Mechanistic insights into methanol steam reforming over a ZnZr oxide catalyst with improved activity

被引:10
作者
Wei, Jinxing [1 ]
Liu, Tangkang [1 ]
Wang, Yanqiu [1 ]
Jing, Dengwei [2 ]
Hong, Xinlin [1 ]
Liu, Guoliang [1 ]
机构
[1] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China
[2] Xi An Jiao Tong Univ, Int Res Ctr Renewable Energy, State Key Lab Multiphase Flow Power Engn, Xian 710049, Shaanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
Hydrogen production; Methanol steam reforming; MSR mechanism; Composite oxide catalyst; Synergistic effect; GAS SHIFT REACTION; HYDROGEN-PRODUCTION; MOLYBDENUM CARBIDE; METHYL FORMATE; SURFACE; WATER; ENERGY; ZNO; DECOMPOSITION; ADSORPTION;
D O I
10.1016/j.ijhydene.2022.08.062
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
Methanol steam reforming (MSR) holds great potential for mobile hydrogen production, but it still requires an active and stable catalyst. In this work, we report a high-performance ZnZr-0.5 composite oxide catalyst for this reaction, with a hydrogen production rate of 2.80 mol center dot gcat -1 center dot h-1 and CO2 selectivity of 99.6% at a methanol space velocity of 22,762 mL center dot gcat -1 center dot h-1. It also exhibits superior long-term durability in the TOS test for more than 100 h. Such good activity results from a synergistic effect of ZnO-ZrO2 dual sites. ZrO2 is capable of stabilizing and storing more CH3O* and HCOO* intermediates while ZnO is in charge of the dehydrogenation of these key intermediates. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and chemisorption results reveal that the MSR reaction experiences successively the hydrolysis of methyl formate and dehydrogenation of formate. More importantly, it is found that H2O significantly promotes the dehydrogenation of HCOO* intermediate by directly participating in this reaction from pulse chemisorption experiments. (c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:34312 / 34322
页数:11
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