Low temperature CO2 hydrogenation to alcohols and hydrocarbons over Mo2C supported metal catalysts

被引:112
作者
Chen, Yuan
Choi, Saemin
Thompson, Levi T. [1 ]
机构
[1] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
基金
美国国家科学基金会;
关键词
CO2; hydrogenation; Liquid phase reaction; Molybdenum carbide supported catalysts; Alcohol and hydrocarbon production; FISCHER-TROPSCH SYNTHESIS; GAS-SHIFT REACTION; CARBON-DIOXIDE HYDROGENATION; GROUP-VIII METALS; METHANOL SYNTHESIS; MOLYBDENUM; MECHANISM; CARBIDE; METHANATION; SELECTIVITY;
D O I
10.1016/j.jcat.2016.01.016
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 series of M/Mo2C (M = Cu, Pd, Co and Fe) were synthesized and evaluated for CO2 hydrogenation at 135-200 degrees C in liquid 1,4-dioxane solvent. The Mo2C served as both a support and a co-catalyst for CO2 hydrogenation, exhibiting turnover frequencies of 0.6 x 10(-4) and 20 x 10(-4) s(-1) at 135 and 200 degrees C, respectively. Methanol was the major product at 135 degrees C, while CH3OH, C2H5OH, and C2+ hydrocarbons were produced at 200 degrees C. The addition of Cu and Pd onto the high surface area Mo2C enhanced the production of CH3OH, while Co and Fe enhanced the production of C2+ hydrocarbons. Results for CO2, CO, and CH3OH hydrogenation experiments suggested that CO2 was the primary source for CH3OH while CO was the intermediate to hydrocarbons during CO2 hydrogenation. Characterization of the spent M/Mo2C catalysts revealed very little change in the surface and bulk chemistries and structures, indicating their stability in the liquid environment. (C) 2016 Elsevier Inc. All rights reserved.
引用
收藏
页码:147 / 156
页数:10
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