Templated Synthesis of Exfoliated Porous Carbon with Dominant Graphitic Nitrogen

We present here a new approach for the synthesis of nitrogen-doped porous graphitic carbon (g-NC) with a stoichiometry of C_6.3H_3.6N_1.0O_1.2, using layered silicate as a hard sacrificial template. Autogenous exfoliation is achieved due to the heterostacking of 2D silicate and nitrogen-doped carbon layers. Micro- and meso-porosity is induced by melamine and cetyltrimethylammonium (C₁₆TMA). Our density functional calculations and X-ray photoelectron spectroscopy (XPS) observations confirm that the most dominant nitrogen configuration in g-CN is graphitic, while pyridinic and pyrrolic nitrogens are thermodynamically less favored. Our large-scale lattice dynamics calculations show that surface termination with H and OH groups at pores accounts for the observed H and O in the composition of the synthesized g-NC. We further evaluate the electrocatalytic and the supercapacitance activities of g-NC. Interestingly, this material exhibits a specific capacitance of ca. 202 F g^-1 at 1 A g^-1, retaining 90% of its initial capacitance after 10,000 cycles.