Mechanism of reaction of CeO₂–CaO–Pd/HZSM5 catalyst in the Syngas process in the presence of sulfur-containing impurities

Abstract

CeO2–CaO–Pd/HZSM5 catalyst, prepared using HZSM5 supports, with CeO2–CaO as the additive components, HZSM5 as the acid component and Pd as the hydrogenation component, have been prepared by the impregnation method, and the catalytic and sulfur-tolerant performance in the Syngas-To-Dimethyl ether (STD) reaction with thiophene and H2S as probe sulfur poisons were examined. The prepared catalyst exhibited higher catalytic performance and better sulfur resistance than a conventional catalyst based on Cu/ZnO/Al2O3 and HZSM5. The sulfur content, Pd sulfidity and acid concentration were determined in order to ascertain the adsorption sites of sulfides on the surface of the catalyst, and the products of the STD reaction from sulfur-containing syngas in an autoclave were analysed by GC-MS at different reaction times in order to determine the sulfur-tolerance mechanism of the catalyst. The study confirms that almost no H2S is absorbed on the surface of CeO2–CaO–Pd/HZSM5 catalyst, while thiophene is absorbed and activated on the acid sites of HZSM5, and hydrogen is adsorbed dissociatively on Pd active sites, followed by active hydrogen spillover to the acid sites to promote hydrogenation and thus convert the adsorbed thiophene to hydrocarbons and hydrogen sulfide.

Effect of Surface Structure and Adsorption Activity on Implanting of b-Oriented ZSM-5 Zeolite Film on Modified α-Quartz Substrate

“…And the ZSM-5 pore size distribution agrees with it (Figure 10C). At the same time, there is a typical H4 hysteresis loop in the isotherm at high relative pressure, which is the result of the adsorption and desorption of N 2 in the mesoporous (Han and Liu, 2015; Chu et al, 2016). During the preparation of FC zeolite, the specific surface area (S total ) and micropore volume (V micro ) have different degrees of reduction, but the mesoporous specific surface area (S meso ) and mesopore volume (V meso ) increased to 136.6 [m 2 g −1 ], 0.3455 [m 3 g −1 ], respectively, this can greatly facilitate the rapid diffusion of the product to the catalyst surface and reduce the formation of coke.…”