Mesoporous graphene-layered double hydroxides free-standing films for enhanced flexible supercapacitors

• Free-standing graphene oxide/layered double hydroxide (LDH) films were fabricated by flow-directed assembly.
• Mesoporous reduced graphene oxide (rGO)/LDH films formed after a reduction process.
• Embedded LDH nanosheets act as mesopore-creating guest.
• Flexible rGO/CoAl-LDH//rGO all-solid-state asymmetric SC demonstrates an excellent performance.

Two-dimensional graphene materials as supercapacitors electrode have attracted tremendous attention owing to their high surface area and exceptionally electrical conductivity, while it is still a great challenge to achieve desired mesoporous graphene electrodes as the easy aggregation of graphene nanosheets. Here we report the design and fabrication of mesoporous free-standing reduced graphene oxide (rGO)-based films by introducing layered double hydroxides (LDHs) nanoplatelets into the interlayer of rGO nanosheets. The nanostructures regular evolutions of rGO/CoAl-LDH free-standing film due to the embedding of LDHs were rationally investigated with detail experiments. Moreover, the flexible all-solid-state asymmetric supercapacitor device fabricated by using rGO/CoAl-LDH as positive electrode demonstrates a superior performance compared to most reported rGO-based free-standing film electrodes. The results presented here provide valuable insights into exploring mesoporous graphene-based free-standing architectures for highly-efficient and stable energy storage devices.

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