Dry reforming of methane over 5 wt% Ni/Ce1-xPrxO2-δ catalysts: Performance and characterisation of active and inactive carbon by transient isotopic techniques
作者： M.A. Vasiliades , M.M. Makri , P. Djinović , B. Erjavec , A. Pintar
DOI: 10.1016/J.APCATB.2016.03.012
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摘要: Abstract The effects of Ce1-xPrxO2-δ support composition (x = 0.0–0.8) and reaction temperature (550–750 °C) on the catalytic activity selectivity important features mechanism dry reforming methane (DRM) over supported Ni (5 wt%) were investigated. Of particular interest concentration active inactive carbon formed, relative contribution CH4 CO2 activation routes towards formation structure morphology which was formed. For these characterization studies, steady-state isotopic transient kinetic analysis (13CO2-SSITKA), temperature-programmed oxidation (TPO) following 13CO2/12CH4/He reforming, thermal gravimetric coupled with TPO (TGA-TPO), scanning electron miscroscopy (SEM-EDX) transmission microscopy atomic resolution (HRTEM) powder X-ray diffraction (XRD) employed. amount formed via found to strongly depend Pr-dopant composition. At 550 °C, route (besides that route) 65.7 60.1%, respectively, for CeO2 Ce0.2Pr0.8O2 carriers, whereas at 750 °C respective values 54.0 50.9%. Filamentous thin layers graphitic identified as main morphologies carbon. surface coverage truly participates in CO (θC = 0.03–0.15 at 550 °C 0.07–3.4 at 750 °C). A pool reversibly adsorbed measured (θ = 1.5–4.1) first time, dependent T. introduction 20 atom-% Pr ceria lattice caused a significant reduction rate marginal decrease catalyst’s stability after 25 h stream. Further (80 atom-%) drastic deposited stream (0.07 wt% C) but appreciable CH4- CO2-conversions H2/CO gas-product ratio (a drop by factor 1.85, 1.45 1.47, respectively). latter performance is correlated increase form carbonate-like species.
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