Steam reforming of ethanol over Ni/MgAl2O4 catalysts

被引:64
|
作者
Di Michele, Alessandro [1 ]
Dell'Angelo, Anna [2 ,3 ]
Tripodi, Antonio [2 ,3 ]
Bahadori, Elnaz [2 ,3 ]
Sanchez, Felipe [4 ]
Motta, Davide [4 ]
Dimitratos, Nikolaos [4 ]
Rossetti, Ilenia [2 ,3 ]
Ramis, Gianguido [5 ,6 ]
机构
[1] Univ Perugia, Dip Fis & Geol, Via Pascoli, I-06123 Perugia, Italy
[2] Univ Milan, INSTM Unit Milano Univ, Chem Plants & Ind Chem Grp, Dip Chim, Via C Golgi 19, I-20133 Milan, Italy
[3] CNR ISTM, Via C Golgi 19, I-20133 Milan, Italy
[4] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales
[5] Univ Genoa, Dip Ingn Civile Chim & Ambientale, Via All Opera Pia 15A, Genoa, Italy
[6] INSTM Unit Genova, Via All Opera Pia 15A, Genoa, Italy
关键词
Hydrogen; Ethylene; Ni catalysts; Bioethanol conversion to chemicals; Steam reforming; NI CRYSTAL SIZE; HYDROGEN-PRODUCTION; SUPPORTED CATALYSTS; OXIDATION; METAL; FUEL; BIOETHANOL; GENERATION; STABILITY; GLYCEROL;
D O I
10.1016/j.ijhydene.2018.11.048
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
Hydrogen is considered one of the most promising energy vectors in order to match the current energy and environmental issues. Bioethanol steam reforming is a sound opportunity and close to the industrialization considering an integrated biorefinery concept. MgAl2O4 was selected as a stable support, with improved activity, selectivity and stability due to negligible acidity. Increasing the Ni loading from 1.5 to 10 wt% over MgAl2O4 improved the conversion of ethanol as well as the yield of hydrogen, while the carbon deposition and yield of byproducts decreased. Small acidity characterised the samples, attributed exclusively to the Ni active phase. This prevented extensive catalyst coking due to ethylene formation and subsequent polymerisation. Consequently, small coke amount was found on the spent catalysts, mainly amorphous, allowing rather easy regeneration. DRIFT analysis of adsorbed ethanol at variable temperature evidenced the intermediates of reaction and their evolution with temperature, allowing to suggest the main reaction paths. Acetaldehyde was found as intermediate, rapidly evolving to reformate. Among the possible evolution paths of acetaldehyde, the oxidation to acetate and carbonate species (likely stabilised by the support) was preferred with respect to decomposition to methane and CO. This is reflected in the products distribution evidenced through activity testing. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:952 / 964
页数:13
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