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

Molecular Catalysis [2022]
Feng Li, Haiyang Zhang, Miaomiao Zhang, Wencai Peng, Lisha Yao, Yanzhao Dong, Jinli Zhang
ABSTRACT

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.

MATERIALS

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