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 C6.3H3.6N1.0O1.2, 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.