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Title: Solid-State Lithium/Selenium–Sulfur Chemistry Enabled via a Robust Solid-Electrolyte Interphase

Abstract

Lithium/selenium-sulfur batteries have recently received considerable attention due to their relatively high specific capacities and high electronic conductivity. Different from the traditional encapsulation strategy for suppressing the shuttle effect, an alternative approach to directly bypass polysulfide/polyselenide formation via rational solid-electrolyte interphase (SEI) design is demonstrated here. It is found that the robust SEI layer that in situ forms during charge/discharge via interplay between rational cathode design and optimal electrolytes could enable solid-state (de)lithiation chemistry for selenium-sulfur cathodes. Hence, Se-doped S 22.2Se/Ketjenblack cathodes can attain a high reversible capacity with minimal shuttle effects during long-term and high rate cycling. Moreover, the underlying solid-state (de)lithiation mechanism, as evidenced by in situ 7Li NMR and in operando synchrotron X-ray probes, further extends the optimal sulfur confinement pore size to large mesopores and even macropores that have been long considered as inferior sulfur or selenium host materials, which play a crucial role in developing high volumetric energy density batteries. It is expected that the findings in this study will ignite more efforts to tailor the compositional/structure characteristics of the SEI layers and the related ionic transport across the interface by electrode structure, electrolyte solvent, and electrolyte additive screening.

Authors:
 [1];  [2];  [3];  [4];  [1];  [1];  [5];  [1];  [6];  [6];  [7];  [6];  [6];  [3];  [1]; ORCiD logo [8]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. China Univ. of Petroleum-Beijing (China). State Key Lab. of Heavy Oil Processing. Inst. of New Energy
  3. Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  6. Argonne National Lab. (ANL), Argonne, IL (United States). X-Ray Science Division
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  8. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Stanford Univ., CA (United States). Materials Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1494801
Alternate Identifier(s):
OSTI ID: 1482139; OSTI ID: 1507728; OSTI ID: 1557857
Grant/Contract Number:  
AC02-06CH11357; AC0576RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; (de)lithiation chemistry; cathode; electrolytes; selenium-sulfur; solid-electrolyte interphase

Citation Formats

Xu, Gui-Liang, Sun, Hui, Luo, Chao, Estevez, Luis, Zhuang, Minghao, Gao, Han, Amine, Rachid, Wang, Hao, Zhang, Xiaoyi, Sun, Cheng-Jun, Liu, Yuzi, Ren, Yang, Heald, Steve M., Wang, Chunsheng, Chen, Zonghai, and Amine, Khalil. Solid-State Lithium/Selenium–Sulfur Chemistry Enabled via a Robust Solid-Electrolyte Interphase. United States: N. p., 2018. Web. doi:10.1002/aenm.201802235.
Xu, Gui-Liang, Sun, Hui, Luo, Chao, Estevez, Luis, Zhuang, Minghao, Gao, Han, Amine, Rachid, Wang, Hao, Zhang, Xiaoyi, Sun, Cheng-Jun, Liu, Yuzi, Ren, Yang, Heald, Steve M., Wang, Chunsheng, Chen, Zonghai, & Amine, Khalil. Solid-State Lithium/Selenium–Sulfur Chemistry Enabled via a Robust Solid-Electrolyte Interphase. United States. doi:10.1002/aenm.201802235.
Xu, Gui-Liang, Sun, Hui, Luo, Chao, Estevez, Luis, Zhuang, Minghao, Gao, Han, Amine, Rachid, Wang, Hao, Zhang, Xiaoyi, Sun, Cheng-Jun, Liu, Yuzi, Ren, Yang, Heald, Steve M., Wang, Chunsheng, Chen, Zonghai, and Amine, Khalil. Wed . "Solid-State Lithium/Selenium–Sulfur Chemistry Enabled via a Robust Solid-Electrolyte Interphase". United States. doi:10.1002/aenm.201802235.
@article{osti_1494801,
title = {Solid-State Lithium/Selenium–Sulfur Chemistry Enabled via a Robust Solid-Electrolyte Interphase},
author = {Xu, Gui-Liang and Sun, Hui and Luo, Chao and Estevez, Luis and Zhuang, Minghao and Gao, Han and Amine, Rachid and Wang, Hao and Zhang, Xiaoyi and Sun, Cheng-Jun and Liu, Yuzi and Ren, Yang and Heald, Steve M. and Wang, Chunsheng and Chen, Zonghai and Amine, Khalil},
abstractNote = {Lithium/selenium-sulfur batteries have recently received considerable attention due to their relatively high specific capacities and high electronic conductivity. Different from the traditional encapsulation strategy for suppressing the shuttle effect, an alternative approach to directly bypass polysulfide/polyselenide formation via rational solid-electrolyte interphase (SEI) design is demonstrated here. It is found that the robust SEI layer that in situ forms during charge/discharge via interplay between rational cathode design and optimal electrolytes could enable solid-state (de)lithiation chemistry for selenium-sulfur cathodes. Hence, Se-doped S22.2Se/Ketjenblack cathodes can attain a high reversible capacity with minimal shuttle effects during long-term and high rate cycling. Moreover, the underlying solid-state (de)lithiation mechanism, as evidenced by in situ 7Li NMR and in operando synchrotron X-ray probes, further extends the optimal sulfur confinement pore size to large mesopores and even macropores that have been long considered as inferior sulfur or selenium host materials, which play a crucial role in developing high volumetric energy density batteries. It is expected that the findings in this study will ignite more efforts to tailor the compositional/structure characteristics of the SEI layers and the related ionic transport across the interface by electrode structure, electrolyte solvent, and electrolyte additive screening.},
doi = {10.1002/aenm.201802235},
journal = {Advanced Energy Materials},
number = 2,
volume = 9,
place = {United States},
year = {2018},
month = {11}
}

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