Journal
CHEMCATCHEM
Volume 6, Issue 8, Pages 2339-2344Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201402018
Keywords
activated carbon; heterogeneous catalysis; hydrochlorination; nitrogen; reaction mechanisms
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Funding
- National Basic Research Program of China (973 Program) [2012CB720302]
- Program for Changjiang Scholars and Innovative Research Team in University [IRT1161]
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A highly active nitrogen-doped pitch-based spherical activated carbon catalyst (PSAC-N) is synthesized through a nitrogen-doping treatment and used as a nonmetal catalyst for acetylene hydrochlorination. The conversion of acetylene on PSAC-N exceeds 68% and the selectivity of vinyl chloride is over 99% at a temperature of 250 degrees C, an acetylene gas hourly space velocity of 120 h(-1), and a feed volume ratio V(HCl)/V(C2H2) of 1.15. DFT calculations performed with Gaussian 09 program package reveal that the active site of PSAC-N has a N-6v (quaternary nitrogen bonded between two 6-membered rings) structure. A seven benzene ring unit model is used in the DFT study. In addition, the reason for inactivation for PSAC-N catalysts is discussed. Of all the adsorption energies obtained, the adsorption capacity of hydrogen chloride on PSAC-N is the highest, which indicates strong ability for acetylene hydrochlorination. The reaction mechanism is determined, and the reaction energy of N-6v(7) calculated as 236.2 kJ mol(-1).
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