Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO

C Pischetola; F Hesse; JWG Bos; F Cardenas-Lizana

doi:10.1016/j.apcata.2021.118277

Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO

C Pischetola, F Hesse, JWG Bos, F Cardenas-Lizana^*

^*Corresponding author for this work

School of Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO₂-TPD), d_XRD (4-20 nm) and specific surface area (SSA = 58 246 m² g^-1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li⁺ and Cs⁺ served to decrease SSA and increase d_XRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m²) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O^2- sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity.

Original language	English
Article number	118277
Number of pages	11
Journal	Applied Catalysis. A, General
Volume	623
Early online date	8 Jul 2021
DOIs	https://doi.org/10.1016/j.apcata.2021.118277
Publication status	Published - 5 Aug 2021

Keywords

Benzaldehyde and acetophenone
Benzylideneacetophenone
Li-and Cs-promotion
MgO
Selective gas phase condensation
Surface basicity

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https://researchportal.hw.ac.uk/en/publications/effect-of-lewis-basicity-on-the-continuous-gas-phase-condensationLicence: CC BY-NC-ND

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@article{595fe1b728604888a04e07a35f25db94,

title = "Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO",

abstract = "We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO2-TPD), dXRD (4-20 nm) and specific surface area (SSA = 58 246 m2 g-1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li+ and Cs+ served to decrease SSA and increase dXRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m2) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O2- sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity.",

keywords = "Benzaldehyde and acetophenone, Benzylideneacetophenone, Li-and Cs-promotion, MgO, Selective gas phase condensation, Surface basicity",

author = "C Pischetola and F Hesse and JWG Bos and F Cardenas-Lizana",

note = "Funding: The authors acknowledge the Engineering and Physical Sciences Research Council, Heriot-Watt University, and CRITICAT Centre for Doctoral Training for financial support [Ph.D. studentship to Chiara Pischetola and Fabian Hesse; Grant EP/L016419/1].",

year = "2021",

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doi = "10.1016/j.apcata.2021.118277",

language = "English",

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journal = "Applied Catalysis. A, General",

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TY - JOUR

T1 - Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO

AU - Pischetola, C

AU - Hesse, F

AU - Bos, JWG

AU - Cardenas-Lizana, F

N1 - Funding: The authors acknowledge the Engineering and Physical Sciences Research Council, Heriot-Watt University, and CRITICAT Centre for Doctoral Training for financial support [Ph.D. studentship to Chiara Pischetola and Fabian Hesse; Grant EP/L016419/1].

PY - 2021/8/5

Y1 - 2021/8/5

N2 - We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO2-TPD), dXRD (4-20 nm) and specific surface area (SSA = 58 246 m2 g-1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li+ and Cs+ served to decrease SSA and increase dXRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m2) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O2- sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity.

AB - We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO2-TPD), dXRD (4-20 nm) and specific surface area (SSA = 58 246 m2 g-1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li+ and Cs+ served to decrease SSA and increase dXRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m2) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O2- sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity.

KW - Benzaldehyde and acetophenone

KW - Benzylideneacetophenone

KW - Li-and Cs-promotion

KW - MgO

KW - Selective gas phase condensation

KW - Surface basicity

U2 - 10.1016/j.apcata.2021.118277

DO - 10.1016/j.apcata.2021.118277

M3 - Article

SN - 0926-860X

VL - 623

JO - Applied Catalysis. A, General

JF - Applied Catalysis. A, General

M1 - 118277

ER -

Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO

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Keywords

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