Hollow Carbon Nanospheres Decorated with Abundant Pyridinic N<sup>+</sup>O<sup>–</sup> for Efficient Acetylene Hydrochlorination
Feng Li, Haiyang Zhang, Miaomiao Zhang, Linfeng Li, Lisha Yao, Wencai Peng, Jinli Zhang
Abstract
Considering the disadvantages of metallic catalyst and benchmark commercial activated carbon for acetylene hydrochlorination, such as considerable cost, metal loss, serious carbon deposition, and insufficient active sites, nonmetal hollow carbon nanospherical materials (PACP-T) with hierarchical porous structures were synthesized by the copolymerization of aniline and pyrrole via a self-templating method. Local active sites were constructed by decorating the carbon material with heteroatomic groups. The synthetic process dispersed active sites at the atomic level, which was promoted by local structural forces. Experiments and DFT calculations showed that most active sites were pyridinic N+O–. The superior activity might have been caused by the synergistic adsorption and activation of reactants by highly electronegative heteroatoms and abundant π-containing functional groups (C═C, N═C═N, aromatic ring, and pyridinic N+O–) at active sites on the catalyst. This promoted rapid reactions and impeded carbon deposition, which promoted the continuous exposure of active sites. The significantly improved activity and stability of the optimized PACP-800 catalyst promote its potential industrial applications.