Highly Uniform Carbon Sheets with Orientation-Adjustable Ordered Mesopores.

A soft-hard template-assisted method toward the unconventional free-standing ordered mesoporous carbon sheets (OMCSs) with uniform hexagonal morphology is developed by applying MgAl-layered double hydroxide (MgAl-LDH) as the hard template, triblock copolymer F127 as the soft template, and phenolic resols as the carbon sources. It is found that the surface of MgAl-LDH can induce the morphology variation of resol-F127 monomicelles, leading to the formation of vertically or horizontally aligned mesopore arrays in the OMCSs, which can in turn determine their electrochemical energy storage behaviors in supercapacitors with different configurations. In an all-solid-state supercapacitor with two face-to-face electrodes, an OMCS with vertical mesopores manifests the best performance among the samples. By contrast, in a micro-supercapacitor with in-plane film-like electrodes, an OMCS with horizontal mesopores delivers higher energy/power densities than the other OMCSs, which are also comparable to the state-of-the-art supercapacitors based on ordered mesoporous carbons. The achievement of uniform carbon sheets with orientation-adjustable mesopore arrays can help elucidate their electrochemical storage mechanism and allow the optimization of the performances according to the device configuration, thus providing a powerful tool for the manipulation of energy storage devices on the nanoscale.