Efficient synthesis of bioetheric fuel additive by combining the reductive and direct etherification of furfural in one-pot over Pd nanoparticles deposited on zeolites

Efficient synthesis of bioetheric fuel additive by combining the reductive and direct etherification of furfural in one-pot over Pd nanoparticles deposited on zeolites
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通过沉积在沸石上的 Pd 纳米粒子一锅法结合糠醛的还原和直接醚化,有效合成生物醚燃料添加剂

DOI:
10.1016/j.gee.2021.07.001
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发表时间:
2021-07
期刊:
Green Energy Environ.
影响因子:
--
通讯作者:
关业军
关业军
中科院分区:
其他
文献类型:
--
作者:
Xiaowen Guo;Haihong Wu;Peng WU;Mingyuan He;关业军

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呋喃甲醚被认为是一种很有前途的燃料添加剂。负载型Pd催化剂上的一步还原醚化反应为制备呋喃甲醚提供了一条简便的途径。然而,制备可重复使用的Pd还原醚化催化剂仍然是一个巨大的挑战。本研究制备了一系列SiO_2负载型Pd催化剂,其粒径在2.2~28 nm之间。系统地研究了它们的织构性质和在呋喃还原醚化反应中的催化性能。这一结果揭示了粒子大小对CDouble Bondo在Pd表面上的加氢/氢解竞争的影响。我们发现大于3 nm的Pd纳米粒子是一步还原醚化反应的首选催化剂。基于这一发现,我们制备了Pd/ZSM-5双功能催化剂,该催化剂含有大于3 nm的Pd纳米粒子,并在氨基有机硅烷存在下降低了酸度,成功地用于还原醚化和直接醚化一锅合成醚。这一策略在有效地将主要副产物呋喃乙醇转化为乙醚方面显示出显著的优势,同时抑制了不希望发生的副反应。
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 SiO2supported 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 Cdouble bondO 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.
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