Fabrication of Self-Assembled Graphene Oxide Film and Its Application in Aqueous Zinc Metal Batteries.

Fabrication of well-dispersed thin graphene oxide (GO) films (GOFs) has always been a challenge. Herein, a quick preparation method for GOFs was developed using our homemade GO with a large lateral size. The film can be prepared in less than 2 h via a metal framework-induced self-assembly process. The thickness of the films can be as thin as ∼15.5 μm, which will be thinner with compression. When it is used as a flexible modification layer on the Zn metal for aqueous Zn-ion batteries, Zn can grow along the [010] direction in plane and stack orderly along the [002] direction even on the Cu substrate with GOF through epitaxial plating owing to negligible lattice mismatch between the (002) plane of Zn and the hexagonal ring [also (002) plane for graphite] of GO. Meanwhile, the rich O groups on the GO film can provide abundant zincophilic points and promote uniform distribution of Zn around the anode. Finally, dendrite-free and dense Zn stripping/plating can be achieved and well remained. The GOF@Zn symmetric cell reveals long cyclic stability of 1300 h at 1 mA cm and 1 mA h cm. It still can remain at 350 h even at a very high current density of 10 mA cm accompanied by a high areal capacity of 10 mA h cm. With the same plating amount of 5 mA h cm, the thickness of the plated Zn is only ∼10 μm with GOF modification, very close to the theoretical value of 8.54 μm, much thinner than that without GOF (∼18 μm), indicating very dense deposition. Full cells assembled with the GOF@Zn anode and the MnO cathode exhibit a capacity retention rate of 71% over 1000 cycles at 0.7 A g, showing much better cycling performance than that using bare Zn.