Methanol steam reforming behavior of copper impregnated over CeO 2 –ZrO 2  derived from a surfactant assisted coprecipitation route

Das, Dipak K.; Llorca, Jordi; Domínguez, Montserrat; Colussi, Sara; Trovarelli, Alessandro; Gayen, Arup

doi:10.1016/j.ijhydene.2015.06.130

Cited by 78 publications

(32 citation statements)

References 58 publications

(69 reference statements)

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“…520 K. In case of mixed ceria-zirconia solid solutions (e.g., 0.2CeZr, 0.5CeZr, and 0.8CeZr in this work), this peak is splitted into two peaks towards low temperatures (denoted as Tr1 and Tr2 for low-and high-temperature peaks). From literature [22][23][24][25], the peaks observed at Tr1 and Tr2 are ascribed to the reduction of highly dispersed CuO species strongly interacting with the support and the reduction of segregated CuO crystalline particles, respectively. The shift to low temperatures and the difference between Tr1 and Tr2 becomes larger as the x value increases from 0.2 to 0.8.…”

Section: Catalyst Characterization Resultsmentioning

confidence: 98%

Cross-Aldol Condensation of Acetone and n-Butanol into Aliphatic Ketones over Supported Cu Catalysts on Ceria-Zirconia

et al. 2017

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Abstract:A long-chain hydrocarbon biofuel of jet fuel range can be produced via aldol condensation of fermented products such as acetone and alcohols over the catalysts containing both metallic sites for the dehydrogenation of alcohols and basic sites for the condensation reaction. However, an efficient catalyst system has not been studied widely yet the route is promising for biofuel production. In this work, Cu catalysts supported on ceria-zirconia (Cu/xCeZr) were prepared using coprecipitated Ce x Zr 1-x O 2 supports with different Ce/Zr ratios for the cross-aldol condensation of acetone and n-butanol into mono-and di-alkylated aliphatic ketones, 2-heptanone and 6-undecanone. The acetone conversion and 6-undecanone selectivity increased with specific Cu surface area due to formation of the dehydrogenation product butyraldehyde at a higher concentration. The total yield of cross-aldol condensation products was strongly dependent on a combination of Cu sites and basic sites. This was confirmed by the results in the reaction between acetone and butyraldehyde over supported Cu catalysts that additionally examined the adsorbed acyl species on Cu surface taking part in the aldol condensation reaction. The best catalytic performance was achieved with Cu/0.8CeZr showing the largest Cu surface and the highest base site density among Cu/xCeZr catalysts. While the activity of Cu/0.8CeZ was comparable to or a little higher than that of Cu/MgO, the former catalyst was more stable than the latter suffering from the transformation of MgO to Mg(OH) 2 by the reaction. Consequently, it is suggested that Cu supported on ceria-zirconia of ceria rich contains such a dual function that it can efficiently catalyze the cross-aldol condensation of acetone and n-butanol.

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Section: Catalyst Characterization Resultsmentioning

confidence: 98%

Cross-Aldol Condensation of Acetone and n-Butanol into Aliphatic Ketones over Supported Cu Catalysts on Ceria-Zirconia

et al. 2017

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“…To investigate the stability and reusability of the CCTO samples we have studied the MSR reaction at 533 K (when the conversion is close to the maximum achievable methanol conversion) keeping other reaction parameters unchanged and the TOS behavior is shown in Figure (b). It can be observed that initially the fresh/as‐prepared (AP) CCTO sample registers a good activity showing 68% methanol conversion that decreased steadily to 34% after 13 h. The Cu‐based catalysts generally suffer a loss of conversion with TOS and the present CCTO system is no exception . Our interest was then to see if the same material can be used repeatedly by introducing an intermediate regeneration step through oxidation in air (catalyst named as “Regn”).…”

