Green Energy & Environment ( IF 10.7 ) Pub Date : 2021-07-08 , DOI: 10.1016/j.gee.2021.07.001 Xiaowen Guo , Haihong Wu , Peng Wu , Mingyuan He , Yejun Guan
Furfuryl ethers have been considered to be a promising fuel additive. One step reduction etherification of furfural over supported Pd catalysts provides a facile way for the preparation of furfuryl ether. However, the preparation of a reusable Pd catalyst for reductive etherification remains to be a great challenge. In this study, a series of SiO2 supported Pd catalysts with particle size ranging from 2.2 nm to 28 nm were prepared. Their textural properties and catalytic performance in furfural reductive etherification have been systematically studied. The results herein shed light on the particle size effect on the competition between hydrogenation/hydrogenolysis of CO in furfural over Pd surface. We found out that Pd nanoparticles larger than 3 nm are preferred for one step reductive etherification. Based on this finding, we prepared a Pd/ZSM-5 bifunctional catalyst comprising Pd nanoparticles larger than 3 nm and decreased acidity in presence of amino organosilane, which served as a bifunctional catalyst succeeding in one-pot synthesis of ether via reductive-etherification and direct-etherification. This strategy showed significant advantage in efficiently converting furfuryl acohol, a major side-product, into ether, while suppressing the undesired side-reactions.
中文翻译:
通过在沉积在沸石上的 Pd 纳米颗粒上结合糠醛在一锅中的还原和直接醚化,高效合成生物醚燃料添加剂
糠基醚被认为是一种很有前途的燃料添加剂。糠醛在负载型钯催化剂上的一步还原醚化为制备糠基醚提供了一种简便的方法。然而,制备用于还原醚化的可重复使用的 Pd 催化剂仍然是一个巨大的挑战。在本研究中,制备了一系列粒径为2.2 nm 至28 nm的SiO 2负载Pd 催化剂。系统地研究了它们的结构特性和在糠醛还原醚化中的催化性能。本文的结果阐明了粒度对 C 的氢化/氢解之间竞争的影响Pd 表面糠醛中的 O。我们发现大于 3 nm 的 Pd 纳米粒子更适合一步还原醚化。基于这一发现,我们制备了一种 Pd/ZSM-5 双功能催化剂,该催化剂包含大于 3 nm 的 Pd 纳米颗粒并在氨基有机硅烷存在下降低了酸度,该催化剂作为双功能催化剂成功通过还原醚化一锅法合成醚和直接醚化。该策略在有效地将主要副产物糠醇转化为乙醚方面显示出显着优势,同时抑制了不需要的副反应。