Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 47, Pages 52668-52677Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c15407
Keywords
ruthenium; nanostructure engineering; electronic property; catalyst; selective hydrogenation; heteroarenes; DFT
Funding
- Ministry of Education, Culture, Science, Sports, and Technology (MEXT) of Japan [18H05251]
- CSIR, India [09/086(1231)2015-EMR-I]
- SERB research grant, DST, India [CRG/2019/000647]
- Grants-in-Aid for Scientific Research [18H05251] Funding Source: KAKEN
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Active metal catalysts are the key in chemical industry for sustainable production of multitude of chemical resources. Here, we report a new ruthenium (Ru) composite with a synergistically controlled nanostructure and electronic properties as a highly efficient hydrogenation catalyst which comprises stable small Ru nanoparticles (mean particle size, ca. 0.9 nm) in situ generated into a nanoporous N-functionalized carbon with high surface area (ca. 650 m(2) g(-1)) and has strong electron-donating power of Ru sites of nanoparticles. The scalable and highly reusable catalyst, prepared from a self-assembled Ru complex, performs actively with low per metal usage under mild conditions (60-80 degrees C and 0.5-1.0 MPa H-2) for selective hydrogenation of various quinolines and pyridines. The role of electron-donating properties of the new Ru nanohybrid for highly efficient catalysis was characterized by both experiments and computational studies. Density functional theory calculations reveal that weak adsorption energies of quinoline at the electron-rich Ru surface prevents poisoning caused by its strong coordination and provides excellent reusability of the catalyst, while low activation barriers for the hydrogenation steps of the N-heterocyclic ring correlate with high catalytic activity. Our catalyst exhibits 5-24-fold higher turnover frequency up to ca. 167 h(-1) among the efficient noble metal catalysts reported for selective hydrogenation of quinoline to 1,2,3,4-tetrahydroquinoline.
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