Journal
ACS CATALYSIS
Volume 10, Issue 24, Pages 14560-14566Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04523
Keywords
CeO2 nanocrystals; surface oxygen vacancy; frustrated Lewis pair sites; selective hydrogenation of crotonaldehyde; reaction mechanism
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Funding
- Experimental Technology Development Project of Zhejiang Normal University [20200024]
- Natural Science Foundation of Zhejiang Province [LQ20B030007]
- Natural Science Foundation of China [21773212, 21525313, 91745202, 91945301]
- Chinese Academy of Sciences
- Changjiang Scholars Program of the Ministry of Education of China
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Selective hydrogenation of alpha,beta-unsaturated aldehydes to unsaturated alcohols is important for the synthesis of fine chemicals, yet very challenging. Herein, we reported a metal-free CeO2 nanorods (rCeO(2)) catalyst for gas-phase transformation of crotonaldehyde to crotyl alcohol with the highest selectivity of 93.2% at 323 K. Compared to CeO2 nanocubes and nanopolydra, r-CeO2 shows a much higher crotyl alcohol production rate, comparable turnover frequency to those of noble-metalbased catalysts, and very high crotyl alcohol selectivity. This can be associated with a relatively high density of surface oxygen vacancies on rCeO(2), which constructs the solid frustrated Lewis pair sites with enhanced heterolytic H-2 dissociation and preferred crotonaldehyde adsorption via the C=O bond. However, a further reduction of r-CeO2 by H-2 was observed to be unfavorable with regard to both catalytic activity and selectivity, because of the emergence of crotonaldehyde adsorption via the C=C bond. These findings provide a potential approach to fabricate high-performance and low-cost catalysts for selective hydrogenation of alpha,beta-unsaturated aldehydes to unsaturated alcohols using bare CeO2 with a rigid surface structure design.
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