期刊
CATALYSTS
卷 13, 期 5, 页码 -出版社
MDPI
DOI: 10.3390/catal13050804
关键词
NiZr intermetallic catalyst; methane dry reforming; near ambient pressure XPS; carbon spillover; inverse model catalyst; chemical vapor deposition
To investigate the synergistic action of differently prepared Ni-ZrO2 phase boundaries in methane dry reforming, three catalyst systems including an inverse near-surface intermetallic NiZr catalyst precursor, bulk-intermetallic NixZry material, and a supported Ni-ZrO2 catalyst were compared. All three catalysts exhibit stable and highly efficient methane dry reforming activity with improved resistance to coke deposition due to the presence of extended Ni-ZrO2 phase boundaries formed by in situ activation. Methane is decomposed to carbon at metallic Ni-0 surface sites, while CO2 is converted to CO at reduced Zr centers at the phase boundaries. The surface-ZrO2 modified bulk Ni-0 catalyst shows the best decoking and carbon conversion conditions, attributed to the dispersed ZrO2 islands and short diffusion pathways for carbon.
To identify the synergistic action of differently prepared Ni-ZrO2 phase boundaries in methane dry reforming, we compared an inverse near-surface intermetallic NiZr catalyst precursor with the respective bulk-intermetallic NixZry material and a supported Ni-ZrO2 catalyst. In all three cases, stable and high methane dry reforming activity with enhanced anticoking properties can be assigned to the presence of extended Ni-ZrO2 phase boundaries, which result from in situ activation of the intermetallic Ni-Zr model catalyst systems under DRM conditions. All three catalysts operate bifunctionally; methane is essentially decomposed to carbon at the metallic Ni-0 surface sites, whereas CO2 reacts to CO at reduced Zr centers induced by a spillover of carbon to the phase boundaries. On pure bulk Ni-0, dissolved carbon accumulates in surface-near regions, leading to a sufficiently supersaturated state for completely surface-blocking graphitic carbon segregation. In strong contrast, surface-ZrO2 modified bulk Ni-0 exhibits virtually the best decoking and carbon conversion conditions due to the presence of highly dispersed ZrO2 islands with a particularly large contribution of interfacial Ni-0-ZrO2 sites and short C-diffusion pathways to the latter.
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