Stable Rh particles in hydrotalcite-derived catalysts coated on FeCrAlloy foams by electrosynthesis

被引:20
作者
Benito, Patricia [1 ]
Nuyts, Gert [2 ]
Monti, Marco [1 ]
De Nolf, Wout [2 ]
Fornasari, Giuseppe [1 ]
Janssens, Koen [2 ]
Scavetta, Erika [1 ]
Vaccari, Angelo [1 ]
机构
[1] Univ Bologna, Dipartimento Chim Ind Toso Montanari, I-40136 Bologna, Italy
[2] Univ Antwerp, Dept Chem, B-2020 Antwerp, Belgium
关键词
Electrosynthesis; Rh; Rh/Ni; FeCrAlloy; Catalytic partial oxidation of CH4; METHANE PARTIAL OXIDATION; CH4 PARTIAL OXIDATION; STRUCTURED CATALYSTS; CATHODIC ELECTRODEPOSITION; MODELING ANALYSIS; SYNTHESIS GAS; MONOLITH; REACTOR; TEMPERATURE; SYNGAS;
D O I
10.1016/j.apcatb.2015.05.035
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
Rh-based structured catalysts for the Catalytic Partial Oxidation of CH4 to syngas were prepared by electrosynthesis of Rh/Mg/Al hydrotalcite-type compounds on FeCrAlloy foams and calcination. The effects of Rh content, total metal concentration, and partial replacement of Mg2+ by Ni2+ in the electrolytic solution on coating thickness, Rh speciation, metallic particle size, and catalytic activity were investigated by SEM/EDS, mu-XRF/XANES and tests under diluted and concentrated reaction conditions. The amount of Rh species, present as Mg (RhxAl1-x)(2)O-4, depended on the thickness of the electrosynthesised layer as well as the Rh particle size and dispersion. Smaller and more dispersed particles were obtained by decreasing the Rh concentration in the electrolytic solution from Rh/Mg/Al=11/70/19 to 5/70/25 and 2/70/28 atomic ratio% (a.r.%) and in thinner rather than thicker layers. Despite the improvement in metallic particles features, the CH4 conversion was negatively affected by the low amount of active sites in the coating, the high metal support interaction and possibly the oxidation of metallic particles and carbon formation. A larger amount of solid containing well dispersed Rh particles was deposited by increasing the total metal concentration from 0.03 M to 0.06 M with the Rh/Mg/Al=5/70/25 a.r.%, and the catalytic performances were enhanced. The partial replacement of Mg2+ by Ni2+ gave rise to a very active bimetallic Rh/Ni catalyst, CH4 conversion and selectivity to syngas were above 90%, however, it slightly deactivated with time-on-stream. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:321 / 332
页数:12
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