Interfacial Sites in Ag Supported Layered Double Oxide for Dehydrogenation Coupling of Ethanol to <i>n</i>‐Butanol

Zhang, Jian; Shi, Kai Qi; Zhu, Yanru; An, Zhe; Wang, Wanning; Ma, Xiaodan; Shu, Xin; Song, Hang; Xiang, Xu; He, Jing

doi:10.1002/open.202000295

Cited by 6 publications

(10 citation statements)

References 57 publications

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“…Figure 5c shows the O 1s XPS spectra of the two catalysts. From the results, two distinct peaks at 531.6 eV and 530.2 eV were observed and should be ascribed to the existence of adsorbed oxygen (Oα) and lattice oxygen (Oβ) [27,41]. The relative amounts of Oα and Oβ changed with the composition of supports, suggesting that the chemical form of surface oxygen depends heavily on the chemical composition.…”

Section: Electronic Property Of the Catalystmentioning

confidence: 94%

“…For Cu/MgAlOx (Figure 7a), the bands at 1252 cm −1 are observed at 298 K, which is assigned to the δ(C-OH) of adsorbed 3-hydroxybutanal [45], whereas for Cu/ZnAlOx (Figure 7b), the vibration at 1393 cm −1 could be discerned, indicating the presence of ethyl-acetate species [46]. In addition, the bands at 1076 and 1102 cm −1 were presented in both Cu/MgAlOx and Cu/ZnAlOx catalysts, corresponding to C-O stretching vibrations in adsorbed ethoxide [27,41]. The Cu/ZnAlOx catalyst has higher intensity of adsorbed ethoxide at the elevated temperatures, implying that it is more difficult for ethanol transformation for Cu/ZnAlOx than for Cu/MgAlOx.…”

Section: In Situ Drift Spectra Of Ethanol Adsorption and Transformationmentioning

confidence: 95%

“…In contrast, for the Cu/ZnAlO x catalyst, more O β were present on the surface, suggesting that oxygen appears in the form of metal oxides, i.e., ZnO or Al 2 O 3 . In addition, in the Al 2p XPS spectra (Figure 5d), the binding energy at 73.8-74.2 eV could be assigned to Al 3+ , which corresponded to the Zn-O-Al and Mg-O-Al, respectively [41].…”

Section: Electronic Property Of the Catalystmentioning

confidence: 98%

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Copper Supported on MgAlOx and ZnAlOx Porous Mixed-Oxides for Conversion of Bioethanol via Guerbet Coupling Reaction

Liu

Ding

et al. 2022

Catalysts

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The direct conversion of biomass-derived ethanol to high-valued-added chemicals has attracted widespread attention recently due to the great economic and environmental advantages. In the present study, the conversion of bioethanol through the Guerbet coupling process was studied in a fixed-bed reactor for MgAlOx and ZnAlOx mixed-oxides supported Cu catalysts. From the results, Cu adding into the system greatly enhance the dehydrogenation of ethanol and increase the H-transfer in the course of Guerbet coupling process. Simultaneously, the porous mixed-oxides provide the acid-base property of the catalysts for intermediate transformation. Notably, for Cu/MgAlOx, the main product of ethanol conversion is butanol, but for Cu/ZnAlOx, the primary product is ethyl acetate. Characterizations such as X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and CO2 temperature programmed desorption (TPD) were carried out to evaluate the structure and property of the catalysts. In combination with the catalytic performances with the characterization results, the synergistic catalytic effect between metal sites and acid-base sites were elaborated.

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Section: Electronic Property Of the Catalystmentioning

confidence: 94%

Section: In Situ Drift Spectra Of Ethanol Adsorption and Transformationmentioning

confidence: 95%

Section: Electronic Property Of the Catalystmentioning

confidence: 98%

See 1 more Smart Citation

Copper Supported on MgAlOx and ZnAlOx Porous Mixed-Oxides for Conversion of Bioethanol via Guerbet Coupling Reaction

Liu

Ding

et al. 2022

Catalysts

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“…A variety of homogeneous catalysts have been studied for this transformation. − Jones et al were able to achieve 68% butanol selectivity utilizing a [(PNP)Mn(Br)(CO) 2 ] homogeneous catalyst in neat ethanol, and recently, the Jones group reported a 57% butanol selectivity with [( p -cymene)Ru(6,6′-bpy OH )Cl]Cl as their catalyst in an aqueous solvent system . A variety of heterogeneous catalysts for the Guerbet process involving commercial cobalt powder, metal oxides, − metal–organic frameworks, and hydroxyapatite − have also been reported with butanol selectivities of 70, 50, 99, and 75%, respectively. In a recent report, a homogeneous (NNN)Ru pincer catalyst was used to obtain 62% ethanol conversion with a 45% yield of n-butanol.…”

