Energy storage technologies are essential to overcome the temporal variability in renewable energy. The primary aim of this thesis is to develop reactor solutions to better analyze the potential of thermochemical energy storage (TCES) using non-stoichiometric metal oxides, for the multi-day energy storage application. A TCES system consists of a reduction reactor and an insulated MOx storage bin. The reduction reactor heats (to ~ 1100 °C) and partially reduces the MOx, thereby adding sensible and chemical energy (i.e., charging it) under reduced pO2 environments (~10 Pa). Inert gas removes the oxygen generated during reduction. The storage bin holds the hot and partially reduced MOx (typically particles) until it is used in an energy recovery device (i.e., discharge). Irrespective of the reactor heat source (here electrical), or the particle-inert gas flows (here countercurrent), the thermal reduction temperature and inert gas (here N2) flow minimize when the process approaches reversibility, i.e., operates near equilibrium. This study specifically focuses on developing a reduction reactor based on the theoretical considerations for approaching reversibility along the reaction path. The proposed Zigzag flow reactor (ZFR) is capable of thermally reducing CAM28 particles at temperatures ~ 1000 °C under an O2 partial pressure ~ 10 Pa. The associated analytical and numerical models analyze the reaction equilibrium under a real (discrete) reaction path and the mass transfer kinetic conditions necessary to approach equilibrium. The discrete equilibrium model minimizes the exergy destroyed in a practical reactor and identifies methods of maximizing the energy storage density () and the exergetic efficiency. The mass transfer model analyzes the O2 N2 concentration boundary layers to recommend sizing considerations to maximize the reactor power density. Two functional ZFR prototypes, the -ZFR and the -ZFR, establish the proof of concept and achieved a reduction extent, Δδ = 0.071 with CAM28 at T~950 °C and pO2 = 10 Pa, 7x higher than a previous attempt in the literature. The -ZFR consistently achieved  > 100 Wh/kg during >10 h. runtime and the -ZFR displayed an improved  = 130 Wh/kg during >5 h. operation with CAM28. A techno-economic model of a grid-scale ZFR with an associated storage bin analyzes the cost of scaling the ZFR for grid energy storage requirements. The scaled ZFR capital costs contribute < 1% to the levelized cost of thermochemical energy storage, which ranges from 5-20 ¢/kWh depending on the storage temperature and storage duration.