Department of Materials Science and Biotechnology, Graduate School of Science and Engineering, Ehime University, 3 Bunkyo-cho, Matsuyama, 790-8577, Japan.
Institute for Catalysis, Hokkaido University, Kita 21 Nishi 10, Kita-ku Sapporo, 001-0021, Hokkaido, Japan.
Chemistry. 2019 Nov 22;25(65):14762-14766. doi: 10.1002/chem.201902668. Epub 2019 Oct 23.
The selective and efficient removal of oxygenated groups from lignin-derived phenols is a critical challenge to utilize lignin as a source for renewable aromatic chemicals. This report describes how surface modification of a zeolite-supported Pt catalyst using ionic liquids (ILs) remarkably increases selectivity for the hydrodeoxygenation (HDO) of phenols into arenes under mild reaction conditions using atmospheric pressure H . Unmodified Pt/H-ZSM-5 converts phenols into aliphatic species as the major products along with a slight amount of arenes (10 % selectivity). In contrast, the catalyst modified with an IL, 1-butyl-3-methylimidazolium triflate, keeps up to 76 % selectivity for arenes even at a nearly complete conversion of phenols. The IL on the surface of Pt catalyst may offer the adsorption of phenols in an edge-to-face manner onto the surface, thus accelerating the HDO without the ring hydrogenation.
从木质素衍生的酚类中选择性且高效地去除含氧基团是利用木质素作为可再生芳烃化学品来源的关键挑战。本报告描述了如何使用离子液体(ILs)对沸石负载的 Pt 催化剂进行表面改性,在使用大气压 H2 的温和反应条件下,显著提高了酚类氢解脱氧(HDO)生成芳烃的选择性。未经修饰的 Pt/H-ZSM-5 将酚类转化为主要产物为脂肪族物质,同时生成少量芳烃(选择性为 10%)。相比之下,用 IL,1-丁基-3-甲基咪唑三氟甲磺酸酯修饰的催化剂在酚类几乎完全转化的情况下,芳烃的选择性仍保持在 76%左右。Pt 催化剂表面上的 IL 可能提供酚类以边缘对-面的方式吸附到表面上,从而在不进行环加氢的情况下加速 HDO。