期刊
APPLIED CATALYSIS A-GENERAL
卷 451, 期 -, 页码 28-35出版社
ELSEVIER
DOI: 10.1016/j.apcata.2012.10.038
关键词
Pd-decorated CNTs; Pd-decorated CNT-promoted; Cu-ZrO2/HZSM-5 hybrid catalysts; CO2 hydrogenation; Direct DME synthesis
资金
- 973 project [2011CBA00508]
- NSFC project [20923004]
- PCSIRT [IRT1036]
- Fujian Provincial Key Scientific Projects of China [2009HZ0002-1]
A type of bi-functional hybrid catalyst of Pd-decorated CNT-promoted Cu-ZrO2 admixed with HZSM-5 zeolite was developed, and displayed excellent performance for the direct synthesis of dimethyl ether (DME) from CO2/H-2 via CH3OH in a single fixed-bed continuous flow reactor. Over a CuZr-PdCNTs/HZSM-5 hybrid catalyst under reaction conditions of 5.0 MPa, 523 K, V(H-2)/V(CO2)/V(N-2) = 69/23/8, GHSV = 25,000 mL(STP)/(h g-hydr. catal.), the observed specific rate of CO2 hydrogenation-conversion reached 0.39 mu mol/(s m(2)-Cu-0-SA), which was 1.22 times that of the corresponding Pd/CNTs-free counterpart CuZr/HZSM-5. The addition of a minor amount of the Pd-decorated CNTs into the CuZr/HZSM-5 host catalyst caused little change in the apparent activation energy for CO2 hydrogenation, but led to an increase of metal Cu exposed area (catalytically active Cu surface-sites closely associated with the CO2 hydrogenation to methanol) and marked improvement of adsorption performance of the catalyst for H-2 and CO2. The latter would help generate a micro-environment with higher concentration of active H and CO2 adspecies at the surface of the functioning catalyst, thus increasing the rate of the surface hydrogenation reactions. The present study also demonstrated that combining the methanol-synthesis and methanol-dehydration-to-DME processes in heterogeneous one-pot reactions by using the bifunctional hybrid catalyst could indeed enhance the driving force for CO2 hydrogenation conversion. (C) 2012 Elsevier B.V. All rights reserved.
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