Establishing conclusive proof of ion intercalation/deintercalation is challenging and critical to accurately assessing and optimizing the performance of aqueous aluminum-ion batteries (AAIBs). In this article, we develop oxygen-deficient α-MoO₃ (denoted OD-MoO_3-x) with an ultrahigh rate capability (97 mA h g⁻¹ at 50 A g⁻¹) for AAIBs. The fast kinetics of charge storage are not only due to interlayer expansion but also related to the charge storage mechanism. Through DFT calculations, in situ XRD, in situ Raman spectroscopy, in situ pH monitoring, ex situ TEM and ToF-SIMS, we identify and quantify the contribution of H⁺ intercalation to the total energy storage. The mechanism of the ultrahigh rate capability of OD-MoO_3-x is established as the predominant H⁺ intercalation. Our study may shed some light on the electrode development of high-performance multivalent-ion batteries.

建立离子嵌入/脱嵌的确凿证据对于准确评估和优化水性铝离子电池 (AAIB) 的性能具有挑战性和关键性。在本文中，我们开发了用于 AAIB的具有超高倍率能力（97 mA hg ^-1 at 50 A g ^{-1 ）的缺氧 α-MoO} ₃（表示为 OD-MoO _3-x ） 。电荷存储的快速动力学不仅与层间膨胀有关，还与电荷存储机制有关。通过 DFT 计算、原位 XRD、原位拉曼光谱、原位 pH 监测、非原位 TEM 和 ToF-SIMS，我们识别和量化了 H ⁺插入到总能量存储中。_{OD-MoO 3-x}的超高倍率能力的机制被确立为主要的H ⁺插层。我们的研究可能为高性能多价离子电池的电极开发提供一些启示。