Novel hybrid organic-inorganic CH3NH3NiCl3 active material for high-capacity and sustainable lithium-ion batteries

Abstract Organic−inorganic hybrid materials have recently been investigated in a variety of applications, including solar cells and batteries. Due to its simple processing, abundant precursors, and high availability of structural space to host lithium atoms, in this work the nickel-based hybrid material CH3NH3NiCl3 (MANiCl3) was assessed for first time for lithium ion battery application. The battery electrodes made with this active material showed a remarkable initial capacity of 650 mAh g−1, with a coulombic efficiency of ca. 100% during cycling, and charge retention of ca. 55% after the 19th cycle at current density of ca 32 mA g−1. A reaction mechanism for the charge/discharge processes of the MANiCl3 active material was also proposed, and we found that three reaction steps occur for this material. The first of these corresponds to the lithium intercalation (Li+ insertion/extraction) inside the MANiCl3 structure; the second is a conversion of the active material into chloride salts; and finally an alloying process occurs between lithium and nickel atoms, leading to intermetallic LixNiy compounds. We suggest that the conversion and alloying processes may be irreversible and are responsible for the capacity decay during cycling.