Catalytic conversion of sorbitol to gasoline-ranged products without external hydrogen over Pt-modified Ir-ReOx/SiO2
Catalytic conversion of sorbitol to gasoline-ranged products without external hydrogen over Pt-modified Ir-ReOx/SiO2
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DOI：
10.1016/j.cattod.2015.10.023
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发表时间：
2016-07
期刊：
影响因子：
5.3
通讯作者：
Sibao Liu;Okuyama Yasuyo;M. Tamura;Y. Nakagawa;Imai Akio;K. Tomishige
中科院分区：
文献类型：
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作者：
Sibao Liu;Okuyama Yasuyo;M. Tamura;Y. Nakagawa;Imai Akio;K. Tomishige
在无氢条件下，以Pt修饰的Ir-ReOx/SiO2为催化剂，在正癸烷+ H2O两相溶剂体系中对山梨醇进行了脱氧反应。在此条件下，可以得到较好的汽油馏分产品，包括C5-C6烷烃和C2-C6单官能化合物，如酮、醇、环醚和羧酸。Pt（3wt%）-Ir-ReOx/SiO2催化剂在汽油馏分中的催化性能最好。汽油馏分产品的最高收率为42%。产物的分布可以通过添加HZSM-5来调节。添加HZSM-5时，主要产物为C5-C6烷烃，而未添加HZSM-5时，主要产物为C2-C6单官能化合物。采用TPR、XRD、TEM、XANES、EXAFS、CO吸附等手段对催化剂进行了表征。结果表明，Pt-Ir-ReOx/SiO2催化剂表现出部分被ReOx物种覆盖的Pt-Ir合金颗粒结构。Pt（3）-Ir-ReOx/SiO2中的Pt原子数比Pt/SiO2或Pt-ReOx/SiO2中的多，这是由于Pt-Ir合金颗粒尺寸小的缘故。大量的表面Pt原子以及Pt、Ir和ReOx物种的协同作用使催化剂能够高效地通过山梨醇水相重整制氢，并且所产生的氢被消耗在C单键O键的氢解反应中。
Deoxygenation of sorbitol was carried out over a Pt-modified Ir-ReOx/SiO2catalyst in biphasic solvent system (n-decane + H2O) without external hydrogen. Good yield of gasoline-ranged products was obtained including C5–C6 alkanes and C2–C6 mono-functionalized compounds such as ketones, alcohols, cyclic ethers and carboxylic acids. The Pt(3 wt%)-Ir-ReOx/SiO2catalyst showed the best performance in the production of gasoline-ranged products. The maximum yield of gasoline-ranged products was 42%. The distribution of the products can be tuned by the addition of HZSM-5. The main products were C5–C6 alkanes with addition of HZSM-5 while the main products were C2–C6 mono-functionalized compounds without addition of HZSM-5. Characterizations such as TPR, XRD, TEM, XANES, EXAFS, CO adsorption were performed. The results demonstrated that the Pt-Ir-ReOx/SiO2catalyst showed the structure of Pt-Ir alloy particles partially covered with ReOxspecies. The number of surface Pt atoms in Pt(3)-Ir-ReOx/SiO2was larger than that of Pt/SiO2or Pt-ReOx/SiO2because of the small size of Pt-Ir alloy particles. The large number of surface Pt atoms and the synergetic effect of Pt, Ir and ReOxspecies make the catalyst efficiently generate hydrogen by aqueous phase reforming of sorbitol, and the generated hydrogen is consumed in the hydrogenolysis Csingle bondO bonds.