期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 5, 期 3, 页码 2516-2528出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.6b02865
关键词
Bimetallic catalyst; Carbon dioxide; Electronic property; Formylation; Hydrogenation
资金
- National Natural Science Foundation of China [21172219, 91645119, 21472189]
- Natural Science Foundation of Guangdong Province, China [2015A030312007]
- Jinan Double Hundred Talents Plan
- Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control
Bimetallic Pd-Au catalyst was prepared by depositing the Pd-Au alloy nanoparticles on polyaniline-functionalized carbon nanotubes (PANI-CNT) and the resulting Pd-Au/PANI-CNT catalyst exhibited excellent catalytic activity for the N-formylation of pyrrolidine using CO2/H-2. The structural and electronic properties of the Pd- Au/PANI-CNT was characterized by X-ray powder diffraction (XRD), nitrogen adsorption desorption, transmission electron microscopy (TEM), high angle annular dark-field scanning LU transmission electron microscopy (HAADF-STEM), and X-ray photoelectron spectroscopy (XPS). Under optimized conditions, an N-formylpyrrolidine yield of 98.3% was obtained from pyrrolidine and CO2/H-2 at 125 degrees C by using Pd Au/PANICNT with a Pd/Au molar ratio of 1:1. Our research further reveals that Pd atoms should be the true active sites for the hydrogenation reaction and the N-formylation reaction might occur mainly over Pd atoms or over the interface between Pd atoms and Au atoms for the bimetallic Pd Au/PANI-CNT catalyst. The enhanced catalytic performance of bimetallic Pd Au/PANI-CNT is mainly related to beneficial interactions between Pd atoms and Au atoms, leading to changes of the electronic properties of the formed bimetallic Pd Au nanoparticles.
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