Functionalized ionic liquid coatings in the Pd-catalyzed selective hydrogenation of acetylene in ethylene-rich feeds

Daniel Kremitzl , Karoline Röhrs , Marc B. Williams , Peter S. Schulz , Peter Wasserscheid
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Abstract

This study explores the tuning of a Pd/Al2O3 hydrogenation catalyst for the selective removal of trace acetylene from ethylene-rich feeds by coating the catalyst with non-functionalized and functionalized ionic liquids (denoted as SCILL and Advanced SCILL materials, respectively). These materials were tested in an automated continuous hydrogenation rig converting 3300 ppm of acetylene in excess ethylene, a gas mixture mimicking a technical front-end steam cracker feed composition. While the sulfonic-acid-functionalized IL coating resulted in a highly active but very unselective catalyst converting mainly ethylene to ethane, an Advanced SCILL catalyst prepared from a nitrile-functionalized IL reduced the acetylene concentration down to less than 1 ppm, while leaving over 99% of the ethylene untouched. We also examined the potential transformations of the IL layer under reaction conditions by means of 1H NMR. Except for a ketone-functionalized IL, which was inherently labile, all tested ILs primarily underwent C2-ethylation or remained unaltered. Our findings highlight the great potential of functionalized ILs in modifying heterogeneous hydrogenation catalysts.

Abstract Image

功能化离子液体涂层在 Pd 催化富乙烯原料中乙炔选择性加氢反应中的应用
本研究通过在钯/Al2O3 加氢催化剂上涂覆非官能化和官能化离子液体(分别称为 SCILL 和高级 SCILL 材料),探讨了如何调整钯/Al2O3 加氢催化剂,以便从富含乙烯的进料中选择性地去除痕量乙炔。这些材料在自动连续加氢装置中进行了测试,在过量乙烯中转化 3300 ppm 的乙炔,这种气体混合物模拟了技术前端蒸汽裂解炉进料成分。磺酸官能化 IL 涂层产生的催化剂活性很高,但选择性很差,主要将乙烯转化为乙烷,而用腈官能化 IL 制备的高级 SCILL 催化剂则将乙炔浓度降至 1ppm 以下,而 99% 以上的乙烯未被转化。我们还通过 1H NMR 检查了 IL 层在反应条件下的潜在转化。除了酮官能化 IL 本身具有易变性外,所有测试的 IL 主要都发生了 C2- 乙基化或保持不变。我们的研究结果凸显了官能化 IL 在改性异相加氢催化剂方面的巨大潜力。
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CiteScore
3.70
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