Influence of sulfating method on La–Ni–S2O82–/ZrO2–Al2O3 solid superacid catalyst for n-pentane isomerization

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Progress in Reaction Kinetics and Mechanism Pub Date : 2020-01-01 DOI:10.1177/1468678319897724
Haiqiang Zhao, Hua Song, Lele Zhao, Feng Li
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Abstract

La–Ni–S2O82–/ZrO2–Al2O3 catalysts were successfully prepared by two different methods of sulfate impregnation, and the physico-chemical properties of the catalysts were characterized by X-ray diffraction, Brunauer–Emmett–Teller analysis, Fourier transform infrared spectroscopy, pyridine adsorption–infrared spectroscopy, and X-ray photoelectron spectroscopy techniques. Catalytic activities were evaluated in a fixed-bed flow reactor using n-pentane isomerization as the probe reaction. Compared with catalyst La–Ni–S2O82–/ZrO2–Al2O3-I, prepared by the traditional impregnation method, the catalyst La–Ni–S2O82–/ZrO2–Al2O3-W, prepared by the incipient-wetness impregnation method, possessed higher pore volume, pore size, sulfur content, and stronger Brønsted acid sites. The catalytic activity for La–Ni–S2O82–/ZrO2–Al2O3-W was maintained at around 56% within 3000 min with an isopentane selectivity of 88% which showed much greater stability than that of La–Ni–S2O82–/ZrO2–Al2O3-I. This can be attributed to the fact that (1) the large pore size and pore volume of La–Ni–S2O82–/ZrO2–Al2O3-W can largely suppress carbon deposition and (2) the more numerous and stronger Brønsted acid sites for La–Ni–S2O82–/ZrO2–Al2O3-W guaranteed to provide enough acid sites for isomerization during the reaction process.
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硫酸盐酸化对La-Ni-S2O82 - / ZrO2-Al2O3固体超强酸催化剂正戊烷异构化的影响
采用两种不同的硫酸盐浸渍方法成功制备了La-Ni-S2O82 - / ZrO2-Al2O3催化剂,并通过x射线衍射、Brunauer-Emmett-Teller分析、傅立叶变换红外光谱、吡啶吸附红外光谱和x射线光电子能谱技术对催化剂的理化性质进行了表征。以正戊烷异构化为探针反应,在固定床流动反应器中评价了催化活性。与传统浸渍法制备的La-Ni-S2O82 - / ZrO2-Al2O3-I催化剂相比,初湿浸渍法制备的La-Ni-S2O82 - / ZrO2-Al2O3-W催化剂具有更高的孔容、孔径、硫含量和更强的Brønsted酸位。在3000 min内,La-Ni-S2O82 - / ZrO2-Al2O3-W的催化活性保持在56%左右,异戊烷选择性为88%,稳定性远高于La-Ni-S2O82 - / ZrO2-Al2O3-I。这可以归结为:(1)La-Ni-S2O82 - / ZrO2-Al2O3-W具有较大的孔径和孔体积,可以在很大程度上抑制碳沉积;(2)La-Ni-S2O82 - / ZrO2-Al2O3-W具有更多且更强的Brønsted酸位,保证了在反应过程中为异构化提供足够的酸位。
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来源期刊
CiteScore
2.10
自引率
0.00%
发文量
5
审稿时长
2.3 months
期刊介绍: The journal covers the fields of kinetics and mechanisms of chemical processes in the gas phase and solution of both simple and complex systems.
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