Hierarchically structured carbon replica of hybrid layered double hydroxideElectronic supplementary information (ESI) available: 13C NMR spectra, N2 adsorption-desorption isotherm, variation of the voltammetric charge. See DOI: 10.1039/c0nj00630k

A hierarchically structured carbon replica with a tri-modal distribution of porosity was prepared by pyrolysis of a three-dimensionally ordered macroporous (3-DOM) organic-inorganic hybrid layered double hydroxide (LDH). By an original inverse opal method involving LDH platelet regeneration, macroporous Mg 2 Al-vinyl benzene sulfonate (VBS) was synthesized and subsequently submitted to a moderate thermal treatment to induce the VBS in situ polymerization. Successive steps of carbonization and demineralization were conducted to yield to a carbon replica. A thermal treatment under inert atmosphere ensures the carbonization of the organic part and the simultaneous decomposition of the LDH into oxide and mixed oxide particles. The latter acts as a porogen agent during the acid-leaching step, which induces the removal of the inorganic part. The samples upon carbonization and the capacitive properties of the resulting carbon replica were thoroughly characterized using powder X-ray diffraction (PXRD), Fourier-transform infra-red (FTIR) and 13 C nuclear magnetic resonance (NMR) spectroscopy, field-emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM) and Brunauer-Emmet-Teller (BET) analysis of the nitrogen adsorption isotherm. 3-DOM carbon replicas exhibit poor capacitive behaviour in aqueous electrolyte, explained by a high ionic resistivity present in the porosity. Even though this electrical disruptive effect can be explained on the basis of the macroporosity of the disconnected carbon 3-DOM, this allows us to envisage other applications for this approach in order to obtain tri-modal carbon-based materials. Using a template approach, a 3-DOM LDH hybrid compound intercalated with VBS monomer has been successfully prepared and used to produce a hierarchically micro/meso/macroporous carbonaceous replica.