화학공학소재연구정보센터
Chemical Engineering Journal, Vol.259, 161-169, 2015
High-performance Pd nanoalloy on functionalized activated carbon for the hydrogenation of nitroaromatic compounds
Coconut shell activated carbon (AC) was successfully functionalized with diaminocyclohexane groups. The functionalized AC was used as a carrier to complex metal ions for preparation of the supported Pd, Pd-B and Pd-Ni-B. Pd or its alloy particles were highly dispersed on the functionalized AC and have a narrow size distribution of 2-5 nm. Amorphous structure of Pd-B and Pd-Ni-B were confirmed by the X-ray diffraction (XRD). X-ray photoelectron spectroscopy (XPS) showed that some of the electrons were transferred from B to Pd, which makes Pd electron-enriched. Hydrogen temperature programmed desorption (H-2-TPD) tests indicated that desorption peaks of the amorphous alloys shifted to higher temperatures with respect to Pd/C, indicating that hydrogen was more strongly bonded to the amorphous alloys. Their catalytic performances were evaluated in hydrogenation of nitroaromatic compounds. In hydrogenation of p-chloronitrobenzene (p-CNB), the Pd-Ni-B nanoalloys on the functionalized AC displayed a TOF value of 8316/h, and p-CNB conversion of 98.6% with a p-chloroaniline (p-CAN) selectivity of 94.6%. The highly active hydrogenation property of the Pd-Ni-B/C was further confirmed in reduction of alpha-nitronaphthalene. In addition to reduction of -NO2 groups, partial aromatic rings were also hydrogenated over the Pd-Ni-B/C. The substrate conversion was 99.6% together with a highest TOF value of 88/h. (C) 2014 Elsevier B.V. All rights reserved.