期刊
MATERIALS
卷 14, 期 10, 页码 -出版社
MDPI
DOI: 10.3390/ma14102495
关键词
supported Ni; ZrO2 catalysts; Ni metal particles; methane partial oxidation; activation procedure; heterogeneous catalysis
类别
资金
- Sapienza University of Roma [RM11715C7E58658B]
Ni/ZrO2 catalysts prepared by different methods showed high activity and selectivity for the catalytic partial oxidation of methane to syngas. The interaction between Ni-ZrO2 helped to limit Ni aggregation during catalytic runs, and the catalytic activity depended on the activation procedures.
Ni/ZrO2 catalysts, active and selective for the catalytic partial oxidation of methane to syngas (CH4-CPO), were prepared by the dry impregnation of zirconium oxyhydroxide (Z(hy)) or monoclinic ZrO2 (Z(m)), calcination at 1173 K and activation by different procedures: oxidation-reduction (ox-red) or direct reduction (red). The characterization included XRD, FESEM, in situ FTIR and Raman spectroscopies, TPR, and specific surface area measurements. Catalytic activity experiments were carried out in a flow apparatus with a mixture of CH4:O-2 = 2:1 in a short contact time. Compared to Z(m), Z(hy) favoured the formation of smaller NiO particles, implying a higher number of Ni sites strongly interacting with the support. In all the activated Ni/ZrO2 catalysts, the Ni-ZrO2 interaction was strong enough to limit Ni aggregation during the catalytic runs. The catalytic activity depended on the activation procedures; the ox-red treatment yielded very active and stable catalysts, whereas the red treatment yielded catalysts with oscillating activity, ascribed to the formation of Ni delta+ carbide-like species. The results suggested that Ni dispersion was not the main factor affecting the activity, and that active sites for CH4-CPO could be Ni species at the boundary of the metal particles in a specific configuration and nuclearity.
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