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Thermal Unequilibrium of PdSn Intermetallic Nanocatalysts: From in situ Tailored Synthesis to Unexpected Hydrogenation Selectivity.

Effective control on chemoselectivity to C=O over C=C bonds in catalytic hydrogenation reactions is uncommon with Pd-based catalysts because of the favored adsorption of C=C bonds. Here we report a unique orthorhombic PdSn intermetallic phase with unprecedented chemoselectivity toward C=O hydrogenation. We observed the formation and metastability of this PdSn phase in situ . During a natural cooling process, the PdSn nanoparticles readily revert to the favored Pd 3 Sn 2 phase. Instead, using a thermal quenching method, we prepared a pure-phase PdSn nanocatalyst. PdSn shows an >96% selectivity toward hydrogenating C=O bonds of various α,β-unsaturated aldehydes, highest in reported Pd-based catalysts. Further study suggests that efficient quenching prevents the reversion from PdSn- to Pd 3 Sn 2 -structured surface, the key to the desired catalytic performance. Density functional theory calculations and analysis of reaction kinetics provide an explanation for the observed high selectivity.