Total Hydrogenation of Furfural over Pd/Al2O3 and Ru/ZrO2 Mixture under Mild Conditions: Essential Role of Tetrahydrofurfural as an Intermediate and Support Effect

Total Hydrogenation of Furfural over Pd/Al2O3 and Ru/ZrO2 Mixture under Mild Conditions: Essential Role of Tetrahydrofurfural as an Intermediate and Support Effect
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温和条件下 Pd/Al2O3 和 Ru/ZrO2 混合物上糠醛的全氢化:四氢糠醛作为中间体和支持作用的重要作用

DOI:
10.1021/acssuschemeng.8b00801
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发表时间:
2018-05-01
影响因子:
8.4
通讯作者:
Wu, Peng
Wu, Peng
中科院分区:
化学1区
文献类型:
--
作者:
Huang, Renjie;Cui, Qianqian;Wu, Peng

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在温和条件下,研究了钯钌负载催化剂的物理混合物对糠醛(FAL)在水溶液中的全加氢反应。单金属催化剂对全加氢表现出不完全的选择性:负载型钯催化剂倾向于生成四氢糠醛(THFAL)、糠醇(FA)和四氢糠醇(THFA)的混合物,而负载型钌催化剂倾向于加氢C = O键。当负载Pd和Ru催化剂混合时,THFA的产率显著提高。支持依赖性促进效应显著;在30℃、0.5 MPa H2条件下,Pd/Al2O3和Ru/ZrO2混合物的THFA产率达到99%。详细的动力学研究表明,以THFAL为中间体的反应途径可能参与了这一过程。呋喃在Pd/Al2O3上加氢和随后的C = O键在Ru/ZrO2上加氢的表观活化能分别约为21和30 kJ/mol。低活化能可以很好地解释…
The total hydrogenation of furfural (FAL) in aqueous solution was investigated under mild conditions over a series of a physical mixture of Pd- and Ru-supported catalysts. Monometallic catalysts showed unfulfilled selectivity toward total hydrogenation: supported Pd catalysts tend to give a mixture of tetrahydrofufural (THFAL), furfuryl alcohol (FA), and tetrahydrofurfuryl alcohol (THFA) while supported Ru catalysts are apt to hydrogenate the C═O bond. When supported Pd and Ru catalysts were mixed, the yield of THFA was significantly improved. A support-dependent promotion effect was noticed; in particular, Pd/Al2O3 and Ru/ZrO2 mixture gave 99% yield of THFA at 30 °C and 0.5 MPa H2. Detailed kinetics studies suggest that the reaction pathway with THFAL as the intermediate could be involved in this process. The apparent activation energy of furan hydrogenation over Pd/Al2O3 and the subsequent C═O bond hydrogenation over Ru/ZrO2 is about 21 and 30 kJ/mol, respectively. The low activation energies may well e...