechanism thoroughly for designing advanced electrocatalysts. Herein an electrocatalytic model is constructed to reveal the chemical mechanism of the SRR in Li–S batteries based on systematical density functional theory calculations, taking heteroatoms‐doped carbon materials as an example. The adsorption energy of LiSy⋅ (y=1, 2, or 3) radicals is used as a key descriptor to predict the reaction pathway, rate‐determining step, and overpotential. A diagram for designing advanced electrocatalysts is accordingly constructed. This work establishes a theoretical model, which is an intelligent integration for probing the complicated SRR mechanisms and designing advanced electrocatalysts for high‐performance Li–S batteries. An electrocatalytic model is proposed to probe the sulfur reduction reaction pathway in working lithium–sulfur batteries by considering the adsorption free energy of LiS⋅, LiS2⋅, and LiS3⋅ radicals as descriptors. With an overall consideration of ΔG(LiS3⋅*), ΔG(LiS2⋅*), and ΔG(LiS⋅*) descriptors, a regional diagram model is constructed to visualize the overpotential and rate‐determining step.