关键词: 1,2-pentanediol Organic acids Pt/NC hydrogenation xylose

来  源:   DOI:10.1002/cssc.202401109

Abstract:
The direct synthesis of 1,2-pentanediol (1,2-PeD) from renewable xylose and its derivatives derived from hemicellulose is appealing yet challenging due to its low selectivity for the target product. In this study, one-pot catalytic conversion of xylose to 1,2-PeD was performed by using nitrogen-doped carbon (NC) supported Pt catalysts with the assistance of organic acids. A remarkable yield of 49.3% for 1,2-PeD was achieved by reacting 0.1869 g xylose in 30 mL water at 200 °C under a hydrogen pressure of 3 MPa for 8 h in the presence of 0.1 g of 2.5Pt/NC600 catalyst and 0.1869 g propanoic acid co-catalyst. The presence of vicinal Pt-acid pair sites on the surface of the 2.5Pt/NC600 catalyst exhibited a synergistic effect in promoting the hydrogenation of furfural to furfuryl alcohol intermediate and subsequent hydrogenation and ring-opening reactions leading to the formation of 1,2-PeD. The addition of organic acids, may serve as both acid catalyst for dehydration of xylose and hydrogen donor for hydrogenation of furfural and furfuryl alcohol, thereby promoting the one-pot conversion of xylose to 1,2-PeD. Remarkably, the 2.5Pt/NC600 catalyst demonstrated outstanding catalytic performance and good reusability over five consecutive cycles without significant deactivation.
摘要:
由可再生木糖及其衍生自半纤维素的衍生物直接合成1,2-戊二醇(1,2-PeD)是吸引人的,但由于其对目标产物的低选择性而具有挑战性。在这项研究中,通过使用氮掺杂的碳(NC)负载的Pt催化剂,在有机酸的帮助下,将木糖一锅催化转化为1,2-PeD。1,2-PeD的显著产率为49.3%,通过在0.1g的2.5Pt/NC600催化剂和0.1869g丙酸助催化剂存在下,在3MPa的氢气压力下,在200°C下使0.1869g木糖在30mL水中反应8小时来实现。在2.5Pt/NC600催化剂的表面上存在邻近的Pt-酸对位点在促进糠醛氢化为糠醇中间体以及随后的氢化和开环反应中表现出协同作用,导致1,2-PeD的形成。有机酸的加入,既可以作为木糖脱水的酸催化剂,也可以作为糠醛和糠醇加氢的氢供体,从而促进木糖向1,2-PeD的一锅法转化。值得注意的是,2.5Pt/NC600催化剂在连续五个循环中表现出出色的催化性能和良好的可重用性,而没有明显的失活。
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