For the first time, a macroscopic method was used to measure directly
diffusivity of fast diffusing species such as methane in silicalite. A
form of Wicke-Kallenbach technique was applied to measure intracrysta
lline diffusivity. The technique uses a single embedded zeolite crysta
l as a membrane and a mass-selective detector to determine the transie
nt mass response and hence the diffusion flux passing through the memb
rane. A concentration-difference driving force is used rather than a p
ressure-difference driving force. The diffusivities calculated from bo
th adsorption and desorption transients were in excellent agreement, t
hus providing a check for the self-consistency of the data. The diffus
ivities of carbon dioxide, methane, ethane, propane and butane in sili
calite between 30 and 70 degrees C have been compared with those from
the literature. The diffusivities reported here are between those meas
ured with microscopic methods and those measured with other macroscopi
c methods.