Synthesis Gas Production via Dry Reforming of Methane over Manganese Promoted Nickel/Cerium–Zirconium Oxide Catalyst
Synthesis Gas Production via Dry Reforming of Methane over Manganese Promoted Nickel/Cerium–Zirconium Oxide Catalyst
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DOI：
10.1021/acs.iecr.8b04183
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发表时间：
2018-11
影响因子：
4.2
通讯作者：
Lu Yao;M. Gálvez;Changwei Hu;P. Da Costa
中科院分区：
文献类型：
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作者：
Lu Yao;M. Gálvez;Changwei Hu;P. Da Costa
采用浸渍法制备了Ni/Ce50-Zr50(Ni/Ce50-Zr50)和锰促进的Ni/Ce50-Zr50(Ni-Mn/Ce50-Zr50)催化剂，并将其用于甲烷干法重整反应。采用H_2程序升温还原、透射电子显微镜、X-射线光电子能谱、CO_2程序升温脱附、X-射线衍射仪、原位漫反射红外光谱和热重分析等手段对催化剂进行了表征。在低温下，锰助剂促进了反应中间体-CH2OH物种的形成。Ni和Mn物种之间的协同作用促进了CO2在Ni-Mn/Ce50-Zr50上的吸附。锰助剂不仅提高了催化剂的催化活性，而且生成了高H2/CO比的产物。在600℃、常压、空速20000h-1、CH4/CO2/Ar=1：1：8的条件下，在Ni-Mn/Ce50-Zr50催化剂上，CH4转化率为38.7%，CO2转化率为40.4%，H2/CO比为0.83。
Nickel/cerium–zirconium oxide (Ni/Ce50–Zr50) and manganese promoted Ni/Ce50–Zr50 (Ni–Mn/Ce50-Zr50) catalysts were prepared using an impregnation method and used in the dry reforming of methane. The catalysts were characterized by H2 temperature-programmed reduction, transmission electron microscopy, X-ray photoelectron spectroscopy, CO2 temperature-programmed desorption, X-ray diffraction, in situ diffuse reflectance infrared Fourier transform spectra, and thermogravimetric analysis. A manganese promoter facilitated the formation of the reaction intermediate—CH2OH species at low temperature. A synergistic effect between Ni and Mn species enhanced the adsorption of CO2 on Ni–Mn/Ce50-Zr50. A manganese promoter not only enhanced the catalytic activity but also led to a high H2/CO ratio product. At 600 °C, under atmospheric pressure, with 20 000 h–1 gas hourly space velocity and CH4/CO2/Ar = 1:1:8, on a Ni–Mn/Ce50-Zr50 catalyst, the CH4 conversion (38.7%), CO2 conversion (40.4%), and the H2/CO ratio (0.83) we...