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Complex oxide heterointerfaces and heterostructures have demonstrated enormous emergent phenomena over the last decades, attributed to the reconstructions of mis‐matched crystalline structure, polarity, and spin ordering across the heterointerfaces. This work employs the heterostructures of La0.7Sr0.3MnO3 and CaFeO2.5 as model system to demonstrate an interface‐specific oxygen migration/reconstruction across the interfaces due to the mismatched chemical potential, which dramatically influences the ferromagnetic and electronic states of La0.7Sr0.3MnO3 layer. Specifically, the alternative stacking of octahedral (Oh) and tetrahedral (Td) layers in CaFeO2.5 are used to form two distinct heterointerfaces, namely the Oh‐Td and the Oh‐Oh interfaces with the adjacent La0.7Sr0.3MnO3 layer. Interestingly, the oxygen ion migrates toward opposite directions across the interface for these two cases, in which the CaFeO2.5 layer acts as an “oxygen pump” and manipulates the oxygen contents of its adjacent La0.7Sr0.3MnO3 layers. Such manipulation leads to a dramatically changed ferromagnetic transition temperature for the heterostructure with the Oh‐Td and Oh‐Oh interface. This work establishes a feasible and efficient strategy to control the oxygen ionic distribution through atomic‐scale interface design and opens up new opportunities to exploit emergent states at the complex oxide heterostructures through selective oxygen ion evolution. [ABSTRACT FROM AUTHOR]

Benefiting from high safety, low cost, and competitive energy density, aqueous zinc ion batteries (AZIBs) have emerged as very promising technology for grid energy storage. However, the lifetime of AZIBs is severely affected by uncontrolled zinc dendritic growth and undesirable side reaction. To address the problem, natural aluminum silicate hydroxide covered glass fibers separator (AlSi‐GF) is prepared herein using a simple spraying method. Aluminum silicate hydroxide is a complex oxide, where a large number of adsorption sites can adsorb Zn2+ and guide its deposition process. In particular, the Maxwell–Wagner polarization of aluminum silicate hydroxide under an applied electric field contributes to homogenizing the electric field distribution around the interface, thereby modulating zinc deposition and reducing the nucleation overpotential. Impressively, AlSi‐GF separator enables high‐performance zinc‐metal batteries. The symmetric battery with AlSi‐GF separator has a stable voltage polarization and an ultra‐long cycle life of 2280 h at a current density of 1 mA cm−2, and the Zn//V2O5 full cell based on AlSi‐GF separator can exhibit a high specific capacity of 123 mAh g−1 after 1500 cycles at 1 A g−1. This study provides new insights into the design of reliable and cost‐effective separators for metal anodes in energy storage devices. [ABSTRACT FROM AUTHOR]