Chae Kyunghee, Kim Youngbi, Oh Yookyeong, Hahn Hosik, Son Jaehyun, Kim Youngsin, Kim Hyuk-Joon, Lee Hyun Jeong, Jang Dohyub, Moon Jooho, Kang Kisuk, Han Jeong Woo, Marques Mota Filipe, Kim Dong Ha
Department of Chemistry and Nanoscience, Ewha Womans University, 52 Ewhayeodae-Gil, Seodaemun-Gu, Seoul, 03760, Republic of Korea.
Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), Pohang, 37673, Republic of Korea.
Nanomicro Lett. 2025 Aug 25;18(1):40. doi: 10.1007/s40820-025-01885-z.
Lithium-oxygen (Li-O) batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage, utilizing ambient air as an energy source, eliminating the need for costly cathode materials, and offering the highest theoretical energy density (~ 3.5 kWh kg) among discussed candidates. Contributing to the poor cycle life of currently reported Li-O cells is singlet oxygen (O) formation, inducing parasitic reactions, degrading key components, and severely deteriorating cell performance. Here, we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets (CoO NSs) as cathode materials to suppress O in Li-O batteries for the first time. Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in O during discharge and charge, respectively, compared to conventional carbon paper-based cells, consistent with differential electrochemical mass spectrometry results, which indicate a near-theoretical charge-to-O ratio (2.04 e/O). Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level, enhancing Co 3d-O 2p hybridization, stabilizing reaction intermediates, and lowering activation barriers for LiO formation and decomposition. These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O batteries, abridging the current gap to commercialization.
锂氧（Li-O）电池被视为可持续电化学储能领域一项有前景的突破，它利用环境空气作为能源，无需使用昂贵的阴极材料，并且在所讨论的候选电池中具有最高的理论能量密度（约3.5 kWh/kg）。单线态氧（O）的形成导致了目前报道的锂氧电池循环寿命较差，它引发寄生反应、降解关键组件并严重恶化电池性能。在此，我们首次利用手性氧化钴纳米片（CoO NSs）的手性诱导自旋选择性效应作为阴极材料来抑制锂氧电池中的O。原位光致发光光谱显示，与传统的基于碳纸电极的电池相比，在放电和充电过程中O分别减少了3.7倍和3.23倍，这与差分电化学质谱结果一致，该结果表明电荷与O的比率接近理论值（2.04 e/O）。密度泛函理论计算表明，手性会导致费米能级附近的峰值发生偏移，增强Co 3d - O 2p杂化，稳定反应中间体，并降低LiO形成和分解的活化能垒。这些发现为提高可持续锂氧电池的稳定性和能量效率建立了一种新策略，缩小了目前与商业化之间的差距。
