Taeyong Lee, Seonwoo Choi, Seonwoo Choi, Chihyun Hwang, Sanjo Lee, Sun‐Woo Kim, Myung‐Jun Kwak, Ali M. Abou‐Elanwar, Suk Won Yun, Seojun Kim, Hyungmin Park, Youngtai Noh, Timothy van der Laan, Kyu‐Nam Jung, Dawei Su, Sinho Choi, Sinho Choi, Dong Han Seo
ABSTRACT Aqueous zinc‐ion batteries (AZIBs) have attracted considerable attention as a safe and cost‐effective to energy storage system. Cathode materials, which are critical to determining overall AZIB performance, remain a major hurdle to deployment. Currently, substantial energy is required for synthesis, while improvements in capacity and energy density remain necessary to compete with incumbent lithium‐ion batteries. Herein, we report a high‐performance and durable alkali metal (M = K, Na, Li) and water co‐intercalated vanadium oxide (M‐WiVO) cathode synthesized via a rapid (70 min) and energy‐efficient plasma‐assisted hydrothermal (PAHT) process. The M‐WiVO structure consists of water‐intercalated vanadium oxide (V 2 O 5 ·nH 2 O) and monoclinic M x V 2 O 5 phases, which provide expanded channels for rapid Zn 2+ ion transport. Among the M‐WiVO materials, K‐WiVO delivers the highest capacity of 526.7 mAh g −1 at 0.1 A g −1 (≈90% of the theoretical capacity of V 2 O 5 ) and retains 94.5% of its initial capacity after 4000 cycles at 10 A g −1 . Density functional theory (DFT) calculations confirm the stability of the dual‐intercalated framework and the superior performance of K‐WiVO. Overall, the monoclinic M x V 2 O 5 phase provides long‐term electrochemical stabilities; meanwhile, water intercalation in V 2 O 5 provides high capacity and facilitates the Zn 2+ ion transport, where the dual phase works synergistically to preserve the excellent AZIB performances in M‐WiVO.