Improving Product Yield in the Direct Carboxylation of Glycerol with CO2 through the Tailored Selection of Dehydrating Agents

Razali, Nurul Ashraf; McGregor, James

doi:10.3390/catal11010138

Cited by 12 publications

(8 citation statements)

References 42 publications

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“…In a later study, the same authors provide novel insights into the behavior of dehydrating agents during the conversion of glycerol in the presence of carbon dioxide and a catalyst [76]. Particularly, they observed that conducting the reaction in the presence of adiponitrile resulted in a five-fold increase in GC yield when compared to acetonitrile, which is currently the most applied dehydrating agent.…”

Section: Co 2 Direct Carbonylation Routementioning

confidence: 93%

An Overview of the Latest Advances in the Catalytic Synthesis of Glycerol Carbonate

Procopio

Gioia

2022

Catalysts

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In recent years, the development of renewable energy alternatives to traditional fossil fuels has become one of the major challenges all over the world, due to the decline of fossil fuel reserves and their effect on global warming. Biodiesel has become a popular alternative energy source to reduce gas emissions compared to traditional fossil fuels. According to statistics, a nine-fold increase in global biofuel production between 2000 and 2020 was observed. However, its production generates a large amount of glycerol as a by-product, posing an environmental problem when disposed directly in landfills or by incineration. Therefore, low-value glycerol should be converted into high value-added derivatives. As glycerol carbonate is one of the most important derivatives of glycerol, this review aims to discuss the studies over the last ten years about glycerol carbonate synthetic methods, including the typical routes such as phosgene, esterification reaction, urea, oxidative and direct carbonylation as well as several rare synthetic procedures. At the same time, it summarizes the different catalytic reaction systems of each route comparing the advantages and disadvantages of various catalysts and evaluating their catalytic activity. Finally, the future development of glycerol carbonate synthesis is prospected from the point of view of development, technology research and industrialization.

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Section: Co 2 Direct Carbonylation Routementioning

confidence: 93%

An Overview of the Latest Advances in the Catalytic Synthesis of Glycerol Carbonate

Procopio

Gioia

2022

Catalysts

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“…According to the XRD patterns (Figure 2a), hexagonal Sm 2 O 2 CO 3 is the dominant phase. Combined with multiple carbonate peaks in attenuated total reflectance FTIR (Figure S3), 33 the carbonate groups in Sm 2 O 2 CO 3 are verified. To continue exploring the ability of the Sm 2 O 2 CO 3 to dissociate H 2 O, the experimental characterizations of in situ DRIFTS and mass spectrometry (MS) are employed.…”

Section: Catalytic Measurements and Kineticmentioning

confidence: 95%

Promoting Molecular Exchange on Rare-Earth Oxycarbonate Surfaces to Catalyze the Water–Gas Shift Reaction

Zhou

et al. 2023

J. Am. Chem. Soc.

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It is highly desirable to fabricate an accessible catalyst surface that can efficiently activate reactants and desorb products to promote the local surface reaction equilibrium in heterogeneous catalysis. Herein, rare-earth oxycarbonates (Ln2O2CO3, where Ln = La and Sm), which have molecular-exchangeable (H2O and CO2) surface structures according to the ordered layered arrangement of Ln2O2 2+ and CO3 2– ions, are unearthed. On this basis, a series of Ln2O2CO3-supported Cu catalysts are prepared through the deposition precipitation method, which provides excellent catalytic activity and stability for the water–gas shift (WGS) reaction. Density functional theory calculations combined with systematic experimental characterizations verify that H2O spontaneously dissociates on the surface of Ln2O2CO3 to form hydroxyl by eliminating the carbonate through the release of CO2. This interchange efficiently promotes the WGS reaction equilibrium shift on the local surface and prevents the carbonate accumulation from hindering the active sites. The discovery of the unique layered structure provides a so-called “self-cleaning” active surface for the WGS reaction and opens new perspectives about the application of rare-earth oxycarbonate nanomaterials in C1 chemistry.

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“…The hydrolysis reaction on ACN will leads to the formation of acetamide which on further hydrolysis produces acetic acid. [44] The formed acetic acid reacts with the unreacted glycerol and produces monoacetin and diacetin as side products (Scheme 2). The presence of higher number of Cu active sites at higher loading could favour the hydrolysis and acylation pathways to produce monoacetin and diacetin which resulted into to drop in the selectivity of GC.…”

Section: Chemistryselectmentioning

confidence: 99%

Mingled Metal Oxides Catalyst for Direct Carbonylation of Glycerol into Glycerol Carbonate

Pandey

Pawar

2022

ChemistrySelect

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The escalation of CO 2 into the atmosphere has encouraged the development of sustainable pathways to produce materials and chemicals from CO 2 . In the present manuscript, an attempt has been made for direct carbonylation of glycerol into Glycerol carbonate (GC) by using CO 2 over mingled metal oxide (MMO) catalyst. Several single, bi and trimetal oxides catalysts were explored for direct carbonylation of glycerol. Among the tested catalysts, Cu incorporated MMO showed the profound effect to obtain maximum glycerol conversion and GC selectively. However, a series of MMO catalysts with variable Cu loading were synthesized by simple co-precipitation method and tested for direct carbonylation of glycerol. Of all tested Cu loaded MMO catalyst, 5 % Cu loaded MMO catalyst (CuO/CeO 2 /ZnO) showed highest GC selectivity (99 %). Furthermore, the process intensification study was conducted to investigate the influence of various reaction parameters on glycerol conversion and GC yield such as catalyst loading, temperature, CO 2 pressure, time, and solvent concentration. The intensified process resulted into 57.4 % glycerol conversion with 57.2 % GC yield and 99.65 % selectivity. Moreover, the in-depth physicochemical characterisations of the synthesised MMO catalyst were conducted by using various surface analytical techniques. The synthesised MMO has showed a synergistic and protagonistic effect for direct carbonylation of glycerol. The recyclability study was performed to examine the robustness and efficency of the MMO catalyst that showed the consistency in the GC yield, conversion and selectivity without any significant loss after six consecutive runs. Also, the plausible reaction mechanism over MMO catalyst was proposed. The reported methodology has explored a simple, robust and efficient process for direct carbonylation of glycerol by using MMO catalyst with higher yield and selectivity of GC.

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Improving Product Yield in the Direct Carboxylation of Glycerol with CO2 through the Tailored Selection of Dehydrating Agents

Cited by 12 publications

References 42 publications

An Overview of the Latest Advances in the Catalytic Synthesis of Glycerol Carbonate

An Overview of the Latest Advances in the Catalytic Synthesis of Glycerol Carbonate

Promoting Molecular Exchange on Rare-Earth Oxycarbonate Surfaces to Catalyze the Water–Gas Shift Reaction

Mingled Metal Oxides Catalyst for Direct Carbonylation of Glycerol into Glycerol Carbonate

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