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Acceptorless dehydrogenation and hydrogenation of N- and O-containing compounds on Pd 3 Au 1 (111) facets

Type of publication Peer-reviewed
Publikationsform Original article (peer-reviewed)
Author Cui Xinjiang, Huang Zhangjun, van Muyden Antoine P., Fei Zhaofu, Wang Tao, Dyson Paul J.,
Project Development of sustainable catalytic processes enhanced by ionic liquids
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Original article (peer-reviewed)

Journal Science Advances
Volume (Issue) 6(27)
Page(s) eabb3831 - eabb3831
Title of proceedings Science Advances
DOI 10.1126/sciadv.abb3831

Open Access

URL http://doi.org/10.1126/sciadv.abb3831
Type of Open Access Publisher (Gold Open Access)

Abstract

Catalytic dehydrogenation and hydrogenation of amines and alcohols are important in the synthesis of fine chemicals. Despite several efficient homogeneous catalysts having been identified, highly active heterogeneous catalysts remain elusive, although they would meet an unmet need. Here, we show that bimetallic Pd-Au nanoparticles with Pd-to-Au molar ratios of 3:1 immobilized on multiwall carbon nanotubes (Pd 3 Au 1 /CNT) display high catalytic activity in the oxidant-free and acceptorless dehydrogenation and hydrogenation of N- and O-containing heterocyclic compounds, amines/imines, and alcohols/ketones. Transmission electron microscopy analysis demonstrates the preferential exposure of Pd 3 Au 1 (111) facets on the Pd 3 Au 1 /CNT catalyst. Mechanistic insights combining experimental data with density functional theory calculations reveal that the Pd 3 Au 1 (111) surface enhances both dehydrogenation and hydrogenation reactions and provides a rationale for the observed enhancements.
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