Lithium Bond Chemistry in Lithium–Sulfur Batteries

Ting Zheng Hou, Wen Tao Xu, Xiang Chen, Hong Jie Peng, Jia Qi Huang, Qiang Zhang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

459 Citations (Scopus)

Abstract

The lithium–sulfur (Li–S) battery is a promising high-energy-density storage system. The strong anchoring of intermediates is widely accepted to retard the shuttle of polysulfides in a working battery. However, the understanding of the intrinsic chemistry is still deficient. Inspired by the concept of hydrogen bond, herein we focus on the Li bond chemistry in Li–S batteries through sophisticated quantum chemical calculations, in combination with 7Li nuclear magnetic resonance (NMR) spectroscopy. Identified as Li bond, the strong dipole–dipole interaction between Li polysulfides and Li–S cathode materials originates from the electron-rich donors (e.g., pyridinic nitrogen (pN)), and is enhanced by the inductive and conjugative effect of scaffold materials with π-electrons (e.g., graphene). The chemical shift of Li polysulfides in 7Li NMR spectroscopy, being both theoretically predicted and experimentally verified, is suggested to serve as a quantitative descriptor of Li bond strength. These theoretical insights were further proved by actual electrochemical tests. This work highlights the importance of Li bond chemistry in Li–S cell and provides a deep comprehension, which is helpful to the cathode materials rational design and practical applications of Li–S batteries.

Original languageEnglish
Pages (from-to)8178-8182
Number of pages5
JournalAngewandte Chemie - International Edition
Volume56
Issue number28
DOIs
Publication statusPublished - 3 Jul 2017
Externally publishedYes

Keywords

  • NMR spectroscopy
  • ab initio calculations
  • electrochemistry
  • lithium bond
  • lithium–sulfur batteries

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