Combined oxidation and reforming of methane to produce pure H2 in a membrane reactor

Múnera, John; Carrara, Carlos R.; Cornaglia, Laura María; Lombardo, E.A.

doi:10.1016/j.cej.2010.04.022

Cited by 25 publications

(19 citation statements)

References 24 publications

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“…In fact, CO 2 reacting with a more active species is often used in practice. For example, CO 2 has been used as a reforming reagent for methane in hydrogen production − as well as in methane and syngas production. − Direct synthesis of methanol from CO 2 and hydrogen (CO 2 + 3H 2 → CH 3 OH + H 2 O) is moderately endothermic, with a reaction enthalpy of 49.4 kJ/mol. In fact, CO 2 was commonly cofed with CO in methanol synthesis. − The versatility of methanol makes it an attractive target for practical application: it can be used as a fuel directly or as a commodity chemical to produce more valuable compounds.…”

Section: Introductionmentioning

confidence: 99%

DFT Study of CO₂Adsorption and Hydrogenation on the In₂O₃Surface

Liu

Ge³

2012

J. Phys. Chem. C

292

271

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Catalytic conversion of CO2 to liquid fuels or valuable chemicals is an attractive alternative to geological sequestration. In the present study, we applied density functional theory slab calculations in the investigation of the adsorption and hydrogenation of CO2 on the (110) surface of In2O3. Our results indicate that the adsorbed CO2 is activated, forming a surface carbonate species by combining with surface oxygen, and has an adsorption energy of −1.25 eV. Heterolytic dissociative adsorption of H2 results in a surface hydroxyl from H binding the surface O site and a hydride from H binding the In site. The migration of H from the In site to the neighboring O site is energetically favorable but has a significant activation barrier of 1.32 eV. Water may adsorb on the surface either molecularly or dissociatively, with adsorption energy of −0.83 eV and −1.19 eV, respectively. Starting from CO2 coadsorbed with the H adatoms on the In2O3 surface, we examined two possible conversion pathways for CO2: (a) CO2 is hydrogenated by the H adatom on the In site to form a surface formate species (HCOO); (b) CO2 is protonated by the H adatom on the O site to form a surface bicarbonate species (COOH). Reaction a is endothermic by +0.33 eV, whereas b is exothermic by −0.78 eV. Although the formation of the bicarbonate species is energetically favorable, the subsequent step to form CO and OH is highly endothermic, with a reaction energy of +1.07 eV. Furthermore, the bicarbonate species can react with a surface hydroxyl easily, resulting in coadsorbed H2O and CO2. These results indicate that hydrogenation of CO2 to the formate species is favorable over protonation to the bicarbonate species on the In2O3 surface. These results are consistent with the experimental observations that the indium oxide based catalyst has a high CO2 selectivity and H2O resistance.

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Section: Introductionmentioning

confidence: 99%

DFT Study of CO₂Adsorption and Hydrogenation on the In₂O₃Surface

Liu

Ge³

2012

J. Phys. Chem. C

292

271

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“…Several contributions have studied the combined reaction of methane in fixed-bed or fluidized-bed reactors with Ni [9][10][11] and Pt [12] catalysts. However, few experimental studies using methane reforming reactions and partial oxidation coupled in a membrane reactor can be found in the literature [13,14].…”

Section: Introductionmentioning

confidence: 99%

Ru/La2O3–SiO2 catalysts for hydrogen production in membrane reactors

2011

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“…In this case, hydrogen permeation decreases at higher SG flow rate. This behavior could be related to the change in the reaction atmosphere that takes place when hydrogen is extracted from the reactor, promoting the carbon formation and deactivation of the catalyst [40]. The results obtained with a H 2 O/Ethanol molar ratio of 10 suggest that part of the water excess dilutes the hydrogen produced in the reaction zone resulting in a lower hydrogen partial pressure difference between both sides of the membrane.…”

Section: Comparison Between Rh-based Catalystsmentioning

confidence: 81%