Sandwich-structured graphene hollow spheres limited Mn2SnO4/SnO2 heterostructures as anode materials for high-performance lithium-ion batteries

• Heterostructured Mn 2 SnO 4 /SnO 2 @spherical graphene composite is reported. • Mn 2 SnO 4 /SnO 2 nanoheterostructures are sandwiched between spherical graphene shells. • Mn infiltration promotes SnO 2 dissolution-redeposition and heterostructure formation. • Heterostructures produce internal electric field to improve Li + transport kinetics. • The difference between Mn 2 SnO 4 /SnO 2 @SG and SnO 2 @SG was compared and discussed. Sn-based metal oxides and composites have been widely investigated as candidate anodes for lithium-ion batteries. However, continuous capacity fade caused by serious volumetric expansion and crystal pulverization is often noticed during lithiation and alloying processes. In this study, we design a novel heterogeneous structural composite by constructing sandwich-structured graphene hollow spheres limited Mn 2 SnO 4 /SnO 2 heterostructures (Mn 2 SnO 4 /SnO 2 @SG), of which infiltration of Mn source promotes the dissolution-redeposition of SnO 2 in hollow-spherical graphene (SnO 2 @SG) and their in-situ transformation into Mn 2 SnO 4 ; and the uniform distributed Mn 2 SnO 4 and SnO 2 nanoparticles are adjacent each other to form heterostructure within the sandwiched graphene hollow spheres. By comparing with the single metal oxide SnO 2 @SG material, the influence of the microstructure, chemical composition, element valence state and electrochemical properties of the heterostructured Mn 2 SnO 4 /SnO 2 @SG is investigated. The results show that the construction of Mn 2 SnO 4 /SnO 2 heterostructure dramatically improves electronic/ionic transport kinetics and increases lithium storage reversibility, therefore leading to distinctly superior rate capability (823.8 mAh g −1 at 5 C) and cycling capacity. An ultra-high discharge capacity of 1180.4 mA h g −1 is maintained up to 100 cycles at 100 mA g −1 . The promising electrochemical performances can be attributed to the sandwiched-structure hollow graphene spherical skeleton and the formation of unique Mn 2 SnO 4 /SnO 2 heterostructures.