Hydrogenation of CO2 on MoO3/Al2O3 and γ-Al2O3

IF 1.3 4区 化学 Q4 CHEMISTRY, PHYSICAL
M. A. Kipnis, P. V. Samokhin, R. S. Galkin, E. A. Volnina, N. A. Zhilyaeva
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Abstract

The physicochemical and catalytic (CO2 hydrogenation) characteristics of Mo-containing catalysts were studied. The catalysts containing 8 and 15 wt % Mo oxide were prepared by impregnation of γ‑Al2O3 with ammonium paramolybdate, followed by drying and calcination at 500°C. The introduction of Mo oxide reduced the pore volume of the support and increased the average pore size, indicating that molybdenum oxide was distributed in the support pores. According to the X-ray diffraction analysis, the calcinated catalyst did not contain the crystalline MoO3 phase. According to the Raman spectra, oxygen-containing formations were present on the catalyst surface, with Mo atoms tetrahedrally and octahedrally coordinated to the oxygen atoms. The impregnated MoO3 was partially reduced with hydrogen during linear heating, starting from 320°C. The hydrogenation of CO2 (gas composition, vol %: 30.7 CO2, 68 H2, the rest was N2; 0.5 g sample) was studied under conditions of linear heating to 400°C. The main reaction was the reverse reaction of CO steam reforming. The contribution of methanation to CO2 hydrogenation was small. An increase in the temperature and pressure had a positive effect on CO2 conversion. When the pressure increased from 1 to 5 MPa, the CO content was approximately doubled. In the CO2 hydrogenation, appreciable activity (although significantly lower compared to that of Mo-containing catalysts) was also exhibited by γ-Al2O3, preliminarily heated to 400°C in an H2 flow. The activity of alumina also increased with pressure.

Abstract Image

二氧化碳在 MoO3/Al2O3 和 γ-Al2O3 上的氢化反应
摘要 研究了含钼催化剂的物理化学和催化(二氧化碳加氢)特性。用对钼酸铵浸渍γ-Al2O3,然后在 500°C 下干燥和煅烧,制备了含 8 和 15 wt % 氧化钼的催化剂。氧化钼的引入减少了支撑体的孔隙体积,增加了平均孔径,表明氧化钼分布在支撑体的孔隙中。根据 X 射线衍射分析,煅烧后的催化剂不含结晶 MoO3 相。拉曼光谱显示,催化剂表面存在含氧形态,钼原子与氧原子呈四面体和八面体配位。在 320°C 开始的线性加热过程中,浸渍的 MoO3 被氢气部分还原。在线性加热至 400°C 的条件下,研究了二氧化碳的氢化(气体成分,体积百分比:30.7 CO2,68 H2,其余为 N2;0.5 克样品)。主要反应是 CO 蒸汽重整的逆反应。甲烷化对 CO2 加氢的影响很小。温度和压力的增加对 CO2 转化有积极影响。当压力从 1 兆帕增加到 5 兆帕时,CO 的含量大约增加了一倍。在 CO2 加氢过程中,在 H2 流中初步加热到 400°C 的 γ-Al2O3 也表现出明显的活性(尽管与含 Mo 催化剂相比明显较低)。氧化铝的活性也随着压力的增加而提高。
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来源期刊
Kinetics and Catalysis
Kinetics and Catalysis 化学-物理化学
CiteScore
2.10
自引率
27.30%
发文量
64
审稿时长
6-12 weeks
期刊介绍: Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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