Reaction Kinetics, Mechanisms and Catalysis ( IF 1.7 ) Pub Date : 2018-12-07 , DOI: 10.1007/s11144-018-1515-9 Katarzyna Świrk , Monika Motak , Teresa Grzybek , Magnus Rønning , Patrick Da Costa
Ni/Al/Mg layered double hydroxides (LDHs) modified with low loading of yttrium (0.2 and 0.4 wt%) were used in dry reforming of methane at 700 °C. Physicochemical characterization, such as: X-ray fluorescence, N2 sorption, X-ray diffraction, temperature programmed reduction in H2, temperature programmed desorption of CO2, H2 chemisorption, thermogravimetry analysis coupled by mass spectrometry and Raman spectroscopy, showed that the introduction of low loadings of yttrium lead to a smaller Ni° crystallite size, a decrease in reducibility of the nickel, and a decreased number of basic sites in the modified Ni/LDHs catalysts. The doping with 0.4 wt% of Y improves catalytic activity resulting in higher CH4 and CO2 conversions at 700 °C, i.e., ca. 84% and ca. 87%, respectively with no clear deactivation observed after 5 h run. The increase in CO2 conversion and a decrease of H2/CO ratio indicates that side reactions occurs during DRM.
中文翻译:
钇含量低对CO中Ni基层状双氢氧化物的影响
低负载钇量(0.2和0.4 wt%)改性的Ni / Al / Mg层状双氢氧化物(LDHs)用于在700°C的甲烷干重整中。物理化学表征,例如:X射线荧光,N 2吸附,X射线衍射,H 2的程序升温还原,CO 2的程序升温脱附,H 2化学吸附,质谱和拉曼光谱相结合的热重分析表明:低含量钇的引入导致较小的Ni°微晶尺寸,镍还原性的降低以及改性Ni / LDHs催化剂中碱性位点的减少。掺入0.4 wt%的Y可改善催化活性,从而提高CH 4700°C时的CO2和CO 2转化率,即约 约84%运行5小时后,没有观察到明显的失活,分别为87%。CO 2转化率的增加和H 2 / CO比的降低表明在DRM期间发生了副反应。