Journal
ACS APPLIED MATERIALS & INTERFACES
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c07932
Keywords
carbonate electrolyte; lithium metal; electrolyte decomposition; lithium metal batteries; azamacrocyclic ligand; lithium nitrate
Funding
- National Research Foundation of Korea (NRF) - Korean government (MEST) [NRF-2018M1A2A2063353, 2022M3J1A1085408]
- National Research Foundation of Korea [2022M3J1A1085408] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Introducing a lithium-chelating azamacrocyclic ligand into a carbonate-based electrolyte improves the reversible cycleability of lithium metal negative electrodes. The ligand facilitates reversible lithium plating and stripping on copper electrodes through its dual functionality, acting as a cationic shielding molecule for smooth lithium deposition and strengthening the interphasial characteristics of the lithium metal negative electrode with a Li3N-based solid electrolyte interphase film.
To promote the reversible cycleability of Li metal negative electrodes, a Li-chelating azamacrocyclic ligand molecule is introduced into a carbonate-based electrolyte intended for lithium metal batteries. Reversible Li plating and stripping on the Cu electrode are found to be the outcomes of the bifunctional effects of adding the lithium nitrate-chelating azamacrocyclic ligand. The negatively shifted redox potential of the Li-chelating macrocyclic ligand, relative to that of the free Li-ion, acted as a cationic shielding molecule for smooth Li deposition, and the Li3N-based solid electrolyte interphase (SEI) film derived from the nitrate anion strengthened the interphasial characteristics of the Li metal negative electrode. Cationic shielding and Li3N-based SEI composition could help enhance the cycleability of the Li metal in a cascading manner. Consequently, the physicochemical characteristics of the lithium nitrate-chelated 1,4,8,11-tetramethyl-1,4,8,11-tetraazacylcotetradecane molecule exhibit stable Li/LiNi0.8Co0.1Mn0.1O2 cycleability.
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