Lee, Yun-Jeong Lee, Yurim Kim, So Hee Bae, Jong-Seong Kim, Ki-Hyun Lee, Do-Joong Lee, Chang Hoon Yu, Seung-Ho 2025-09-22T04:30:08Z 2025-09-22T04:30:08Z 2025-09-16 2025-11 https://pubs.kist.re.kr/handle/201004/153209 Lithium–sulfur (Li–S) batteries are promising candidates for next-generation energy storage systems, but practical use is limited by polysulfide (PS) shuttling and Li metal anode instability. Lithium nitrate (LiNO3) is widely used to mitigate these issues; however, its interfacial effects across the anode, electrolyte, and cathode during operation are not fully understood. Here, operando optical microscopy with a custom side-by-side cell enables simultaneous monitoring of the Li anode, liquid electrolyte, and sulfur cathode in a single field of view under conditions with and without LiNO3. In the absence of LiNO3, the Li surface undergoes rough stripping and fragmented, non-coalescent deposition, accompanied by PS-induced corrosion and accumulation of parasitic byproducts at the anode-electrolyte interface. Redness Intensity (RI), introduced to quantify electrolyte-phase PS dynamics, indicates sustained transport toward the anode and delayed conversion to elemental sulfur. By contrast, LiNO3 induces uniform Li stripping and the growth of aggregated, interconnected deposits, while mitigating PS crossover and promoting efficient sulfur crystallization at the cathode. Complementary SEM-EDS, UV–vis, XPS, TXM, and CT analyses corroborate these observations. By elucidating the multifunctional role of LiNO3, this study clarifies the interfacial dynamics that govern Li–S battery performance. English Wiley Comprehensive elucidation of the multifunctional role of lithium nitrate in lithium–sulfur batteries: Expanding beyond shuttle suppression Article 10.1002/inf2.70071 1 InfoMat, v.7, no.11 InfoMat 7 11 Y scie scopus 001565249400001 Materials Science, Multidisciplinary Materials Science Article LI-S BATTERY SOLID-ELECTROLYTE INTERPHASE SELF-DISCHARGE BEHAVIOR CYCLING PERFORMANCES LINO3 ANODE POLYSULFIDES MECHANISM EVOLUTION PRODUCTS electrolyte additives lithium nitrate lithium-sulfur batteries operando optical imaging