Hydrogen production by methanol steam reforming: Catalytic performance of supported-Pd on zinc–cerium oxides’ nanocomposites

Barrios, Celina; Bosco, Marta V.; Baltanás, Miguel Angel; Bonivardi, Adrian Lionel

doi:10.1016/j.apcatb.2015.05.030

Cited by 54 publications

(36 citation statements)

References 53 publications

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“…[5][6][7][8] Commercially available copper-based catalysts( Cu/ZnOa nd Cu/ZnO/Al 2 O 3 )h ave been widely used for hydrogen production from methanol, whereas experimental studies have also included group 8-10 metal-based catalysts supported mainly on ZnO and CeO 2 . [51][52][53][54][55][56][57][58][59][60][61][62][63][64] Regardingt he former catalysts,the presence of highly dispersed reduced copper species together with stable redox behavioru nder methanol reforming conditions are key requirements for the achievemento f high activitya nd low CO selectivity.N evertheless,c ommercial CuZn(Al)O x catalysts have not been designed for portable energy applications,a nd apart from commont hermal sintering, their main drawback pertains to pyrophoricity phenomena, which appear when the used catalyst is exposed to air. Rapid re-oxidation of the metallic copper species takes place to al arge extent (sometimes autoignition might occur), thus resulting in sintering of copper nanoparticles and irreversiblec atalyst deactivation.…”

Section: Introductionmentioning

confidence: 99%

Redox Behavior of a Copper‐Based Methanol Reformer for Fuel Cell Applications

Słowik

Avgouropoulos

2018

Energy Tech

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Remarkable cycling performance and operation during steam reforming of methanol at 210 °C can be obtained with a CuZnAlOx catalyst supported on the gas diffusion layer of a carbon paper incorporated into the fuel cell anode compartment. Exceptional stability is obtained for at least 100 h under reaction conditions, whereas 10–15 % deactivation is obtained afterwards, in accordance with typical behavior for copper‐based catalysts. Despite that most catalysts of this type suffer from pyrophoricity and sintering phenomena after exposure in air, this is not the case in the present work, where the proposed methanol reformer shows high tolerance under repeated on/off cycles. In accordance with in situ characterization under similar conditions, controlled passivation during shut‐down protects the active metallic copper and prevents undesirable sintering.

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Section: Introductionmentioning

confidence: 99%

Redox Behavior of a Copper‐Based Methanol Reformer for Fuel Cell Applications

Słowik

Avgouropoulos

2018

Energy Tech

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“…Barrios et al [69] tested the performances of Pd/CeO2 and Pd/ZnO/CeO2 catalysts for methanol steam reforming. Pd/CeO2 can only decompose methanol to CO at the reforming temperature of 250 °C and the steam to carbon ratio of 1.…”

Section: Performances Of Palladium Based Catalystsmentioning

confidence: 99%

Review on Copper and Palladium Based Catalysts for Methanol Steam Reforming to Produce Hydrogen

Shuai

2017

Catalysts

109

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Abstract:Methanol steam reforming is a promising technology for producing hydrogen for onboard fuel cell applications. The methanol conversion rate and the contents of hydrogen, carbon monoxide and carbon dioxide in the reformate, significantly depend on the reforming catalyst. Copper-based catalysts and palladium-based catalysts can effectively convert methanol into hydrogen and carbon dioxide. Copper and palladium-based catalysts with different formulations and compositions have been thoroughly investigated in the literature. This work summarized the development of the two groups of catalysts for methanol steam reforming. Interactions between the activity components and the supports as well as the effects of different promoters were discussed. Compositional and morphological characteristics, along with the methanol steam reforming performances of different Cu/ZnO and Pd/ZnO catalysts promoted by Al 2 O 3 , CeO 2 , ZrO 2 or other metal oxides, were reviewed and compared. Moreover, the reaction mechanism of methanol steam reforming over the copper based and palladium based catalysts were discussed.

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“…Moreover, the active role of ceria in the important watergas-shift (WGS, CO + H 2 O −→ CO 2 + H 2 ) and steam reforming of alcohols reactions for hydrogen production, in particular methanol (MSR, CH 3 OH + H 2 O −→ CO 2 + 3 H 2 ), has been widely reported. [9][10][11][12][13][14][15][16][17] The possibility of understanding the mechanism of catalytic reactions, which is essential for rational catalyst design, depends very much on the chances of isolating intermediates in the study of each step in the catalytic cycle. It has been argued that formate (HCOO) transient species might be playing intermediate or spectactor roles during WGS [18][19][20][21][22][23] and MSR 24 or its reverse reaction, [25][26][27][28] that is, the methanol synthesis from carbon oxides.…”

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confidence: 99%

Insights into the Nature of Formate Species in the Decomposition and Reaction of Methanol over Cerium Oxide Surfaces: A Combined Infrared Spectroscopy and Density Functional Theory Study

et al. 2015

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Formation of formate species on oxide surfaces plays a role in reactions for hydrogen production such as the water-gas shift, and the steam reforming of alcohols. It has been suggested that bridge formates are the most common and stable configuration on metal oxides. Ceria-based catalysts are important for these reactions where ceria is a "noninnocent" support. In this work, the nature of the formate species that are formed during decomposition and reaction of methanol on ceria surfaces have been studied using a combination of infrared temperature programmed surface reaction (TPSR-IR) on a real powder catalyst support, and density functional theory (DFT) together with statistical thermodynamics for model CeO 2 (111) surfaces. The influence of surface oxygen vacancies, hydroxyl groups, and water has been considered. Three different formate species have been identified (450 − 550 K). Initially, formates are adsorbed on the oxidized surface that is gradually hydroxylated by the release of hydrogen from methoxy groups (> 500 K), which leads to a partially reduced surface. On the former one kind of species is observed, whereas on the latter the other two kinds appeared. We provide computational evidence that the bonding is only initially of the bridge type, but becomes of the monodentate type, as the surface concentration of hydroxyl groups rises.The calculated frequencies of the O−C−O symmetric and asymmetric stretching modes for the three structures are in good agreement with those experimentally observed. The existence of monodentate species is discussed in terms of a stabilizing effect of hydrogen bonds. The combined experimental and theoretical results on real and model systems, respectively, thus provide important insights on the reaction of methanol on ceria surfaces.

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Hydrogen production by methanol steam reforming: Catalytic performance of supported-Pd on zinc–cerium oxides’ nanocomposites

Cited by 54 publications

References 53 publications

Redox Behavior of a Copper‐Based Methanol Reformer for Fuel Cell Applications

Redox Behavior of a Copper‐Based Methanol Reformer for Fuel Cell Applications

Review on Copper and Palladium Based Catalysts for Methanol Steam Reforming to Produce Hydrogen

Insights into the Nature of Formate Species in the Decomposition and Reaction of Methanol over Cerium Oxide Surfaces: A Combined Infrared Spectroscopy and Density Functional Theory Study

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