4.6 Article

Interface effect of mixed phase Pt/ZrO2 catalysts for HCHO oxidation at ambient temperature

期刊

JOURNAL OF MATERIALS CHEMISTRY A
卷 5, 期 26, 页码 13799-13806

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ROYAL SOC CHEMISTRY
DOI: 10.1039/c7ta03888g

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资金

  1. National Key Research and Development Program of China [2016YFC0202202]
  2. National Natural Science Foundation of China [21407152, 21590811]

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A series of high-efficiency Pt/ZrO2 catalysts were successfully prepared by simple methods on the basis of a ZrO2 support with a mixed monoclinic/tetragonal phase structure. The activity test results showed that the mixed phase catalysts exhibited higher catalytic activity than the pure monoclinic phase, and HCHO can be completely oxidized into CO2 and H2O at near ambient temperature. XRD, Raman and HRTEM results demonstrated that the monoclinic-tetragonal phase interface with abundant defects was formed due to the introduction of the tetragonal phase. According to the results of TEM, XPS and H-2-TPR, the mixed phase interfacial structure can induce the formation of the active oxygen species, ionic Pt delta+ species, strong metal-support interaction and low-temperature reducibility, which was vital for the significant improvement of the catalytic activity. Furthermore, the specific HCHO reaction rate of the catalysts at 55 degrees C increased from 0.8 x 10(-3) to 10.4 x 10(-3) mmol h(-1) m(-2) and the activation energy decreased remarkably from 213.5 to 24.7 kJ mol(-1) with the increase of the biphase interface content. In situ DRIFTS spectra showed that the special interfacial structure can change the reaction pathway of HCHO oxidation and inhibit the formation of inert carbonate species, thus greatly enhancing the HCHO oxidation activity.

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