Graphdiyne-based Pd single-atom catalyst for semihydrogenation of alkynes to alkenes with high selectivity and conversion under mild conditions
| Autor: | Xue-Peng Yin, Hong-Juan Wang, Rui Si, Xiu-Li Lu, Tong-Bu Lu, Shang-Feng Tang, Chao Zhang |
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| Rok vydání: | 2020 |
| Předmět: |
chemistry.chemical_classification
Renewable Energy Sustainability and the Environment Infrared spectroscopy Alkyne 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Combinatorial chemistry 0104 chemical sciences Catalysis Styrene chemistry.chemical_compound Adsorption chemistry Phenylacetylene Atom General Materials Science 0210 nano-technology Selectivity |
| Zdroj: | Journal of Materials Chemistry A. 8:20925-20930 |
| ISSN: | 2050-7496 2050-7488 |
| Popis: | The development of efficient heterogeneous catalysts for alkyne hydrogenation with high activity and selectivity is highly desirable and yet remains a great challenge. Herein, a Pd single-atom catalyst (Pds–GDY) is prepared using graphdiyne as support, and used in the semihydrogenation of alkynes. As a proof of concept, the Pds–GDY exhibits a high activity for the semihydrogenation of phenylacetylene under mild reaction conditions, with a TOF of 6290 h−1, and a selectivity of 99.3% at 100% conversion, both much higher than those of the counterparts comprising Pd nanoparticles (NPs), namely, PdNP1–GDY (with 2 nm Pd NPs) and PdNP2–GDY (with 12 nm Pd NPs). In addition, after the full conversion of phenylacetylene, Pds–GDY could still maintain a selectivity as high as 98.9% towards styrene, with almost no phenylethane produced even with a prolonged reaction time; in contrast, for PdNP1–GDY and PdNP2–GDY, within the same reaction time, the selectivity decreases dramatically to 66.6% and 8.5%, respectively. Infrared spectroscopy reveals that Pds–GDY features the weakest adsorption to styrene, which is responsible for its high performance. This work provides an effective strategy to rationally design Pd catalysts for semihydrogenation of alkynes to alkenes with desirable activity and selectivity. |
| Databáze: | OpenAIRE |
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