Section: Resultsmentioning

confidence: 99%

Synthesis, Characterization and Catalytic Activity of Quadruple Perovskite: CaCu_3‐xMn_xTi_4‐xMn_xO₁₂ (x=0, 0.5 and 1.0)

et al. 2018

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We report the low temperature synthesis of nanosized CaCu 3-x Mn x Ti 4-x Mn x O 12 (x = 0, 0.5 and 1.0) quadruple perovskites and their magnetic, dielectric and catalytic performance towards CO oxidation and methanol steam reforming (MSR). Our investigations reveal the pronounced effects of particle size and chemical substitution on all the physical properties reported here. The manganese doped samples exhibit remarkable change in magnetic properties, where antiferromagnetic pristine phase converted to ferrimagnetic phase for x = 1. The dielectric constant values of the cold-pressed nanosized perovskites are~10 3 and follows Maxwell-Wagner type relaxation. This value is about 100 fold lower than that of the bulk samples that has been ascribed to the effect of particle size and the absence of nano-twinning in the material as revealed from HRTEM studies. The doping of manganese further reduces the magnitude of dielectric value, which is the chemical effect. Mndoped samples show greater catalytic activity compared to the pristine sample towards CO oxidation due to a synergistic CuÀMn interaction. The catalytic performance of these oxides for MSR reaction is intriguing. Although the catalyst undergoes decomposition in the MSR atmosphere causing a decrease in methanol conversion during time-on-stream (TOS) tests, the activity can be regenerated by in-situ or ex-situ annealing in air. The notable catalytic activity and reversibility between pristine and decomposed form are very interesting.

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“…We have also calculated the TOF values of the as-prepared and aged samples of Cu10CZ80 by considering the surface concentration of copper from XPS and Cu particle size from HRTEM as reported recently. 25 The TOF values of the As a complementary chemical characterization tool, we have also conducted electron energy loss spectroscopy (EELS) measurements over the Ce-Zr crystallites to check for the presence of substitutional Cu in the Cu10CZ80 catalyst in its as-prepared form. In all cases, the signals of Cu were absent, suggesting that the Ce-Zr crystallites do not contain Cu at all in their structure.…”

Section: Xrd Studiesmentioning

confidence: 99%

“…23,24 In a very recent report, we have studied the MSR behavior of copper impregnated over various Ce-Zr oxides. 25 Single step combustion synthesized Cu/ Ce 0. 8 In this work, we report the synthesis of Cu (5-15 at.…”

Section: Introductionmentioning

confidence: 99%

Single step combustion synthesized Cu/Ce_0.8Zr_0.2O₂for methanol steam reforming: structural insights fromin situXPS and HRTEM studies

Das

Llorca

Domínguez

et al. 2015

Catalysis, Structure & Reactivity

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Methanol steam reforming behavior of copper impregnated over CeO 2 –ZrO 2 derived from a surfactant assisted coprecipitation route

Cited by 78 publications

References 58 publications

Cross-Aldol Condensation of Acetone and n-Butanol into Aliphatic Ketones over Supported Cu Catalysts on Ceria-Zirconia

Cross-Aldol Condensation of Acetone and n-Butanol into Aliphatic Ketones over Supported Cu Catalysts on Ceria-Zirconia

Synthesis, Characterization and Catalytic Activity of Quadruple Perovskite: CaCu_3‐xMn_xTi_4‐xMn_xO₁₂ (x=0, 0.5 and 1.0)

Single step combustion synthesized Cu/Ce_0.8Zr_0.2O₂for methanol steam reforming: structural insights fromin situXPS and HRTEM studies

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Methanol steam reforming behavior of copper impregnated over CeO 2 –ZrO 2 derived from a surfactant assisted coprecipitation route

Cited by 78 publications

References 58 publications

Cross-Aldol Condensation of Acetone and n-Butanol into Aliphatic Ketones over Supported Cu Catalysts on Ceria-Zirconia

Cross-Aldol Condensation of Acetone and n-Butanol into Aliphatic Ketones over Supported Cu Catalysts on Ceria-Zirconia

Synthesis, Characterization and Catalytic Activity of Quadruple Perovskite: CaCu3‐xMnxTi4‐xMnxO12 (x=0, 0.5 and 1.0)

Single step combustion synthesized Cu/Ce0.8Zr0.2O2for methanol steam reforming: structural insights fromin situXPS and HRTEM studies

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Synthesis, Characterization and Catalytic Activity of Quadruple Perovskite: CaCu_3‐xMn_xTi_4‐xMn_xO₁₂ (x=0, 0.5 and 1.0)

Single step combustion synthesized Cu/Ce_0.8Zr_0.2O₂for methanol steam reforming: structural insights fromin situXPS and HRTEM studies