journal article·2020-07Open access

Regulating the Hidden Solvation‐Ion‐Exchange in Concentrated Electrolytes for Stable and Safe Lithium Metal Batteries

Rachid Amine, Jianzhao Liu, Ilona Acznik, Tian Sheng, Katarzyna Lota, Hui Sun, Cheng‐Jun Sun, Krzysztof Fic, Xiaobing Zuo, Yang Ren, Deia Abd EI‐Hady, Wael Alshitari, Abdullah S. Al‐Bogami, Zonghai Chen, Khalil Amine, Gui‐Liang Xu

Advanced Energy Materials· Volume 10· Issue 25

Abstract

Abstract Lithium–sulfur batteries are attractive for automobile and grid applications due to their high theoretical energy density and the abundance of sulfur. Despite the significant progress in cathode development, lithium metal degradation and the polysulfide shuttle remain two critical challenges in the practical application of Li–S batteries. Development of advanced electrolytes has become a promising strategy to simultaneously suppress lithium dendrite formation and prevent polysulfide dissolution. Here, a new class of concentrated siloxane‐based electrolytes, demonstrating significantly improved performance over the widely investigated ether‐based electrolytes are reported in terms of stabilizing the sulfur cathode and Li metal anode as well as minimizing flammability. Through a combination of experimental and computational investigation, it is found that siloxane solvents can effectively regulate a hidden solvation‐ion‐exchange process in the concentrated electrolytes that results from the interactions between cations/anions (e.g., Li+, TFSI−, and S2−) and solvents. As a result, it could invoke a quasi‐solid‐solid lithiation and enable reversible Li plating/stripping and robust solid‐electrolyte interphase chemistries. The solvation‐ion‐exchange process in the concentrated electrolytes is a key factor in understanding and designing electrolytes for other high‐energy lithium metal batteries.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemical Engineering University of Illinois at Chicago Chicago IL 60607 USA

Materials Science Division Argonne National Laboratory Lemont IL 60439 USA

Chemical Sciences and Engineering Division Argonne National Laboratory 9700 S Cass Avenue Lemont IL 60439 USA

Department of Chemistry Virginia Tech 900 West Campus Drive Blacksburg VA 24061 USA

Institute of Non‐Ferrous Metals Division in Poznan Central Laboratory of Batteries and Cells Forteczna 12 Poznan 61‐362 Poland

College of Chemistry and Materials Science Anhui Normal University Wuhu 241000 P. R. China

State Key Laboratory of Heavy Oil Processing Institute of New Energy China University of Petroleum‐Beijing Beijing 102249 P. R. China

X‐ray Science Division Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA

Poznan University of Technology Pl. Marii Sklodowskiej‐Curie 5 Poznan 60‐965 Poland

Department of Chemistry College of Science University of Jeddah P.O. 80327 Jeddah 21589 Saudi Arabia

Materials Science and Engineering Stanford University Stanford CA 94305 USA

IRMC Imam Abdulrahman Bin Faisal University (IAU) Dammam 34212 Saudi Arabia

Funding

U.S. Department of Energy · Vehicle Technologies Office · Argonne National Laboratory · National Natural Science Foundation of China · Natural Science Foundation of Anhui Province · European Research Council

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