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Selective hydrogenation of cinnamaldehyde with NixFe1-xAl2O4+δ composite oxides supported Pt catalysts: CO versus CC selectivity switch by varying the Ni/Fe molar ratios
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-12-03 , DOI: 10.1016/j.jcat.2020.11.036
Huiyue Xin , Wenbo Zhang , Xixi Xiao , Li Chen , Peng Wu , Xiaohong Li

Due to coexistence of two conjugated unsaturated functional groups in cinnamaldehyde (CAL), exploring efficient catalysts with desirable selectivity to highly value-added products is still challengeable for the selective hydrogenation of CAL. Herein, NixFe1-xAl2O4+δ spinel composite metal oxides (SCMOs) supported Pt catalysts were developed and proved to be active and selective for the selective hydrogenation of CAL. Moreover, the selectivity switch can be realized just by changing the Ni/(Fe + Ni) molar ratios in NixFe1-xAl2O4+δ SCMOs. As a result, the excellent cinnamyl alcohol (COL) selectivity (~92.2%) and hydrocinnamaldehyde (HCAL) selectivity (~80.7%) were achieved on Pt/FeAl2O4+δ and Pt/NiAl2O4+δ, respectively. Based on the kinetic investigation of further hydrogenation of semi-hydrogenated product, the reason for the selectivity switch with Pt/NixFe1-xAl2O4+δ was revealed. In combination with detailed characterization, the excellent COL selectivity on Pt/FeAl2O4+δ can be attributed to more Pt(1 1 1) facets and FeOx species which can facilitate the preferential activation of Cdouble bondO bonds; while the high HCAL selectivity on Pt/NiAl2O4+δ is owing to the fact that there are more low coordinated active sites and two neighbouring Pt sites.



中文翻译:

用Ni x Fe 1- x Al 2 O 4+ δ复合氧化物负载的Pt催化剂对肉桂醛进行选择性加氢:通过改变Ni / Fe摩尔比来改变C 双键OC 双键C的选择性

由于肉桂醛(CAL)中两个共轭不饱和官能团的共存,对于CAL的选择性加氢而言,探索对高附加值产品具有所需选择性的有效催化剂仍然是挑战。本文中,开发了Ni x Fe 1- x Al 2 O 4+ δ尖晶石复合金属氧化物(SCMOs)负载的Pt催化剂,并证明其对CAL的选择性加氢具有活性和选择性。而且,仅通过改变Ni x Fe 1- x Al 2 O 4+ δ中的Ni /(Fe + Ni)摩尔比就可以实现选择性切换。SCMO。其结果是,优良的肉桂醇(COL)选择性(〜92.2%)和氢化肉桂醛(HCAL)选择性(〜80.7%)是在Pt / FeAl金属实现2 ö 4+ δ和Pt /的NiAl 2 ö 4+ δ分别。通过对半氢化产物进一步加氢的动力学研究,揭示了Pt / Ni x Fe 1- x Al 2 O 4+ δ选择性切换的原因。结合详细的表征,Pt / FeAl 2 O 4+ δ上出色的COL选择性可归因于更多的Pt(1 1 1)面和FeO x能促进优先激活双键CO键的物质;而对Pt / NiAl 2 O 4+ δ的HCAL选择性较高,是由于存在更多的低配位活性位点和两个相邻的Pt位点。

更新日期:2021-01-04
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