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Title: Ferrocene-Promoted Long-Cycle Lithium-Sulfur Batteries

Abstract

Confining lithium polysulfide intermediates is one of the most effective ways to alleviate the capacity fade of sulfur-cathode materials in lithium–sulfur (Li–S) batteries. To develop long-cycle Li–S batteries, there is an urgent need for material structures with effective polysulfide binding capability and well-defined surface sites; thereby improving cycling stability and allowing study of molecular-level interactions. This challenge was addressed by introducing an organometallic molecular compound, ferrocene, as a new polysulfide-confining agent. With ferrocene molecules covalently anchored on graphene oxide, sulfur electrode materials with capacity decay as low as 0.014 % per cycle were realized, among the best of cycling stabilities reported to date. With combined spectroscopic studies and theoretical calculations, it was determined that effective polysulfide binding originates from favorable cation–π interactions between Li+ of lithium polysulfides and the negatively charged cyclopentadienyl ligands of ferrocene.

Authors:
 [1];  [2];  [2];  [2];  [3];  [2];  [2];  [2];  [2];  [2];  [4];  [2]
  1. Yale Univ., New Haven, CT (United States); Peking Univ., Beijing (China)
  2. Yale Univ., New Haven, CT (United States)
  3. School of Chemistry and Chemical Engineering; Southeast University; Nanjing Jiangsu 211189 China
  4. Peking Univ., Beijing (China)
Publication Date:
Research Org.:
Yale Univ., New Haven, CT (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1533089
Grant/Contract Number:  
FG02-07ER15909
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 47; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Chemistry; ferrocene; graphene oxide; lithium polysulfides; lithium–sulfur batteries; long-cycle batteries

Citation Formats

Mi, Yingying, Liu, Wen, Yang, Ke R., Jiang, Jianbing, Fan, Qi, Weng, Zhe, Zhong, Yiren, Wu, Zishan, Brudvig, Gary W., Batista, Victor S., Zhou, Henghui, and Wang, Hailiang. Ferrocene-Promoted Long-Cycle Lithium-Sulfur Batteries. United States: N. p., 2016. Web. doi:10.1002/anie.201609147.
Mi, Yingying, Liu, Wen, Yang, Ke R., Jiang, Jianbing, Fan, Qi, Weng, Zhe, Zhong, Yiren, Wu, Zishan, Brudvig, Gary W., Batista, Victor S., Zhou, Henghui, & Wang, Hailiang. Ferrocene-Promoted Long-Cycle Lithium-Sulfur Batteries. United States. https://doi.org/10.1002/anie.201609147
Mi, Yingying, Liu, Wen, Yang, Ke R., Jiang, Jianbing, Fan, Qi, Weng, Zhe, Zhong, Yiren, Wu, Zishan, Brudvig, Gary W., Batista, Victor S., Zhou, Henghui, and Wang, Hailiang. Tue . "Ferrocene-Promoted Long-Cycle Lithium-Sulfur Batteries". United States. https://doi.org/10.1002/anie.201609147. https://www.osti.gov/servlets/purl/1533089.
@article{osti_1533089,
title = {Ferrocene-Promoted Long-Cycle Lithium-Sulfur Batteries},
author = {Mi, Yingying and Liu, Wen and Yang, Ke R. and Jiang, Jianbing and Fan, Qi and Weng, Zhe and Zhong, Yiren and Wu, Zishan and Brudvig, Gary W. and Batista, Victor S. and Zhou, Henghui and Wang, Hailiang},
abstractNote = {Confining lithium polysulfide intermediates is one of the most effective ways to alleviate the capacity fade of sulfur-cathode materials in lithium–sulfur (Li–S) batteries. To develop long-cycle Li–S batteries, there is an urgent need for material structures with effective polysulfide binding capability and well-defined surface sites; thereby improving cycling stability and allowing study of molecular-level interactions. This challenge was addressed by introducing an organometallic molecular compound, ferrocene, as a new polysulfide-confining agent. With ferrocene molecules covalently anchored on graphene oxide, sulfur electrode materials with capacity decay as low as 0.014 % per cycle were realized, among the best of cycling stabilities reported to date. With combined spectroscopic studies and theoretical calculations, it was determined that effective polysulfide binding originates from favorable cation–π interactions between Li+ of lithium polysulfides and the negatively charged cyclopentadienyl ligands of ferrocene.},
doi = {10.1002/anie.201609147},
journal = {Angewandte Chemie (International Edition)},
number = 47,
volume = 55,
place = {United States},
year = {Tue Oct 25 00:00:00 EDT 2016},
month = {Tue Oct 25 00:00:00 EDT 2016}
}

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