Transition metal-containing MgFe ex-LDH mixed oxides, effective catalysts in the hydrodeoxygenation of benzyl alcohol

被引:5
|
作者
Toderasc, Alexandru-Tudor [1 ]
Atkinson, Irina [2 ]
Culita, Daniela Cristina [2 ]
Mereuta, Paul Emil [3 ]
Papa, Florica
Urda, Adriana [1 ,4 ]
Marcu, Ioan-Cezar [1 ,4 ]
机构
[1] Univ Bucharest, Fac Chem, Dept Inorgan & Organ Chem Biochem & Catalysis, Lab Chem Technol & Catalysis, 4-12 Blvd Regina Elisabeta, Bucharest 030018, Romania
[2] Romanian Acad, Ilie Murgulescu Inst Phys Chem, 202 Splaiul Independentei, Bucharest 060021, Romania
[3] Horia Hulubei Natl Inst Phys & Nucl Engn IFIN HH, 30 Reactorului, Magurele 077125, Ilfov, Romania
[4] Univ Bucharest, Fac Chem, Res Ctr Catalysts & Catalyt Proc, 4-12,Blvd Regina Elisabeta, Bucharest 030018, Romania
关键词
Mixed oxide; LDH; Copper; Hydrodeoxygenation; Reverse Mars-van Krevelen mechanism; Benzyl alcohol; LAYERED DOUBLE HYDROXIDE; SELECTIVE HYDRODEOXYGENATION; MODEL COMPOUNDS; LIGNIN; OXIDATION; HYDROGENATION; HYDROTALCITE; CONVERSION; BIOMASS; PHASE;
D O I
10.1016/j.apcata.2023.119063
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
Several M-MgFe-LDH precursors were prepared via co-precipitation and then calcined at 500 degrees C to yield the corresponding M-MgFeO mixed oxide catalysts, which were tested in the hydrodeoxygenation (HDO) of benzyl alcohol. The prepared LDH contained Mg and Fe in a mol ratio of 3:1 and 10 at% M with respect to cations, where M = Ni, Co, Ag and Cu. The Cu-MgFeO mixed oxide gave the best results, therefore we proceeded with the preparation of a Cu(x)-MgFeO series, where x = 2.5-20 at% Cu. The prepared solids were characterized by powder X-ray diffraction, nitrogen adsorption-desorption, temperature-programmed reduction with H2, temperature-programmed desorption of CO2 and energy dispersive X-ray spectroscopy. We studied the influence of the nature of the transition metal M on the activity and selectivity of the catalysts and, for the Cu-containing samples, the influence of Cu loading, reaction time and reaction temperature on their performance in the HDO reaction of benzyl alcohol. With 93.8% conversion and 93.8% selectivity towards toluene at 230 degrees C, 3 h reaction time and under a hydrogen pressure of 5 atm, the Cu(10)-MgFeO catalyst proved to have the best performance in the studied reaction. Therefore, its stability and reusability were checked. We also proposed a sequence of re-actions for the entire HDO process, based on a reverse Mars-van Krevelen mechanism driven by oxygen vacancies formed on the catalyst surface.
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页数:14
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