H-ZSM5, Zn/H-ZSM5, and Co/H-ZSM5 catalyze thiophene desulfurization with high H2S selectivity using propane as the exclusive hydrogen source, Desulfurization rates and selectivities were much higher than at the Hz concentrations present during propane reactions. Zn+2 and Co+2 cations at exchange sites increased desulfurization rates. On H-ZSM5, desulfurization rates and selectivities with propane coreactants (20 kPa) were equivalent to those obtained with >200 kPa H-2; on Zn- and Co-exchanged H-ZSM5, the equivalent H2 pressures were 50-100 kPa. These data show that alkane dehydrogenation can be coupled with thiophene hydrogenation on surfaces to increase thiophene desulfurization and propane dehydrogenation rates simultaneously.