Section: Introductionmentioning

confidence: 99%

Ethanol Upgrading ton-Butanol Using Transition-Metal-Incorporated Poly(triazine)imide Frameworks

Cypher,

Pauly,

Castro

et al. 2023

ACS Appl. Mater. Interfaces

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The upgrading of ethanol to n-butanol was performed using a molecular catalyst integrated into a carbon nitride support, one of the first examples of a supported molecular catalyst performing the Guerbet process. Initial studies using crystalline poly(triazine)imide (PTI) with lithium or transition-metal cations imbedded in the support together with a base as the catalyst system did not produce any significant amounts of n-butanol. However, when using the catalyst material formed by treatment of PTI-LiCl with [(Cp*)IrCl2]2 (Cp* = pentamethylcyclopentadienyl) along with sodium hydroxide, a 59% selectivity for butanol (13% yield) was obtained at 145 °C. This PTI-(Cp*)Ir material exhibited distinct UV–vis absorption features and powder X-ray diffractions which differ from those of the parent PTI-LiCl and [(Cp*)IrCl2]2. The PTI-(Cp*)Ir material was found to have a metal loading of 27% iridium per empirical unit of the framework. Along with the formation of n-butanol from the Guerbet reaction, the presence of higher chain alcohols was also observed.

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“…They discovered that the atomic Ru can promote ethanol dehydrogenation to acetaldehyde and the aldol condensation of acetaldehyde by adjusting the Ru dispersion and the acid-base properties [33]. Besides, Mg-Al mixed oxides supported by Pd [37], Ag [39], and Ni [40] catalysts are also synthesized and evaluated for ethanol coupling to butanol. However, the utilization of noble metal catalysts increases the final cost of the whole process.…”

Section: Introductionmentioning

confidence: 99%

Highly Selective and Stable Cu Catalysts Based on Ni–Al Catalytic Systems for Bioethanol Upgrading to n-Butanol

Yan

Zhan

et al. 2023

Molecules

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The catalytic upgrading of ethanol into butanol through the Guerbet coupling reaction has received increasing attention recently due to the sufficient supply of bioethanol and the versatile applications of butanol. In this work, four different supported Cu catalysts, i.e., Cu/Al2O3, Cu/NiO, Cu/Ni3AlOx, and Cu/Ni1AlOx (Ni2+/Al3+ molar ratios of 3 and 1), were applied to investigate the catalytic performances for ethanol conversion. From the results, Ni-containing catalysts exhibit better reactivity; Al-containing catalysts exhibit better stability; but in terms of ethanol conversion, butanol selectivity, and catalyst stability, a corporative effect between Ni–Al catalytic systems can be clearly observed. Combined characterizations such as XRD, TEM, XPS, H2-TPR, and CO2/NH3-TPD were applied to analyze the properties of different catalysts. Based on the results, Cu species provide the active sites for ethanol dehydrogenation/hydrogenation, and the support derived from Ni–Al–LDH supplies appropriate acid–base sites for the aldol condensation, contributing to the high butanol selectivity. In addition, catalysts with strong reducibility (i.e., Cu/NiO) may be easily deconstructed during catalysis, leading to fast deactivation of the catalysts in the Guerbet coupling process.

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Interfacial Sites in Ag Supported Layered Double Oxide for Dehydrogenation Coupling of Ethanol to n‐Butanol

Cited by 6 publications

References 57 publications

Copper Supported on MgAlOx and ZnAlOx Porous Mixed-Oxides for Conversion of Bioethanol via Guerbet Coupling Reaction

Copper Supported on MgAlOx and ZnAlOx Porous Mixed-Oxides for Conversion of Bioethanol via Guerbet Coupling Reaction

Ethanol Upgrading ton-Butanol Using Transition-Metal-Incorporated Poly(triazine)imide Frameworks

Highly Selective and Stable Cu Catalysts Based on Ni–Al Catalytic Systems for Bioethanol Upgrading to n-Butanol

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