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- Title
Breaking scaling relationships in alkynol semi-hydrogenation by manipulating interstitial atoms in Pd with d-electron gain.
- Authors
Yang, Yang; Zhu, Xiaojuan; Wang, Lili; Lang, Junyu; Yao, Guohua; Qin, Tian; Ren, Zhouhong; Chen, Liwei; Liu, Xi; Li, Wei; Wan, Ying
- Abstract
Pd catalysts are widely used in alkynol semi-hydrogenation. However, due to the existence of scaling relationships of adsorption energies between the key adsorbed species, the increase in conversion is frequently accompanied by side reactions, thereby reducing the selectivity to alkenols. We report that the simultaneous increase in alkenol selectivity and alkynol conversion is achieved by manipulating interstitial atoms including B, P, C, S and N in Pd catalysts. A negative linear relationship is observed between the activation entropies of 2-methyl-3-butyn-2-ol and 2-methyl-3-buten-2-ol which is highly related to the filling of d-orbital of Pd catalysts by the modification of p-block elements. A catalyst co-modified by B and C atoms has the maximum d charge of Pd that achieves a 17-fold increase in the turn-over frequency values compared to the Lindlar catalysts in the semi-hydrogenation of 2-methyl-3-butyn-2-ol. When the conversion is close to 100%, the selectivity can be as high as 95%. Circumventing the linear scaling relationship in the semi-hydrogenation is challenging. Here the authors report a method for breaking the scaling relationships using ordered mesoporous carbon-supported Pd nanocatalysts with d-electron gain by p-block atoms occupying interstitial sites in the lattice as a greener alternative to Lindlar catalysts for the selective hydrogenation of alkynols.
- Subjects
ATOMS; ENOLS; YNOLS; CATALYSTS; ADSORPTION (Chemistry); CATALYTIC hydrogenation; HYDROGENATION
- Publication
Nature Communications, 2022, Vol 13, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-022-30540-z