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A successive hydrogenation system was constructed using a two-compartment cell separated by a Pd sheet. The hydrogenation rate changed greatly, depending on the kind of substrates used. For the purpose of improving the hydrogenation rate, the surface of a Pd sheet was modified with highly active catalysts such as Pd black, Pt, and Au by using active hydrogen passing through the Pd sheet as a reducing agent. As a result, the hydrogenation rate of unsaturated organic compounds such as 4-methylstyrene was markedly increased by the surface modification with these catalysts due to the increase in reaction zone and appearance of new active sites.