Co-production of hydrogen and acetaldehyde from ethanol over a highly dispersed Cu catalyst

Liu, Haolan; Jiang, Yuanyuan; Zhou, Ruru; Chang, Zhili; Hou, Zhenshan

doi:10.1016/j.fuel.2022.123980

Cited by 19 publications

(14 citation statements)

References 54 publications

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“…43 Additionally, the encapsulated catalyst of (Cu/ MFI)@MFI showed higher acetaldehyde productivities than Cu/MFI catalysts based on normalized Cu loadings, confirming the robust activity of encapsulated and unsaturated Cu species (Figure S4). 23 The ethanol conversion and product distribution at 523 K and a WHSV of 0.53 h −1 were analyzed in detail for Cu/MFI catalysts before and after encapsulation. As shown in Figure 4C, the selectivity to acetaldehyde was 68.1% at 98.7% ethanol conversion over the pristine Cu/MFI catalyst, coproducing large amounts of ethylene, ethyl acetate, butyraldehyde, and dioxane (Figure S5) due to the presence of abundant Lewis acid sites on the catalyst (Figure S6).…”

Section: Resultsmentioning

confidence: 99%

“…Among these, copper (Cu)-based catalysts demonstrate unique activity and selectivity in O–H and C–H bond cleavages. − Nevertheless, Cu-based catalysts are prone to be deactivated because of particle aggregation, carbon deposition, or catalyst crushing. Under most hydrogen-involved reactions, the leading reason for catalyst deactivation is aggregation of Cu nanoparticles via Ostwald ripening or migration–coalescence processes due to the low Tammann temperature of Cu. − To suppress the deactivation of catalysts, some strategies including strong metal and support interactions, alloys and space confinements have been applied to stabilize Cu particles and achieved great successes. − For instance, in our previous work, Cu-MFI-AE catalysts were prepared via an ammonia evaporation method, which generated strong interactions between the metal and support. As a result, the catalyst demonstrated distinguished acetaldehyde selectivity and very high catalyst stability in the ethanol dehydrogenation reaction .…”

Section: Introductionmentioning

confidence: 99%

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Redispersion and Stabilization of Cu/MFI Catalysts by the Encapsulation Method for Ethanol Dehydrogenation

Pang

Yin

et al. 2023

ACS Sustainable Chem. Eng.

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Encapsulation of metal particles with ordered porous zeolite is a promising method to stabilize nanoparticles. In this work, Cu/MFI catalysts prepared by the impregnation method were encapsulated with MFI to yield (Cu/MFI)@MFI catalysts for ethanol dehydrogenation. The encapsulation process not only anchored Cu particles into MFI but also redispersed Cu with decreased particle sizes and newly formed Cu + species. During the ethanol dehydrogenation reaction, the Cu + and Cu 0 species confined in (Cu/MFI)@MFI catalysts demonstrated synergistic effects and afforded 95.7% acetaldehyde selectivity, 97.2% ethanol conversion at 523 K, and a weight hourly space velocity (WHSV) of 0.53 h −1 in the 200 h time on stream over the optimized (Cu/MFI)@MFI 100% catalyst, which is significantly better than the counterpart of the Cu/MFI catalyst.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Redispersion and Stabilization of Cu/MFI Catalysts by the Encapsulation Method for Ethanol Dehydrogenation

Pang

Yin

et al. 2023

ACS Sustainable Chem. Eng.

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“…Temperature-programmed desorption of O 2 and NH 3 from Pt/AC and PtSb 2 /AC catalysts was carried out according to the procedures in the literature, − and these experiments are addressed in detail in the Supporting Information.…”

Section: Methodsmentioning

confidence: 99%

Selective Oxidation of 1,3-Butanediol to 3-Hydroxybutyric Acid over PtSb₂ Alloy

Zhong

Liu

Zhou

et al. 2022

ACS Sustainable Chem. Eng.

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3-Hydroxybutyric acid (3-HBA) is an important monomer for manufacturing biodegradable polymers such as polyhydroxyalkanoates, which are currently produced via an expensive and time-consuming microbial fermentation route. Herein, the catalytic synthesis of 3-HBA via the selective oxidation of 1,3-butanediol (1,3-BDO) in the presence of molecular oxygen is reported for the first time. It was found that the PtSb2 alloy could catalyze the selective formation of 3-HBA, and the selectivity of 3-HBA was 82.3% at a 1,3-BDO conversion level of 95.5%. The calculated turnover frequency of each surface Pt atom in the PtSb2/AC catalyst was 344.3 h–1 at 70 °C. The characterization results indicated that the prominent performance of the PtSb2 alloy over monometallic Pt nanoparticles could be because the alloy could promote the tandem oxidation of the 3-hydroxybutyraldehyde (3-HBAD) intermediate to 3-HBA and reduce the dehydration of 3-HBAD to the byproduct. At the same time, the PtSb2 alloy was also effective for the selective oxidation of several diols to hydroxyl-substituted acids.

