Synergistic Catalysis between Pd and Fe in Gas Phase Hydrodeoxygenation of m-Cresol

被引:181
作者
Hong, Yongchun [1 ,2 ,3 ]
Zhang, He [1 ]
Sun, Junming [1 ]
Ayman, Karim M. [2 ]
Hensley, Alyssa J. R. [1 ]
Gu, Meng [3 ]
Engelhard, Mark H. [3 ]
McEwen, Jean-Sabin [1 ,4 ]
Wang, Yong [1 ,2 ]
机构
[1] Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn, Pullman, WA 99164 USA
[2] Pacific NW Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA
[3] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA
[4] Washington State Univ, Dept Chem, Pullman, WA 99164 USA
来源
ACS CATALYSIS | 2014年 / 4卷 / 10期
关键词
hydrodeoxygenation; biomass conversion; bimetallic catalysis; synergistic effects; iron catalyst; noble metal catalysis; H-2 sticking probability; BIMETALLIC NANOPARTICLE CATALYSTS; SULFIDE PARTIAL-PRESSURE; AB-INITIO; DISSOCIATIVE ADSORPTION; HYDROGENATION; GUAIACOL; AU; PHENOLS; LIGNIN; GOLD;
D O I
10.1021/cs500578g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this work, a series of Pd/Fe2O3 catalysts were synthesized, characterized, and evaluated for the hydrodeoxygenation (HDO) of m-cresol. It was found that the addition of Pd remarkably promotes the catalytic activity of Fe while the product distributions resemble that of monometallic Fe catalyst, showing high selectivity toward the production of toluene (C-O cleavage without saturation of aromatic ring and C-C cleavage). Reduced catalysts featured with Pd patches on the top of reduced Fe nanoparticle surface, and the interaction between Pd and Fe, was further confirmed using X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), and X-ray absorption near edge fine structure (XANES). A possible mechanism, including Pd assisted H-2 dissociation and Pd facilitated stabilization of the metallic Fe surface as well as Pd enhanced product desorption, is proposed to be responsible for the high activity and HDO selectivity in Pd-Fe catalysts. The synergic catalysis derived from Pd Fe interaction found in this work was proved to be applicable to other precious metal promoted Fe catalysts, providing a promising strategy for future design of highly active and selective HDO catalysts.
引用
收藏
页码:3335 / 3345
页数:11
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