Pd/Nb2O5/SiO2 Catalyst for the Direct Hydrodeoxygenation of Biomass-Related Compounds to Liquid Alkanes under Mild Conditions
Pd/Nb2O5/SiO2 Catalyst for the Direct Hydrodeoxygenation of Biomass-Related Compounds to Liquid Alkanes under Mild Conditions
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Pd/Nb2O5/SiO2 催化剂在温和条件下生物质相关化合物直接加氢脱氧为液态烷烃
DOI：
10.1002/cssc.201500053
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发表时间：
2015-05-22
期刊：
影响因子：
8.4
通讯作者：
Wang, Yanqin
中科院分区：
文献类型：
--
作者：
Shao, Yi;Xia, Qineng;Wang, Yanqin
制备了一种简单的负载pd的Nb2O5/SiO2催化剂，用于在温和条件下将生物质相关化合物加氢脱氧为烷烃。采用溶胶-凝胶法制备了分散在二氧化硅（Nb2O5/SiO2）中的氧化铌作为载体，并通过N-2吸附、XRD、NH3程序升温解吸（TPD）、TEM和能谱x射线能谱（EDAX）原子作图等多种技术对其进行了表征。表征结果表明，氧化铌是无定形的，并且在二氧化硅中分散良好。与商业Nb2O5相比，Nb2O5/SiO2表面暴露的活性氧化铌明显增加。在温和条件下（170℃，2.5 MPa）， Pd/10% Nb2O5/SiO2对4（2-呋喃基）-3-丁烯-2-酮（糠醛与丙酮的醛醇加合物）、棕榈酸、三硬脂和二苯醚（微藻油、植物油和木质素的模式化合物）的加氢脱氧反应有效，产率高（约94%），C-C键断裂少。更重要的是，由于NbOx对C-O键的裂解有明显的促进作用，且反应条件温和，C-C的裂解受到了很大的抑制，在150 h的流时间测试中，该催化剂对棕榈酸的加氢脱氧表现出了良好的活性和稳定性，十六烷的产率几乎没有下降（94-95%）。
A simple Pd-loaded Nb2O5/SiO2 catalyst was prepared for the hydrodeoxygenation of biomass-related compounds to alkanes under mild conditions. Niobium oxide dispersed in silica (Nb2O5/SiO2) as the support was prepared by the sol-gel method and characterized by various techniques, including N-2 adsorption, XRD, NH3 temperature-programmed desorption (TPD), TEM, and energy-dispersive X-ray spectroscopy (EDAX) atomic mapping. The characterization results showed that the niobium oxide species were amorphous and well dispersed in silica. Compared to commercial Nb2O5, Nb2O5/SiO2 has significantly more active niobium oxide species exposed on the surface. Under mild conditions (170 degrees C, 2.5 MPa), Pd/10% Nb2O5/SiO2 was effective for the hydrodeoxygenation reactions of 4( 2-furyl)-3-buten-2-one (aldol adduct of furfural with acetone), palmitic acid, tristearin, and diphenyl ether (model compounds of microalgae oils, vegetable oils, and lignin), which gave high yields (> 94%) of alkanes with little C-C bond cleavage. More importantly, owing to the significant promotion effect of NbOx species on C-O bond cleavage and the mild reaction conditions, the C-C cleavage was considerably restrained, and the catalyst showed an excellent activity and stability for the hydrodeoxygenation of palmitic acid with almost no decrease in hexadecane yield (94-95%) in a 150 h time-on-stream test.