Tailoring hierarchical porous core-shell SnO₂@Cu upon Cu-Sn alloys through oxygen binding energy difference for high energy density lithium-ion storage

Rational design and construction of self-supporting anodes with high energy density is an essential part of research in the field of lithium-ion batteries. Tin oxide (SnO2) is restricted in application as a prospective high energy density anode due to inherent low conductivity and huge volume expansion of the charge/discharge process. A new strategy that combines high energy ball milling and nonsolvent induced phase separation (NIPS) method was employed to synthesize self-supporting electrodes in which porous SnO2 was encapsulated in a three-dimensional hierarchical porous copper (Cu) shell structure (3DHPSnO(2)@Cu). This unique structure was constructed due to the different binding energy of the alloy with oxygen, which are -0.91 eV for Cu41Sn11 and -1.17 eV for Cu5.6Sn according to the density functional theory calculation. 3DHPSnO(2)@Cu electrodes exhibited excellent discharge capacity with an initial reversible capacity of 4.35 mAh cm(-2) and a reversible capacity of 3.13 mAh cm(-2) after 300 cycles at a current density of 1.4 mA cm(-2). It is attributed that the porous Cu shell encapsulated with porous SnO2 provides buffer volume. Among them, the SnO2-Cu-SnO2 interface increases the electrical conductivity and the porous structure provides ion transport channels. This strategy opens a new pathway in the development of self-supporting electrode materials with high energy density.