Journal
ADVANCED ENERGY MATERIALS
Volume 10, Issue 25, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202000901
Keywords
concentrated electrolytes; lithium metal batteries; siloxanes; solvation-ion-exchange; sulfur
Categories
Funding
- U.S. Department of Energy (DOE), Vehicle Technologies Office
- DOE [DE-AC02-06CH11357]
- National Natural Science Foundation of China [21903001]
- Natural Science Foundation of Anhui Province [1908085QB58]
- University of Jeddah, Saudi Arabia [UJ-07-18-ICP]
- European Commission under the European Union's Horizon 2020 Research and Innovation Programme [GA 759603]
- European Research Council under the European Union's Horizon 2020 Research and Innovation Programme [GA 759603]
- Polish Ministry of Science and Education [3787/E-138/S/2017]
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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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