4.5 Article

The texture evolution of g-C3N4 nanosheets supported Fe catalyst during Fischer-Tropsch synthesis

期刊

MOLECULAR CATALYSIS
卷 444, 期 -, 页码 90-99

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ELSEVIER SCIENCE BV
DOI: 10.1016/j.molcata.2016.12.011

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资金

  1. Natural Science Foundation of China [21373254, 21503256, 21673272]
  2. PetroChina [PRIKY14006, PRIKY15038, PRIKY15039, PRIKY15042]

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Graphitic carbon nitride (GCN) nanosheets decorated with iron nanoparticles (Fe/g-C3N4) were synthesized and used as catalysts in FTS. The crystal structure and morphology of Fe/g-C3N4 were characterized with XRD, FT-IR, HRTEM, EXAFS, BET, and its texture evolution during Fischer-Tropsch synthesis was monitored. It was shown that there were two types of iron species in Fe/GCN, i.e., dissolved iron, in which irons dissolved into g-C3N4 matrix as single atoms, and formed mainly at low Fe loadings. In contrast, when the loading exceeded the dissolved saturation, the irons would coordinate with (-N N-)(2-) to form the second type of iron species, Fe(NCN) like species. The dissolved iron was more difficult to thermally decompose and convert into iron carbide than Fe(NCN) like species. Such a slow transformation gave birth to unique induction period for low loading Fe catalysts. Moreover, the N-containing bases or defects of g-C3N4 might play a critical role in enhancing O/P ratio. As a result, g-C3N4 supported 40 wt% Fe sample exhibited highest activity and C2(=)-C4(=) selectivity. Besides, the g-C3N4 possessed a structure memory effect analogous to hydrotalcite

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