Controlled synthesis of series NixCo3-xO4 products: Morphological evolution towards quasi-single-crystal structure for high-performance and stable lithium-ion batteries

Transition metal oxides are very promising alternative anode materials for high-performance lithium-ion batteries (LIBs). However, their conversion reactions and concomitant volume expansion cause the pulverization, leading to poor cycling stability, which limit their applications. Here, we present the quasi-single-crystal NixCo3-xO4 hexagonal microtube (QNHM) composed of continuously twinned single crystal submicron-cubes as anode materials for LIBs with high energy density and long cycle life. At the current density of 0.8 A g(-1), it can deliver a high discharge capacities of 1470 mAh g(-1) over 100 cycles (105% of the 2nd cycle) and 590 mAh g(-1) even after 1000 cycles. To better understand what underlying factors lead our QNHMs to achieve excellent electrochemical performance, a series of NixCo3-xO4 products with systematic shape evolution from spherical to polyhedral, and cubic particles as well as circular microtubes consisted of spheres and square microtubes composed of polyhedra have been synthesized. The excellent electrochemical performance of QNHMs is attributed to the unique stable quasi-single-crystal structure, which can both provide efficient electrical transport pathway and suppress the electrode pulverization. It is important to note that such quasi-single-crystal structure would be helpful to explore other high-energy lithium storage materials based on alloying or conversion reactions.