H2 production by selective photo-dehydrogenation of ethanol in gas and liquid phase on CuOx/TiO2 nanocomposites

被引:76
作者
Ampelli, Claudio [1 ,2 ]
Passalacqua, Rosalba [1 ,2 ]
Genovese, Chiara [1 ,2 ]
Perathoner, Siglinda [1 ,2 ]
Centi, Gabriele [1 ,2 ]
Montini, Tiziano [3 ,4 ]
Gombac, Valentina [3 ,4 ]
Delgado Jaen, Juan Jose [5 ]
Fornasiero, Paolo [3 ,4 ]
机构
[1] Univ Messina, Dipartimento Ingn Elettr Chim & Ingn Ind, I-98166 Messina, Italy
[2] INSTM CASPE, Lab Catalysis Sustainable Prod & Energy, I-98166 Messina, Italy
[3] Univ Trieste, Dipartimento Sci Chim & Farmaceut, ICCOM CNR, I-34127 Trieste, Italy
[4] INSTM, I-34127 Trieste, Italy
[5] Univ Cadiz, Fac Ciencias, Dept Ciencia Mat & Ingn Met & Quim Inorgan, Cadiz 11510, Spain
关键词
PHOTOCATALYTIC HYDROGEN-PRODUCTION; TIO2; REACTOR; COPPER; GLYCEROL; METHANOL; ADSORPTION; CONVERSION; CU2O/TIO2; MECHANISM;
D O I
10.1039/c3ra22804e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
CuOx/TiO2 nanocomposites prepared by copper photodeposition (1.0 and 2.5 wt% copper loading) on TiO2 (synthesized by three different routes) are studied in the ethanol photo-dehydrogenation in gas- and liquid-phase operations, and characterized in terms of surface area, phase composition by XRD, morphology and copper-oxide nanoparticle size distribution, and copper species by UV-visible diffuse reflectance spectroscopy. Cu2+ ions partially enter into the titania structure leading to the creation of oxygen vacancies responsible for the shift in the band gap, but also the creation of traps for photogenerated holes and electrons. While the band gap shifts to lower energies with the copper content, a maximum photocatalytic activity is shown for the intermediate copper loading. Gas-phase operations allow a higher H-2 productivity with respect to liquid-phase operations, and especially a higher selectivity (about 92-93%) to acetaldehyde. It is remarked that the route of photo-dehydrogenation of ethanol to H-2 and acetaldehyde has an economic value about 3.0-3.5 times higher than the alternative route of photoreforming to produce H-2. Gas-phase operations would be preferable for the photo-dehydrogenation of ethanol.
引用
收藏
页码:21776 / 21788
页数:13
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