Construction of multistage porous carbon materials for the hydrochlorination of acetylene: Impact of nitrogen incorporation.

• Multistage porous carbon materials rich in C-N local active domains were constructed. • Reactants were synergistically activated by C-N active sites and π-containing groups. • The structure-performance relationship was also clarified using DFT calculations. • The disadvantages of acetylene hydrochlorination catalyzed by AC were resolved. • Significantly improved stability endows the catalyst a bright application prospect. The benchmark carbon-based catalyst, activated carbon (AC), has a low catalytic activity due to its uniform surface charge distribution and stable structure. To overcome these problems, melamine-phenol-formaldehyde (MPF) resin, which is rich in pyridinic N and pyrrolic N, multi-porous C-N materials rich with defect sites were synthesized in situ by heat treatment using silica sol as the template and phenol, melamine, and formaldehyde as the carbon and nitrogen sources. The experimental results and characterization techniques revealed that carbon materials with abundant hierarchical pores and local C-N active sites were constructed by incorporating heteroatom-containing groups. Hydrogen chloride and acetylene molecules were activated due to the high electronegativity of defective sites, and the synergistic interactions between pyridinic N and π-containing functional groups (C=C, triazine ring, etc.). The structure-performance relationship was also clarified using DFT calculations. In addition, the strong interactions between heteroatomic sites and metal species also made MPF-800 an admirable metal catalyst support. Overall, the disadvantages of acetylene hydrochlorination catalyzed by benchmark AC were resolved. : The non-metallic carbon materials (MPF- T) exhibit remarkable catalytic performance and maintain outstanding long-term stability in the hydrochlorination of acetylene [Display omitted] [ABSTRACT FROM AUTHOR]