Higher alcohol production from ethanol over occluded [Mg4(OH)4]4+ clusters in MgO/KNaX

Nattapol Yotkkham; Kittisak Choojun; Pratya Promchana; Xiaolei Fan; Tawan Sooknoi

doi:10.1016/j.apcata.2022.118502

Higher alcohol production from ethanol over occluded [Mg₄(OH)₄]⁴⁺ clusters in MgO/KNaX

Nattapol Yotkkham, Kittisak Choojun, Pratya Promchana, Xiaolei Fan, Tawan Sooknoi

Research output: Journal Publication › Article › peer-review

1 Citation (Scopus)

Abstract

Conversion of ethanol to higher alcohols was studied over MgO/KNaX, prepared by ion exchange with Mg(OAc)₂, followed by KOH washing. The catalysts were characterized by XRF, XRD, SEM, BET, ²⁷Al MAS NMR, EXAFS, NH₃- and CO₂-TPD. All catalysts showing MgO nanopetals and aggregates on the external surface, contained occluded [Mg₄(OH)₄]⁴⁺ clusters in the zeolite cavities, providing medium basic (M_b) and acid (M_a) sites. Ethanol conversion and higher alcohols selectivity (up to 78%) increased with M_b/M_a ratio due to the increase in both MgO (4–6 wt%) and K (14.7–17.3 wt%) loadings. Decreasing occluded [Mg₄(OH)₄]⁴⁺ clusters and/or increasing MgO aggregates led to the lower conversion and yields of higher alcohols. The essential role of the occluded [Mg₄(OH)₄]⁴⁺ clusters in producing higher alcohols was verified by the reactions using various control catalysts. The MgO/KNaX showed high stability even after steaming at 380 °C, as well as being regenerated by calcination (450 °C in air).

Original language	English
Article number	118502
Journal	Applied Catalysis A: General
Volume	632
DOIs	https://doi.org/10.1016/j.apcata.2022.118502
Publication status	Published - 25 Feb 2022
Externally published	Yes

Keywords

Ethanol conversion
Guerbet reaction
Higher alcohol
MgO nanopetals
Occluded MgO clusters
Zeolite X

ASJC Scopus subject areas

Catalysis
Process Chemistry and Technology

Access to Document

10.1016/j.apcata.2022.118502

Cite this

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title = "Higher alcohol production from ethanol over occluded [Mg4(OH)4]4+ clusters in MgO/KNaX",

abstract = "Conversion of ethanol to higher alcohols was studied over MgO/KNaX, prepared by ion exchange with Mg(OAc)2, followed by KOH washing. The catalysts were characterized by XRF, XRD, SEM, BET, 27Al MAS NMR, EXAFS, NH3- and CO2-TPD. All catalysts showing MgO nanopetals and aggregates on the external surface, contained occluded [Mg4(OH)4]4+ clusters in the zeolite cavities, providing medium basic (Mb) and acid (Ma) sites. Ethanol conversion and higher alcohols selectivity (up to 78%) increased with Mb/Ma ratio due to the increase in both MgO (4–6 wt%) and K (14.7–17.3 wt%) loadings. Decreasing occluded [Mg4(OH)4]4+ clusters and/or increasing MgO aggregates led to the lower conversion and yields of higher alcohols. The essential role of the occluded [Mg4(OH)4]4+ clusters in producing higher alcohols was verified by the reactions using various control catalysts. The MgO/KNaX showed high stability even after steaming at 380 °C, as well as being regenerated by calcination (450 °C in air).",

keywords = "Ethanol conversion, Guerbet reaction, Higher alcohol, MgO nanopetals, Occluded MgO clusters, Zeolite X",

author = "Nattapol Yotkkham and Kittisak Choojun and Pratya Promchana and Xiaolei Fan and Tawan Sooknoi",

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2022",

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T1 - Higher alcohol production from ethanol over occluded [Mg4(OH)4]4+ clusters in MgO/KNaX

AU - Yotkkham, Nattapol

AU - Choojun, Kittisak

AU - Promchana, Pratya

AU - Fan, Xiaolei

AU - Sooknoi, Tawan

PY - 2022/2/25

Y1 - 2022/2/25

N2 - Conversion of ethanol to higher alcohols was studied over MgO/KNaX, prepared by ion exchange with Mg(OAc)2, followed by KOH washing. The catalysts were characterized by XRF, XRD, SEM, BET, 27Al MAS NMR, EXAFS, NH3- and CO2-TPD. All catalysts showing MgO nanopetals and aggregates on the external surface, contained occluded [Mg4(OH)4]4+ clusters in the zeolite cavities, providing medium basic (Mb) and acid (Ma) sites. Ethanol conversion and higher alcohols selectivity (up to 78%) increased with Mb/Ma ratio due to the increase in both MgO (4–6 wt%) and K (14.7–17.3 wt%) loadings. Decreasing occluded [Mg4(OH)4]4+ clusters and/or increasing MgO aggregates led to the lower conversion and yields of higher alcohols. The essential role of the occluded [Mg4(OH)4]4+ clusters in producing higher alcohols was verified by the reactions using various control catalysts. The MgO/KNaX showed high stability even after steaming at 380 °C, as well as being regenerated by calcination (450 °C in air).

AB - Conversion of ethanol to higher alcohols was studied over MgO/KNaX, prepared by ion exchange with Mg(OAc)2, followed by KOH washing. The catalysts were characterized by XRF, XRD, SEM, BET, 27Al MAS NMR, EXAFS, NH3- and CO2-TPD. All catalysts showing MgO nanopetals and aggregates on the external surface, contained occluded [Mg4(OH)4]4+ clusters in the zeolite cavities, providing medium basic (Mb) and acid (Ma) sites. Ethanol conversion and higher alcohols selectivity (up to 78%) increased with Mb/Ma ratio due to the increase in both MgO (4–6 wt%) and K (14.7–17.3 wt%) loadings. Decreasing occluded [Mg4(OH)4]4+ clusters and/or increasing MgO aggregates led to the lower conversion and yields of higher alcohols. The essential role of the occluded [Mg4(OH)4]4+ clusters in producing higher alcohols was verified by the reactions using various control catalysts. The MgO/KNaX showed high stability even after steaming at 380 °C, as well as being regenerated by calcination (450 °C in air).

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KW - Guerbet reaction

KW - Higher alcohol

KW - MgO nanopetals

KW - Occluded MgO clusters

KW - Zeolite X

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