화학공학소재연구정보센터
Chemical Engineering Journal, Vol.176, 42-48, 2011
Evaluation of gold on alumina catalyst deactivation dynamics during alpha-pinene isomerization
Synthesis of camphene is an important step in an industrial process for camphor production from alpha-pinene. Compared to conventional way of alpha-pinene to camphene transformation over acid-hydrated TiO2, gold on alumina catalyst was found to provide alpha-pinene isomerization conversion up to 99.9% and selectivity 60-80% making this catalyst very promising from an industrial viewpoint. However, deactivation of gold catalyst might be a serious obstacle for real industrial implementation. According to TPO and UV-vis-mass in situ it was shown that deactivation is caused by adsorption of hydrocarbons on the gold species. The dynamics of catalyst deactivation during alpha-pinene isomerization was presented based on a so-called "separable" deactivation model assumption. Effects of isomerization temperature, initial alpha-pinene concentration and gas atmosphere on catalyst deactivation with time-on-stream were investigated experimentally and correlated with the proposed deactivation function. The results showed that the alpha-pinene concentration was the major factor governing the deactivation of Au/gamma-Al2O3 catalyst under substrate-feeding conditions. When the alpha-pinene concentration was controlled at a relatively low level such as 0.4 vol.%, especially in hydrogen atmosphere, the total deactivation rate was negligible. An equation of the reaction rate taking into account the catalyst deactivation was suggested making prediction of deactivation behavior in alpha-pinene conversion at different initial concentrations. (C) 2011 Elsevier B.V. All rights reserved.