Birch reduction of aromatic systems by solvated electrons in alkali metal-ammonia solutions is widely recognized as a key reaction that functionalizes highly stable π-conjugated organic systems. In spite of recent advances in Birch reduction with regard to reducing agent and reaction conditions, there remains an ongoing challenge to develop a simple and efficient Birch reaction under mild conditions. Here, we demonstrate that the inorganic electride [Ca 2 N] +• e − promotes the Birch reduction of polycyclic aromatic hydrocarbons (PAHs) and naphthalene under alcoholic solvent in the vicinity of room temperature as a solid-type analogy to solvated electrons in alkali metal ammonia solutions. The anionic electrons from electride [Ca 2 N] +• e − are transferred to PAHs and naphthalene via alcoholysis in a polar cosolvent medium. It is noteworthy that a high conversion yield to the hydrogenated products is ascribed to the extremely high electron transfer efficiency of 98%. This simple protocol utilizing an inorganic electride offers a direct and practical strategy for the reduction of aromatic compounds and provides an outstanding reducing agent for synthetic chemistry.

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Magnetism of pure electrons is fundamental for understanding diverse magnetic phenomena in condensed matters but has not been fully investigated in experiments due to the lack of a tractable model system. Such an exotic material necessitates an exclusive magnetic interaction of electrons being devoid of orbital and lattice degrees of freedom. Here, we report the two-dimensional mixed-cation [YGdC]2+∙2e− electride, showing ferrimagnetic nature from the direct exchange interaction of magnetic interstitial electrons in interlayer space. We identify that magnetic interstitial electrons are periodically localized in octahedral and tetrahedral cavities between 2D cationic Y2−xGdx arrays. The mixed configuration of non-magnetic and magnetic cations in cavities induces divergent spin states and interactions of magnetic interstitial electrons, in which their direct exchange interaction overwhelms the interactions with magnetic cations, triggering the ferrimagnetic spin-alignment. This discovery facilitates further exploration of magnetic electrides and nurtures the study of two-dimensional magnetism of layered crystals and electron phases.

Layer‐structured materials are of central importance in a wide range of research fields owing to their unique properties originating from their two dimensionality and anisotropy. Herein, quasi‐2D layer‐structured IMnV (I: alkali metals and V: pnictogen elements) compounds are investigated, which are potential antiferromagnetic (AFM) semiconductors. Single crystals of IMnV compounds are successfully grown using the self‐flux method and their electronic and magnetic properties are analyzed in correlation with structural parameters. Combined with theoretical calculations, the structural analysis indicates that the variation in the bonding angle between VMnV is responsible for the change in the orbital hybridization of Mn and V, predominantly affecting their anisotropic semiconducting properties. Anisotropy in the magnetic properties is also found, where AFM ordering is expected to occur in the in‐plane direction, as supported by spin–structure calculations. Furthermore, a possible ferromagnetic (FM) transition is discussed in relation to the vacancy defects. This study provides a candidate material group for AFM and FM spintronics and a basis for exploring magnetic semiconductors in quasi‐2D layer‐structured systems.