Ni-decorated carbon nanotube-promoted Ni-Mo-K catalyst for highly efficient synthesis of higher alcohols from syngas

被引:62
作者
Ma, Chun-Hui [1 ]
Li, Hai-Yan [1 ]
Lin, Guo-Dong [1 ]
Zhang, Hong-Bin [1 ,2 ,3 ]
机构
[1] Xiamen Univ, Dept Chem, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
[2] Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
[3] Xiamen Univ, Natl Engn Lab Green Chem Product Alcohols Ethers, Xiamen 361005, Peoples R China
关键词
Higher alcohol synthesis; Multi-walled carbon nanotubes; Ni-decorated MWCNTs; x% Ni/CNT-doped Ni-Mo-K catalyst; CU-ZNO-AL2O3; CATALYST; METHANOL SYNTHESIS; AMMONIA-SYNTHESIS; RAMAN-SPECTRA; SYNTHESIS GAS; CO; DECOMPOSITION; HYDROGEN; SPECTROSCOPY; NANOFIBERS;
D O I
10.1016/j.apcatb.2010.07.040
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
A type of metallic nickel-decorated CNT-doped Ni-Mo-K oxide-based catalysts was developed, with excellent performance for the selective formation of C1-3-alcohols from syngas. Under reaction condition of 8.0 MPa and 558 K. the space-time-yield of C1-3-alcohols plus dimethyl ether reached 555 mg h(-1) g(-1) over the Ni1Mo1K0.05-11% (5% Ni/CNT) catalyst. The addition of a minor amount of the Ni-decorated CNTs into the NiiMojKk host catalyst caused little change in the apparent activation energy for the higher alcohol synthesis (HAS), but led to the increase of the molar percentage of NiO(OH) and Mo4+/Mo5+ (the two kinds of catalytically active surface-species related closely to selective formation of C1-3-alcohols) and the dramatic decrease of the molar percentage of Ni-0 and Mo-0 (the two kinds of catalytically active surface-species related closely to selective formation of hydrocarbons, especially methanation of CO). An excellent adsorption performance of the Ni-decorated CNTs for H-2 would be conducive to generating a surface micro-environment with a high concentration of H-adspecies in the form of sp(2)-C-H on the functioning catalyst. In addition, high concentration of H-adspecies on the catalyst would greatly inhibit the water-gas-shift side-reaction. All these factors contribute to an increase in the yield of C1-3-alcohols. (C) 2010 Published by Elsevier B.V.
引用
收藏
页码:245 / 253
页数:9
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