Influence of Support Properties on the Activity of Basic Catalysts for Aldol Condensation of Formaldehyde and Methyl Acetate in a Continuous Flow Reactor

Wang, Yanan; Chen, Huanhui; Zhao, Guoqing; Liu, Min; Lang, Xuewei; Zhu, Zhirong

doi:10.1556/jfc-d-14-00035

Cited by 10 publications

(4 citation statements)

References 24 publications

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“…Still, lots of by-products were detected over HBeta zeolites. Although the acidic sites were reported to be essential to improve the aldol condensation [4,14] , strong acidic sites lead to many side reactions such as olefin polymerization and cracking to increase by-product and coke contents. After nitridation, formaldehyde conversion and methyl acrylate selectivity increase to 97% and 94%, respectively, over NBeta catalyst.…”

Section: Aldol Condensation Catalyzed By Nbeta Zeolitesmentioning

confidence: 99%

“…At present, aldol condensation reactions are mainly carried out on solid catalysts, including acidic [4,8,9] , basic [5,10] , and acid-base bifunctional catalysts [11][12][13] . Solid acidic catalysts mainly include phosphates [8] and zeolites [9,14] . Khalameida et al reported titanium phosphates for aldol condensation of acetic acid and formaldehyde with an acrylic acid selectivity of 80% [8] .…”

Section: Introductionmentioning

confidence: 99%

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Highly selective production of renewable methyl acrylate via aldol condensation over Cu modified nitrogen-containing Beta zeolites

Wang,

Xu,

Zhang

2024

Chem Synth

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Highly selective synthesis of renewable methyl acrylate from bio-sourced formaldehyde and methyl acetate through one-step aldol condensation was successfully realized on Cu-modified nitrogen-containing Beta (NBeta) catalysts. Silicon-29 magic angle spinning nuclear magnetic resonance (29Si MAS NMR), Fourier transform infrared spectroscopy (FT-IR), temperature-programmed desorption of ammonia, temperature-programmed desorption of carbon dioxide, and element analysis indicate that nitridation weakens the acid strength, reduces the number of acidic sites and introduces basic sites through the formation of Si−N bond on Beta zeolites, thereby promoting methyl acrylate selectivity and reducing the coke formation. Adding Cu into NBeta further finely tunes the basicity and acidity balance and thus inhibits the by-product acetone. High methyl acrylate selectivity of 95% and formaldehyde conversion of 99% were achieved over Cu/NBeta catalyst under optimized conditions. The coke content decreases remarkably from 28% on H-form Beta (HBeta) zeolites to 17% on NBeta zeolites doped with Cu due to its appropriate basicity/acidity. Cu/NBeta has good regeneration capability, and the weakening of Si-N species may account for the decline of catalytic performance after successive regeneration. The catalytic performance was restored when the regenerated catalyst was nitridated again.

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Section: Aldol Condensation Catalyzed By Nbeta Zeolitesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Highly selective production of renewable methyl acrylate via aldol condensation over Cu modified nitrogen-containing Beta zeolites

Wang,

Xu,

Zhang

2024

Chem Synth

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“…A new potential way to synthesize MA using methyl acetate (Ma) with formaldehyde (FA) by vapor phase aldol condensation in a one-step process (Scheme ) has been developed. , Solid base and acid–base catalysts with cesium as the main active component that supported porous silica, alumina, magnesia, and zeolites showed good activity for aldol condensation reactions. − Yan et al reported a 48.4 mol % conversion of Ma and 95.0 mol % selectivity of MA over Cs/SBA-15 catalyst in a single-pass, fixed-bed, and flow reactor. Wang et al reported a series of supported cesium basic catalysts with commercially available materials (ZSM-5, SiO 2 , and γ-Al 2 O 3 ) as support for aldol condensation of FA and Ma in a continuous-flow reactor. Ai found that Cs–Si catalyst exhibited the best catalytic performance for the formation of methyl methacrylate (MMA) from aldol condensation of FA and propionic acid (PA), with a continuous-flow system.…”

