RESUMO
The catalysts comprising the main active compounds of Sn-Nx were synthesized using trichlorophenylstannane ((C6H5)Cl3Sn), nitrogen carbon-dots (NCDs), and activated carbon (AC) as starting materials, and the activity and stability of catalysts was evaluated in the acetylene hydrochlorination. According to the results on the physical and chemical properties of catalysts (TEM, XRD, BET, XPS and TG), it is concluded that NCDs@AC can increase (C6H5)Cl3Sn dispersity, retard the coke deposition of (C6H5)Cl3Sn/AC and lessen the loss of (C6H5)Cl3Sn, thereby further promoting the stability of (C6H5)Cl3Sn/AC. Based on the characterization results of C2H2-TPD and HCl adsorption experiments, we proposed that the existence of Sn-Nx can effectively strengthen the reactants adsorption of catalysts. By combing the FT-IR, C2H2-TPD and Rideal-Eley mechanism, the catalytic mechanism, in which C2H2 is firstly adsorbed on (C6H5)Cl3Sn to form (C6H5)Cl3Sn-C2H2 and then reacted with HCl to produce vinyl chloride, is proposed.
RESUMO
In the present work, tin-sulfur based catalysts were prepared using Na2SO3 and (CH3SO3)2Sn and were tested in acetylene hydrochlorination. Based on the analysis of experiments results, the acetylene conversion of (CH3SO3)2Sn/S@AC is still over 90%after a 50 h reaction, at the reaction conditions of T = 200 oC, VHCl/VC2H2 = 1.1:1.0 and C2H2-GSHV = 15 h-1. According to the results of X-ray photoelectron spectroscopy (XPS), HCl adsorption experiments, and acetylene temperature programmed desorption (C2H2-TPD), it is reasonable to conclude that the interaction between Sn and S not only can retard the oxidation of Sn2+ in catalysts but also strengthen the reactant adsorption capacity of tin-based catalysts. Furthermore, results obtained from nitrogen adsorption/desorption and XPS proved that the CH3SO3- can effectively decrease the coke deposition of (CH3SO3)2Sn/AC and thus prolong the lifetime of (CH3SO3)2Sn/AC.