La 2 (Ni 1-x Co x ) 7 (x = 0.05, 0.1, 0.2) alloys were synthesized directly from sintered mixture of La 2 O 3 + NiO + CoO in the molten CaCl 2 electrolyte by the electro-deoxidation method at 850 • C and the electrochemical hydrogen storage characteristics of the synthesized alloys were observed. Sintering (at 1200 • C for 3 h) converted the hygroscopic La 2 O 3 (by the reaction with NiO) into the non-hygroscopic LaNiO 3 , La 3 Ni 2 O 6.5 and La 4 Ni 3 O 9 depending on the Co content of the oxide mixture. The X-ray diffraction peaks indicated that La 2 NiO 4 was the main La-Ni-O phase formed as a result of partial reduction or dissociation reaction to initiate the LaNi 5 phase formation. The target La 2 Ni 7 phase formed much later than LaNi 5 phase probably due to the sluggish reduction of LaOCl. It was observed that La 2 (Ni 1-x Co x ) 7 (x = 0.05, 0.1, 0.2) alloys had promising discharge capacities changed between 227 mA h g −1 (La 2 (Ni 0.95 Co 0.05 ) 7 ) and 332 mA h g −1 (La 2 (Ni 0.8 Co 0.2 ) 7 ) depending on the alloy Co content. This work clearly indicated that the electro-deoxidation was very effective method in the synthesis of the hydrogen storage materials.The extensive developments in the portable electronic devices and the requirement for the environmental friendly transportation industry withdraw the attention of many researchers on the nickel metal hydride batteries. 1-3 The big portion of the works is conducted on the development of the high performance electrode alloy with the proper synthesis methods for these secondary batteries. 4-9 Recently a novel technique called electro-deoxidation, which is also known as Fray-Farthing-Chen (FFC) Cambridge process, 10,11 is reported as very promising for the economical synthesis of the hydrogen storage alloys. [12][13][14] One of the well-known commercial alloy groups for the nickel metal hydride batteries is lanthanum-nickel based alloys and they are generally synthesized by the melting and casting under the protective atmosphere. [15][16][17][18][19] Of course the individual elements (La, Ni and other additive elements) must be already extracted and refined for the melting and casting processes. The cast products need annealing for several hours to get the structural homogeneity. 20 Obviously this production pathway for the La-Ni based hydrogen storage alloys is not very encouraging especially for the large scale applications like battery systems of the electrical vehicles. The electro-deoxidation method looks more cost-effective since it provides direct synthesis of the alloy with the final stoichiometry from the raw materials (oxides). 21 In this work, as the continuation of our previous work, 22 La 2 (Ni 1-x Co x ) 7 (x = 0.05, 0.1, 0.2) hydrogen storage alloy was synthesized by the molten salt electro-deoxidation method for the first time in the literature. In our previous work we presented the alloy development stages of La 2 Ni 7 during electro-deoxidation. 22 In this work part of Ni was replaced by Co systematically and then the alloy developmen...