Section: Introductionmentioning

confidence: 99%

“…11−17 Yan et al 7 reported a 48.4 mol % conversion of Ma and 95.0 mol % selectivity of MA over Cs/ SBA-15 catalyst in a single-pass, fixed-bed, and flow reactor. Wang et al 12 reported a series of supported cesium basic catalysts with commercially available materials (ZSM-5, SiO 2 , and γ-Al 2 O 3 ) as support for aldol condensation of FA and Ma in a continuous-flow reactor. Ai 13 found that Cs−Si catalyst exhibited the best catalytic performance for the formation of methyl methacrylate (MMA) from aldol condensation of FA and propionic acid (PA), with a continuous-flow system.…”

Section: Introductionmentioning

confidence: 99%

One-Step Synthesis of Methyl Acrylate Using Methyl Acetate with Formaldehyde in a Fluidized Bed Reactor

Jiang

Chen

et al. 2017

Ind. Eng. Chem. Res.

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A fluidized bed process for the one-step synthesis of methyl acrylate (MA) using methyl acetate (Ma) and formaldehyde (FA) was developed for the first time. New spherical antiwear acid−base catalysts Cs−P/γ-Al 2 O 3 were prepared using ultrasonic impregnation method and characterized with XRD, BET, SEM, PSD, ICP, TG/DTA, NH 3 -TPD, and CO 2 -TPD methods. Catalytic performance was evaluated, and 10.0 wt % Cs−5.0 wt % P/γ-Al 2 O 3 with weak acid−base sites was determined to be the best catalyst for MA production. Response surface methodology (RSM) was employed to optimize aldol condensation of Ma with FA over 10.0 wt % Cs−5.0 wt % P/γ-Al 2 O 3 . The effects of various process parameters such as reaction temperature, molar ratio of Ma and FA, and liquid hourly space velocity (LHSV) on MA yield were addressed by Box−Behnken experimental design (BBD). The coefficient of determination (R 2 ) of this model was 0.997, and 39.5 mol % yield of MA was obtained after optimization. The developed catalyst exhibited high stability, with no significant decrease in catalytic activity after 1000 h of lifetime evaluation.

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Gaseous catalytic condensation reaction of methyl propionate and formaldehyde in a fluidized bed reactor

Li¹,

Qi²,

Xie³

et al. 2019

Can J Chem Eng

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A one-step aldol condensation reaction of methyl propionate and formaldehyde to produce methyl methacrylate is a promising environmentally sustainable strategy. In this work, the aldol condensation reaction was firstly conducted in a fluidized bed reactor using different types of catalysts. Zirconium and cesium-loaded SiO 2 and Al 2 O 3 acid-base bifunctional catalysts were prepared by wetness impregnation. Experimental results demonstrated the 15 % Cs-0.05 %Zr/SiO 2 (100-200 mesh) catalyst exhibited excellent catalytic performance. The effects of the supports, reaction temperature, carrier gas flow rate, and feed rate were investigated and optimized. When the flow rate of carrier gas (N 2 ) was 280 cm 3 /min and the feed rate was 0.6 cm 3 /min, the methyl propionate conversion was 25.2 % and the methyl methacrylate selectivity could reach 86.1 %. Although the catalytic activity of the 15 %Cs-0.05 %Zr/SiO 2 catalyst dropped with reaction time on stream due to carbon deposition on the surface of catalyst, its activity was restored by a simple regeneration method.

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Influence of Support Properties on the Activity of Basic Catalysts for Aldol Condensation of Formaldehyde and Methyl Acetate in a Continuous Flow Reactor

Cited by 10 publications

References 24 publications

Highly selective production of renewable methyl acrylate via aldol condensation over Cu modified nitrogen-containing Beta zeolites

Highly selective production of renewable methyl acrylate via aldol condensation over Cu modified nitrogen-containing Beta zeolites

One-Step Synthesis of Methyl Acrylate Using Methyl Acetate with Formaldehyde in a Fluidized Bed Reactor

Gaseous catalytic condensation reaction of methyl propionate and formaldehyde in a fluidized bed reactor

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