The methodology of metal‐involved preparation for carbon materials is favored by researchers and has attracted tremendous attention. Decoupling this process and the underlying mechanism in detail are highly required. Herein, the intrinsic mechanism of carbon fixation in graphitic carbon nitride (g‐C3N4) via the magnesium‐involved carbonization process is reported and clarified. Magnesium can induce the displacement reaction with the small carbon nitride molecule generated by the pyrolysis of g‐C3N4, thus efficiently fixing the carbon onto the in situ template of Mg3N2 product to avoid the direct volatilization. As a result, the N‐doped carbon nanosheet frameworks with interconnected porous structure and suitable N content are constructed by reconstruction of carbon and nitrogen species, which exhibit a comparable photoelectric conversion efficiency (8.59%) and electrocatalytic performances to that of Pt (8.40%) for dye‐sensitized solar cells.
Carbon materials have rapidly grown as highly promising candidates to replace noble metal catalysts in energy storage/conversion technologies. In this work, a strategy of hydrogen‐bonding triggered assembly to configure hollow carbon nanosheets by applying Silicalite‐1 as a substrate in the aqueous solution of dopamine is reported. Remarkably, the combined density functional theory modelling and experimental verification present a molecule/nano‐scale insight into the nature of the bonding behavior during the fabrication process. It is demonstrated that the SiOH on the surface of Silicalite‐1 acts as an anchor and that it is energetically favorable to pre‐adsorb the building blocks of polydopamine by hydrogen‐bonding, which triggers the subsequent assembly. As an example, the as‐prepared hollow carbon nanosheets with unique structure can efficiently catalyze tri‐iodide reduction and a power conversion efficiency up to 8.58%.
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