Journal
NANO RESEARCH
Volume 15, Issue 6, Pages 5024-5031Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-4235-4
Keywords
heterogeneous catalysis; single atom; synergistic; quinoline; hydrogenation
Categories
Funding
- National Natural Science Foundation of China [92161112, 21932006]
- National Key Research and Development Program of China [2018YFA0208504, 2018YFA0703503]
- Youth Innovation Promotion Association of CAS [2017049]
- National Science Basic Program of Shaanxi [S2020-JC-WT-0001]
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Single-atom catalysts (SACs) with the advantages of homogeneous and heterogeneous catalysts have become a hot-spot in catalysis field. However, the lack of metal-metal bond in SACs limits their hydrogenation activity. This study proposes a catalyst, Ir1+NPs/CMK, which combines single iridium atoms and nanoparticles to boost the catalytic activity of quinoline hydrogenation, and achieves significant improvement in reactivity.
Single-atom catalysts (SACs) with the advantages of homogeneous and heterogeneous catalysts have become a hot-spot in catalysis field. However, for lack of metal-metal bond in SACs, H-2 has to go through heterolytic dissociation pathway, which has higher barrier than homolytic dissociation pathway, and thus limits the hydrogenation activity of SACs. Herein, we propose and demonstrate through constructing synergistic iridium single atoms and nanoparticles co-existed catalyst (denoted as Ir1+NPs/CMK) to boost the catalytic activity of quinoline hydrogenation. Both experimental and density functional theory calculation results confirm that Ir-1 single sites activate quinoline, while Ir nanoparticles boost hydrogen dissociation. H atoms generated at Ir nanoparticles migrate to the quinoline bounded Ir-1 single sites to complete hydrogenation. The Ir1+NPs/CMK catalyst exhibits much higher reactivity with turnover frequency of 7,800 h(-1) than those counterpart Ir-1/CMK and Ir-NPs/CMK catalysts, and is 20,000 times higher activity of commercial Ir/C benchmark catalyst for hydrogenation of quinoline under the same reaction conditions. This synergistic catalysis strategy between single atoms and nanoparticles provides a solution to further improve the performance of SACs for hydrogenation.
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