Ammonium Intercalation Induced Expanded 1T-Rich Molybdenum Diselenides for Improved Lithium Ion Storage

Transition metal dichalcogenides (TMDs), particularly molybdenum diselenides (MoSe2), have the merits of their unique two-dimensional (2D) layered structures, large interlayer spacing (∼0.64 nm), good electrical conductivities, and high theoretical capacities when applied in lithium-ion batteries (LIBs) as anode materials. However, MoSe2 remains suffering from inferior stability as well as unsatisfactory rate capability because of the unavoidable volume expansion and sluggish charge transport during lithiation-delithiation cycles. Herein, we develop a simultaneous reduction-intercalation strategy to synthesize expanded MoSe2 (e-MoSe2) with an interlayer spacing of 0.98 nm and a rich 1T phase (53.7%) by rationally selecting the safe precursors of ethylenediamine (NH2C2H4NH2), selenium dioxide (SeO2), and sodium molybdate (Na2MoO4). It is noteworthy that NH2C2H4NH2 can effectively reduce SeO2 and MoO42- forming MoSe2 nanosheets; in the meantime, the generated ammonium (NH4+) efficiently intercalates between MoSe2 layers, leading to charge transfer, thus stabilizing 1T phases. The obtained e-MoSe2 exhibits high capacities of 778.99 and 611.40 mAh g-1 at 0.2 and 1 C, respectively, together with excellent cycling stability (retaining >90% initial capacity at 0.2 C over 100 charge-discharge cycles). It is believed that the material design strategy proposed in this paper provides a favorable reference for the synthesis of other transition metal selenides with improved electrochemical performance for battery applications.