Non-syngas direct steam reforming of methanol to hydrogen and carbon dioxide at low temperature

Yu, Kai; Tong, Weiyi; West, Adam H. C.; Cheung, Kevin; Li, Tong; Smith, George Davey; Guo, Yanglong; Tsang, Shik Chi Edman

doi:10.1038/ncomms2242

Cited by 134 publications

(67 citation statements)

References 17 publications

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“…There are many studies that support this assumption, and attribute the formation of CO to the RWGS due to the high concentrations of CO 2 and H 2 in the reaction medium [5,11,15,25].…”

Section: For Instance Peppley Et Al Has Reported a Kinetic Model Tmentioning

confidence: 99%

Low-temperature methanol steam reforming kinetics over a novel CuZrDyAl catalyst

Silva

Mateos-Pedrero

Ribeirinha

et al. 2015

Reac Kinet Mech Cat

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A kinetic study within the low-temperature methanol steam reforming (MSR) reaction range (170 ºC -200 ºC) was performed over a novel CuZrDyAl catalyst. The physicochemical and catalytic properties of the CuZrDyAl catalyst were compared with those of a conventional CuO/ZnO/Al 2 O 3 (G66 MR, Süd-Chemie) sample, taken as reference. The in-house catalyst displays better performances, in terms of methanol conversion and H 2 production, than the reference G66 MR sample.Interestingly, the in-house catalyst is significantly more selective (namely, yielding lower CO concentration) than the commercial one, which gives extra interest for producing fuel cell grade hydrogen. Physicochemical characterization evidences that the in-house catalyst have improved reducibility of copper species compared with the G66-MR, which might account for its better performances.The parameters of a simple power-law equation and two mechanistic kinetic models were determined by non-linear regression, minimizing the sum of the residual squares; the best fitting with the experimental data was obtained when using Model 3, based on the reported work from Peppley et al. [10] for the commercial CuO/ZnO/Al 2 O 3 .This article was published in Reaction Kinetics, Mechanisms and Catalysis, 115(1), 321-339, 2015 http://dx.doi.org/10.1007/s11144-015-0846-z 03-11-2017 2 Noteworthy, is the scarce number of MSR kinetic studies at such lower temperature range.

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“…There are many studies that support this assumption, and attribute the formation of CO to the RWGS due to the high concentrations of CO 2 and H 2 in the reaction medium [5,11,15,25].…”

Section: For Instance Peppley Et Al Has Reported a Kinetic Model Tmentioning

confidence: 99%

Low-temperature methanol steam reforming kinetics over a novel CuZrDyAl catalyst

Silva

Mateos-Pedrero

Ribeirinha

et al. 2015

Reac Kinet Mech Cat

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“…A catalyst able to work efficiently at lower temperatures is also cost-effective and desirable taking into consideration the integration between the endothermic MSR and exothermic PEMFC operation. Furthermore, low operating temperatures are beneficial for applications as power supplies for small portable devices, where heat and space management are of primary concern [12]. However, the development of a suitable catalytic system promoting both endothermic MSR and exothermic WGS at reasonably low temperatures (below 200 • C) remains a challenge.…”

Section: Introductionmentioning

confidence: 99%

“…Thus, several catalyst formulations were studied, such as binary compositions; Cu/ZnO, Cu/SiO2, Cu/CeO2 [4], commercially based Cu/ZnO/y-Al2O3 and its variations with added promoters; Cu/ZrO2/y-Al2O3, Cu/Cr/y-Al2O3 [2] or CuTiP/y-Al2O3 [6]. More recently CuZnGaOx [12] and CuZn catalyst promoted by rare earth metals such as Tb and Pr [14] were reported to have high activity at low temperature MSR. Nevertheless, Cu based catalysts have some considerable drawbacks which include pyrophoricity and easy deactivation due to thermal instability [7,15] or coke formation [13].…”

Section: Introductionmentioning

confidence: 99%

Ultraselective low temperature steam reforming of methanol over PdZn/ZnO catalysts—Influence of induced support defects on catalytic performance

Eblagon

Concepción

Silva

et al. 2014

Applied Catalysis B: Environmental

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The influence of the calcination atmosphere of ZnO precursor (Zn4(CO)3(OH)6·H2O) on the catalytic performance of a series of PdZn/ZnO catalysts was studied for production of H2 via low temperature (180 • C) direct methanol steam reforming (low temperature-MSR). The catalytic activity and selectivity of PdZn/ZnO were found to be strongly influenced by the calcination atmosphere of ZnO precursor and increased from oxidizing to reducing atmosphere, following the order (O2 < air < N2 < H2). As a result, a very active catalyst was obtained by simply supporting Pd on ZnO calcined in H2. Further evidence from XPS and TPR analysis indicated that calcination in reducing atmosphere gave rise to a significant increase in the concentration of oxygen vacancies on the surface of ZnO support. Thus, the superb performance of the best catalyst was attributed to the defect chemistry of ZnO support; mainly to the amount of oxygen vacancies present in the interface region, which act as additional active sites for water adsorption and subsequent activation. In addition, the formation of CO was drastically suppressed by replenishment of oxygen vacancies on ZnO support. Thus, it is clear that the abundance of specific active sites on PdZn/ZnO catalyst is strongly influenced by the preparation route of the ZnO support. Additionally, the PdZn alloy was discovered to be unstable under prolonged exposure to CO atmosphere and the stability test under methanol steam reforming conditions showed a 24% drop in conversion over 48 h testing period. This phenomena can have detrimental effect on the performance of this type of catalytic systems in continuous prolonged duty cycle time on-stream.

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“…However, the tendency of copper nanoparticles (NPs) to grow into larger crystallites through migration and coalescence of particles, or through the transport of monoatomic or molecular species between individual particles, is an impediment to stable performance 6,7 . Notably, the loss of active surface area by metal-particle growth is a major cause of deactivation for many supported catalysts.…”

mentioning

confidence: 99%

A copper-phyllosilicate core-sheath nanoreactor for carbon–oxygen hydrogenolysis reactions

et al. 2013

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Hydrogenolysis of carbon-oxygen bonds is a versatile synthetic tool in organic synthesis. Copper-based catalysts have been intensively explored as the copper sites account for the highly selective hydrogenation of carbon-oxygen bonds. However, the inherent drawback of conventional copper-based catalysts is the deactivation by metal-particle growth and unstable surface Cu 0 and Cu þ active species in the strongly reducing hydrogen and oxidizing carbon-oxygen atmosphere. Here we report the superior reactivity of a core (copper)-sheath (copper phyllosilicate) nanoreactor for carbon-oxygen hydrogenolysis of dimethyl oxalate with high efficiency (an ethanol yield of 91%) and steady performance (4300 h at 553 K). This nanoreactor, which possesses balanced and stable Cu 0 and Cu þ active species, confinement effects, an intrinsically high surface area of Cu 0 and Cu þ and a unique tunable tubular morphology, has potential applications in high-temperature hydrogenation reactions.

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Non-syngas direct steam reforming of methanol to hydrogen and carbon dioxide at low temperature

Cited by 134 publications

References 17 publications

Low-temperature methanol steam reforming kinetics over a novel CuZrDyAl catalyst

Low-temperature methanol steam reforming kinetics over a novel CuZrDyAl catalyst

Ultraselective low temperature steam reforming of methanol over PdZn/ZnO catalysts—Influence of induced support defects on catalytic performance

A copper-phyllosilicate core-sheath nanoreactor for carbon–oxygen hydrogenolysis reactions

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