Iron-based alkaline rechargeable batteries such as nickel-iron and iron-air batteries are promising candidates for large-scale energy storage applications because of their relatively low cost, inherent robustness to cycling, and eco-friendliness. In the present study, we demonstrate iron electrodes containing iron (II) sulfide and bismuth oxide additives that do not exhibit any noticeable capacity loss even after 1200 cycles at 100% depth of discharge in each cycle. In iron electrodes prepared with bismuth sulfide additive, capacity loss occurred during cycling, accompanied by a decrease in discharge rate capability and rapid passivation. The recovery of capacity by adding sulfide ions to the electrolyte confirmed that the electrode that suffered capacity fade did not have an adequate supply of sulfide ions. We also found that the loss of cycleability was accompanied by the steady accumulation of magnetite and loss of iron sulfides at the iron electrode. The use of sparingly soluble iron (II) sulfide as an electrode additive ensured a sustained and steady supply of sulfide preventing the accumulation of magnetite during cycling. Thus, we have gained understanding of the critical role of sulfide additives in achieving long cycle life in rechargeable alkaline iron electrodes. Inexpensive and efficient methods of storing electrical energy are essential for the successful integration of solar and wind-based electricity generation into the grid. Among the various means to store electrical energy at a large scale, batteries are particularly promising because of their advantages of high energy efficiency, modularity and flexibility to siting.1-4 The state-of-art commercially-available lithium-ion, lead-acid, nickel-metal hydride and vanadium redox flow batteries may be rated by the levelized cost of energy delivered (LCOE). LCOE is calculated as the ratio of the cost (including capital and operating costs) to the total amount of energy delivered by the battery over its useful lifetime. The LCOE for commercially-available batteries is at least five to ten times higher than the DoE targets of $0.10 to $0.20/kWh. 5,6 Also, since energy storage will be required at the scale of thousands of gigawatt-hours, we are faced with the challenge of providing a sustainable solution, as the global material reserves are quite limited for these state-of-art batteries.7 Therefore, the development of inexpensive, efficient, robust and sustainable battery systems for grid-scale energy storage is a topic of intense research.3-6 Under an effort funded by ARPA-E, we have been focusing on developing such batteries. 7,[8][9][10][11][12] Iron-based battery systems such as nickel-iron and iron-air batteries are based on raw materials that are relatively inexpensive, globally-abundant, and eco-friendly. The promise of iron-based batteries for large-scale energy storage has spurred renewed interest in their development. 11,[13][14][15][16] The development of iron-based alkaline batteries began several decades ago. [17][18][19][20][21][22] In the U...