The search for efficient nontoxic catalysts able to perform industrial hydrogenations is a topic of interest, with relevance to many catalytic processes. Herein, we describe a mechanistic phenomenon for the activation and spillover of hydrogen for remarkable selectivity in the semi-hydrogenation of acetylene over sub-1 nm Pd nanoclusters confined within sodalite (SOD) zeolite (Pd@SOD). Specifically, hydrogen is dissociated on the Pd nanoclusters to form hydrogen species (i.e., hydrogen atoms and hydroxyl groups) that spill over the SOD surfaces. The design and utilization of the small-pore zeolite SOD (six-membered rings with 0.28×0.28 nm channels) is crucial as it only allows H diffusion into the channels to reach the encapsulated Pd nanoclusters and thus avoids over-hydrogenation to form ethane. Pd@SOD exhibits an ethylene selectivity of over 94.5 %, while that of conventional Pd/SOD is approximately 21.5 %.
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