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首页> 外文期刊>Catalysis Today >Influence of nickel precursors on the properties and performance of Ni impregnated zeolite 5A and 13X catalysts in CO2 methanation
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Influence of nickel precursors on the properties and performance of Ni impregnated zeolite 5A and 13X catalysts in CO2 methanation

机译:镍前体对二氧化碳硫酸盐5A和13X催化剂性能和性能的影响

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Zeolite 13X and 5A supported Ni catalysts were synthesized for CO2 methanation using the evaporation impregnation method. The influence of using different Ni precursors (nitrate, citrate, and acetate) as well as calcination temperatures on the catalyst properties and performance were investigated. XRD, SEM-EDX, TEM, STEM-EDX, N-2 physisorption, H-2-TPR, TPD-NH3 and TG/DTA were used for detailed characterization of the catalysts. The parent structure of the zeolites did not change during catalyst synthesis. Using nickel citrate and acetate resulted in smaller NiO particle size compared to nitrate. STEM-EDX results showed that all the Ni-precursor complexes entered more efficiently the 13X zeolite structure, which is mainly due to steric hindrance resulting from the smaller pore size of 5A. Methanation experiments revealed that the 13X catalysts synthesized using nickel citrate (5% Ni) displayed clearly higher activity, compared to the catalysts synthesized using nickel nitrate or nickel acetate. A 79% conversion at 320 degrees C was obtained with 100% selectivity towards CH4 and the catalyst showed excellent stability during 200 h testing. Overall, it can be concluded that the Ni precursor significantly influences the physico-chemical characteristics and catalytic properties of Ni 13X and Ni 5A zeolite catalysts in CO2 methanation: complex size and pore size matter.
机译:采用蒸发浸渍法合成了13X和5A沸石负载镍催化剂,用于CO2甲烷化反应。研究了使用不同镍前驱体(硝酸盐、柠檬酸盐和醋酸盐)以及煅烧温度对催化剂性能和性能的影响。采用XRD、SEM-EDX、TEM、STEM-EDX、N-2物理吸附、H-2-TPR、TPD-NH3和TG/DTA对催化剂进行了详细表征。在催化剂合成过程中,分子筛的母体结构没有发生变化。与硝酸盐相比,使用柠檬酸镍和醋酸盐可使NiO粒径更小。STEM-EDX结果表明,所有镍前驱体配合物都能更有效地进入13X沸石结构,这主要是由于5A孔径较小导致的空间位阻。甲烷化实验表明,与使用硝酸镍或醋酸镍合成的催化剂相比,使用柠檬酸镍(5%镍)合成的13X催化剂显示出明显更高的活性。在320℃下,转化率为79%,对CH4的选择性为100%,催化剂在200小时的试验中表现出良好的稳定性。总的来说,可以得出结论,镍前驱体显著影响Ni 13X和Ni 5A沸石催化剂在CO2甲烷化中的物理化学特性和催化性能:复杂尺寸和孔径物质。

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