Lim, Jaehong Chang, Hongjun Jeong, In Young Jeong, Minji Yoo, Yiseul Baeg, Haeun Yim, Taeeun Byun, Dongjin Chung, Kyung Yoon Kim, Hyung-Seok Moon, Janghyuk Oh, Si Hyoung 2026-02-03T08:30:29Z 2026-02-03T08:30:29Z 2026-02-02 2026-01 2050-7488 https://pubs.kist.re.kr/handle/201004/154156 Despite their great promise as a sustainable alternative to lithium-ion batteries for stationary energy storage systems, aqueous zinc-ion batteries (AZIBs) continue to suffer from interfacial instability between metal anodes and electrolytes, stemming from the high activity of free water molecules in the electrolyte. Incorporating chaotropic co-solvents or additives with a strong affinity toward Zn has long been recognized as a viable and cost-effective approach to mitigate these issues, yet such strategies often face intrinsic miscibility limitations. To address this issue, we employed tetrahydrofuran (THF) to rationally design fully miscible electrolytes by balancing kosmotropic and chaotropic interactions between THF and anions in THF–H2O solutions. In these systems, THF not only disrupts the hydrogen-bonding network in water clusters, but also forms robust adsorbate layers on the zinc surface, suppressing Zn metal corrosion and promoting uniform and compact Zn deposition, thereby leading to excellent long-term electrochemical performance. Furthermore, the spontaneous phase separation into THF-rich and sulfate-rich phases, driven by the salting-out effect among THF, triflate and sulfate in aqueous solution, was exploited to prepare biphasic electrolytes capable of providing tailored electrolyte environments for the cathode and anode, respectively, in Zn–I2 batteries. This study offers new insights and opportunities to design advanced electrolytes to tackle longstanding challenges with various AZIBs. English Royal Society of Chemistry Rational design of aqueous zinc-ion battery electrolytes based on intermolecular interactions between co-solvents and anions Article 10.1039/d5ta08096g 1 Journal of Materials Chemistry A, v.14, pp.8052 - 8063 Journal of Materials Chemistry A 14 8052 8063 Y scie scopus 2-s2.0-105028449749 Chemistry, Physical Energy & Fuels Materials Science, Multidisciplinary Chemistry Energy & Fuels Materials Science Article; Early Access BIPHASIC SYSTEMS SALTS