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“…From a similar study but with high HSV, Liu et al. reported that well-dispersed Cu nanoparticles started agglomerating after 150 h on stream …”

Section: Introductionmentioning

confidence: 99%

“…Non-oxidative dehydrogenation of ethanol () has been gaining interest because of the co-production of hydrogen and the lower operating temperature range, 200–300°C . The endothermic non-oxidative route is thermodynamically favored only above 600 K, with low-temperature reactions being strongly limited with respect to achievable conversion .…”

Section: Introductionmentioning

confidence: 99%

Production of Acetaldehyde via Oxidative Dehydrogenation of Ethanol in a Chemical Looping Setup

et al. 2023

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A novel chemical looping (CL) process was demonstrated to produce acetaldehyde (AA) via oxidative dehydrogenation (ODH) of ethanol. Here, the ODH of ethanol takes place in the absence of a gaseous oxygen stream; instead, oxygen is supplied from a metal oxide, an active support for an ODH catalyst. The support material reduces as the reaction takes place and needs to be regenerated in air in a separate step, resulting in a CL process. Here, strontium ferrite perovskite (SrFeO 3−δ ) was used as the active support, with both silver and copper as the ODH catalysts. The performance of Ag/SrFeO 3−δ and Cu/SrFeO 3−δ was investigated in a packed bed reactor, operated at temperatures from 200 to 270 °C and a gas hourly space velocity of 9600 h −1 . The CL capability to produce AA was then compared to the performance of bare SrFeO 3−δ (no catalysts) and materials comprising a catalyst on an inert support, Cu or Ag on Al 2 O 3 . The Ag/Al 2 O 3 catalyst was completely inactive in the absence of air, confirming that oxygen supplied from the support is required to oxidize ethanol to AA and water, while Cu/Al 2 O 3 gradually got covered in coke, indicating cracking of ethanol. The bare SrFeO 3−δ achieved a similar selectivity to AA as Ag/SrFeO 3−δ but at a greatly reduced activity. For the best performing catalyst, Ag/SrFeO 3−δ , the obtained selectivity to AA reached 92−98% at yields of up to 70%, comparable to the incumbent Veba-Chemie process for ethanol ODH, but at around 250 °C lower temperature. The CL-ODH setup was operated at high effective production times (i.e., the time spent producing AA to the time spent regenerating SrFeO 3−δ ). In the investigated configuration with 2 g of the CLC catalyst and 200 mL/min feed flowrate ∼5.8 vol % ethanol, only three reactors would be required for the pseudo-continuous production of AA via CL-ODH.

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Co-production of hydrogen and acetaldehyde from ethanol over a highly dispersed Cu catalyst

Cited by 19 publications

References 54 publications

Redispersion and Stabilization of Cu/MFI Catalysts by the Encapsulation Method for Ethanol Dehydrogenation

Redispersion and Stabilization of Cu/MFI Catalysts by the Encapsulation Method for Ethanol Dehydrogenation

Selective Oxidation of 1,3-Butanediol to 3-Hydroxybutyric Acid over PtSb₂ Alloy

Production of Acetaldehyde via Oxidative Dehydrogenation of Ethanol in a Chemical Looping Setup

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Co-production of hydrogen and acetaldehyde from ethanol over a highly dispersed Cu catalyst

Cited by 19 publications

References 54 publications

Redispersion and Stabilization of Cu/MFI Catalysts by the Encapsulation Method for Ethanol Dehydrogenation

Redispersion and Stabilization of Cu/MFI Catalysts by the Encapsulation Method for Ethanol Dehydrogenation

Selective Oxidation of 1,3-Butanediol to 3-Hydroxybutyric Acid over PtSb2 Alloy

Production of Acetaldehyde via Oxidative Dehydrogenation of Ethanol in a Chemical Looping Setup

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Selective Oxidation of 1,3-Butanediol to 3-Hydroxybutyric Acid over PtSb₂ Alloy