Volume 134, Issue 8 e202114539
Forschungsartikel

Mesoporosity-Enabled Selectivity of Mesoporous Palladium-Based Nanocrystals Catalysts in Semihydrogenation of Alkynes

Hao Lv

Hao Lv

Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu, 610064 China

These authors contributed equally to this work.

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Huaiyu Qin

Huaiyu Qin

Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu, 610064 China

These authors contributed equally to this work.

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Mingzi Sun

Mingzi Sun

Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR

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Fengrui Jia

Fengrui Jia

Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu, 610064 China

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Prof. Bolong Huang

Corresponding Author

Prof. Bolong Huang

Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR

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Prof. Ben Liu

Corresponding Author

Prof. Ben Liu

Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu, 610064 China

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First published: 16 December 2021
Citations: 3

Abstract

We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)-based nanobundles catalysts. The best mesoporous PdP displayed full conversion, remarkable activity, excellent selectivity, and high stability in semihydrogenation of 1-phenyl-1-propyne, all of which are remarkably better than commercial Lindlar catalysts. Mechanistic investigations ascribed high semihydrogenation selectivity to the continuous crystalline framework and penetrated mesoporous channel of catalysts that weakened the adsorption and interaction capacity of alkenes and thus inhibited over-hydrogenation of alkenes to industrially unfavorable alkanes. Density functional theory calculations further demonstrated that convex crystalline mesoporosity of nanobundles catalysts electronically optimized the coordination environment of Pd active sites and energetically changed hydrogenation trends, resulting in a superior semihydrogenation selectivity to targeted alkenes.

Conflict of interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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