Synthesis of stable Cu-MCM-41 nanocatalysts for H2 production with high selectivity via steam reforming of methanol

被引:86
作者
Deshmane, Vishwanath G. [1 ,2 ]
Abrokwah, Richard Y. [3 ]
Kuila, Debasish [1 ]
机构
[1] North Carolina Agr & Tech State Univ, Dept Chem, Greensboro, NC 27411 USA
[2] North Carolina Agr & Tech State Univ, Dept Chem Biol & Bioengn, Greensboro, NC 27411 USA
[3] North Carolina Agr & Tech State Univ, Dept Energy & Environm Syst, Greensboro, NC 27411 USA
基金
美国国家科学基金会;
关键词
Steam reforming; Cu-MCM-41; Metal loading; One-pot synthesis; Catalyst deactivation; N2O chemisorption; TEMPERATURE-PROGRAMMED REDUCTION; MESOPOROUS MOLECULAR-SIEVES; HYDROGEN-PRODUCTION; EFFICIENT CATALYST; COPPER CATALYST; OXIDATION; PERFORMANCE; CU/MCM-41; ETHANOL; MCM-41;
D O I
10.1016/j.ijhydene.2015.06.084
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
High surface area MCM-41 containing copper catalysts (with different loading from 5 to 20 wt%) were synthesized using one-pot procedure for steam reforming of methanol (SRM) studies. A variety of techniques including BET, XRD, TGA-DSC, TEM, EDX, ICP-OES, H-2-TPR, N2O chemisorption and EPR were used to characterize the physical and chemical properties of catalysts. Structural characterization by means of XRD and BET revealed that %Cu loading has a strong influence on the ordered structure and the textural properties of the Cu-MCM-41 catalysts. The BET surface area of MCM-41 decreased from 1039 to 662 m(2)/g with increase in Cu loading from 0 to 15 wt% and then dropped to 314 m(2)/g with the loss of ordered structure at 20 wt% loading. The chemical composition analyses of catalysts using ICP-OES and EDX showed that the intended amount of copper was successfully retained in MCM-41 during one pot synthesis. Steam reforming of methanol for hydrogen production was carried out in a fixed bed reactor at atmospheric pressure in the temperature range of 200-350 degrees C. The effect of %Cu loading, reaction temperature, CH3OH/H2O molar ratio, reactants space velocity, catalyst time on-stream on the catalytic activity and selectivity were investigated. The Cu-MCM-41 samples showed excellent catalytic performance for the SRM reactions. The best results were obtained with 15%Cu-MCM-41 which showed similar to 89% methanol conversion, 100% H-2 selectivity and CO selectivity of 0.8% at 300 degrees C and 2838 h(-1) GHSV. However, methanol conversion decreased to about 77% when the loading of Cu was increased to 20 wt%. This can be attributed to more than 50% decrease in catalyst surface area leading to decrease in Cu-dispersion. The catalyst with 15 wt% loading showed strong resistance to deactivation and maintained consistent performance over a time on-stream for 48 h, indicating that the use of high surface area MCM-41 support significantly enhanced the stability of Cu-based catalyst. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:10439 / 10452
页数:14
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