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A Pt/CeO2‐ZrO2 catalytic system was able to initiate an extremely intense hydrogen spillover providing a huge amount of activated hydrogen (12 mol/mol Pt) at temperatures –50°C ‐ +25°C, which was not observed before. The idea was to use this activated hydrogen for reduction of carbonyl compounds under ambient conditions. Thus, the efficient and selective heterogeneous hydrogenation of carbonyl compounds of different structure, including 5‐hydroxymethylfurfural and cinnamaldehyde, to the corresponding alcohols with quantitative yields was successfully performed over the Pt/CeO2‐ZrO2 catalysts at room‐temperature and atmospheric pressure of H2. The proposed catalysts afforded hydrogenation under significantly milder conditions with a much higher activity and selectivity compared to the commercial catalysts and reported catalytic systems. Hydrogenation of the C=O bond in the presence of a C=C bond proceeded with a high regioselectivity.

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