F. Engelke et al., ADSORPTION, DESORPTION, AND INTERPARTICLE MOTION OF HYDROGEN ON SILICA-SUPPORTED RUTHENIUM - A STUDY BY IN-SITU NUCLEAR-MAGNETIC-RESONANCE, The Journal of chemical physics, 101(9), 1994, pp. 7262-7272
H-1 NMR line shapes of hydrogen adsorbed on silica-supported ruthenium
at pressures of 10(-6)-10 Torr were studied by using selective excita
tion via DANTE sequences. A transition from inhomogeneous to homogeneo
us line broadening was observed at hydrogen coverage of similar to 0.5
. The spectra were simulated by using generalized Bloch equations that
included N-site exchange processes. The homogeneous line shape origin
ates from increased hydrogen mobility, whereas proton-proton dipolar c
ouplings are negligibly small. A rate parameter k obtained from this m
odel quantifies the average mobility of hydrogen in the exchange proce
ss. This parameter increases by more than three orders of magnitude wh
en the hydrogen coverage changes from 0.4 to 0.8. The simulations of l
ine shapes obtained at variable temperatures showed that k exhibits Ar
rhenius behavior with an activation energy of 52 (+/-5) kJ/mol and pre
exponential factor k(0)=4X10(10) is implied that the motion of hydroge
n must involve desorption, interparticle diffusion, and readsorption.