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Promoting effect of Co addition on the catalytic partial oxidation of methane at short contact time over a Rh/MgO catalyst

机译:在Rh / MgO催化剂上短时间内接触Co的添加对甲烷催化部分氧化的促进作用

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摘要

In catalytic partial oxidation of methane under isothermal conditions, a 0.3 wt% Rh/MgO catalyst modified with Co at a molar ratio of Co/Rh = 1 gave greater CH4 conversion and selectivity to CO and H2 than unmodified 0.3 wt% Rh/MgO. Characterization results using temperature-programmed reduction, extended X-ray absorption fine structure, and transmission electron microscopy demonstrated alloy formation between Rh and Co. In catalytic partial oxidation of methane without N2 dilution, the Rh–Co/MgO catalyst with Co/Rh = 1 suppressed the temperature increase near the catalyst bed inlet and yielded a flat temperature profile. This behavior can be interpreted as greater selectivity in the direct partial oxidation route in the presence of gas-phase oxygen and lower activity in the steam reforming of methane in the absence of gas-phase oxygen. The better performance of Rh–Co/MgO (Co/Rh = 1) compared with Rh/MgO may result from greater methane dissociation and reduction degree during the partial oxidation of methane.
机译:在等温条件下甲烷的催化部分氧化中,与未改性的0.3 wt%的Rh / MgO相比,以Co / Rh = 1的摩尔比进行Co改性的0.3 wt%的Rh / MgO催化剂具有更高的CH4转化率和对CO和H2的选择性。使用程序升温还原,扩展的X射线吸收精细结构和透射电子显微镜进行的表征结果表明,Rh和Co之间形成了合金。在不经N2稀释的甲烷催化部分氧化反应中,Rh–Co / MgO催化剂的Co / Rh =图1抑制了催化剂床入口附近的温度升高,并产生了平坦的温度曲线。可以将这种行为解释为在存在气相氧的情况下在直接部分氧化路线中具有更高的选择性,以及在不存在气相氧的情况下进行甲烷蒸汽重整时的较低活性。与Rh / MgO相比,Rh–Co / MgO(Co / Rh = 1)的性能更好,可能是由于甲烷在部分氧化过程中甲烷的分解度和还原度更高。

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