Bottom-up fabrication of DABCO-based bicationic ionic liquid-grafted MIL-101(Cr): Facilitating simultaneous activation of CO2 and epoxides for cyclic carbonate synthesis

Separation and Purification Technology, Год журнала: 2024, Номер 354, С. 128851 - 128851

Опубликована: Июль 20, 2024

Язык: Английский

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Sustainable One-Pot Cellulose Dissolution and Derivatization via a Tandem Reaction in the DMSO/DBU/CO₂ Switchable Solvent System

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(44), С. 18693 - 18702

Опубликована: Окт. 29, 2021

New sustainable concepts have to be developed overcome the increasing problems of resource availability. Cellulose derivatives with tunable material properties are promising biobased alternatives existing petroleum-derived polymeric materials. However, chemical modification cellulose is very challenging, often requiring harsh conditions and complex solubilization or activation steps. More procedures toward novel therefore great interest. Herein, we describe a concept combining two approaches, (i) tandem catalysis (ii) derivatization, by applying single catalyst for three transformations in DMSO/DBU/CO2 switchable solvent system. was functionalized four different isothiocyanates, which were formed situ via catalytic sulfurization isocyanides elemental sulfur, preventing exposure handling isothiocyanates. The degree substitution O-cellulose thiocarbamates shown controllable range 0.52-2.16 varying equivalents reactants. All obtained products analyzed ATR-IR, 1H, 13C, 31P NMR spectroscopy as well size exclusion chromatography, analysis, differential scanning calorimetry, thermal gravimetric analysis. Finally, reaction approach beneficial terms efficiency sustainability compared stepwise synthesis. Recycling ratios ranging from 79.1% 95.6% employed components, resulting an E-factor 2.95 overall process.

Язык: Английский

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Straightforward construction of amino-functionalized ILs@SBA-15 catalysts via mechanochemical grafting for one-pot synthesis of cyclic carbonates from aromatic olefins and CO2

Journal of CO2 Utilization, Год журнала: 2022, Номер 59, С. 101962 - 101962

Опубликована: Март 5, 2022

Язык: Английский

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Nitrogen-rich cobalt (II) MOFs as efficient bifunctional catalysts for single or tandem oxidation and CO2 conversion reactions

Journal of CO2 Utilization, Год журнала: 2022, Номер 67, С. 102298 - 102298

Опубликована: Ноя. 3, 2022

The development of efficient catalysts that include the advantages homogeneous and heterogeneous is a challenge can be achieved with metal-organic frameworks (MOFs) since they incorporate different functionalities in their structure make them promising for processes. Herein, two new isoreticular nitrogen-rich naphthalene cobalt-MOFs, Co-NDTz Co-NDPhTz, were successfully prepared under solvothermal conditions from corresponding linkers (H2NDTz=2,6-naphthaleneditetrazole H2NDPhTz=2,6-bis(4-(1H-tetrazol-5-yl)phenyl)naphthalene). These Co-tetrazole-based MOFs combine Lewis acid redox good CO2 adsorption after being thermally activated resulted to excellent epoxidation alkenes cycloaddition epoxides yielding cyclic carbonates, reaching turnover numbers up 2500. Furthermore, these reactions take place following highly desired one-pot tandem process carbonate was obtained styrene solvent-free conditions. In addition, are easily recycled without noticeable loss catalytic activity important structural deterioration.

Язык: Английский

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Metal-Free N-Doped Carbons for Solvent-Less CO₂ Fixation Reactions: A Shrimp Shell Valorization Opportunity

ACS Sustainable Chemistry & Engineering, Год журнала: 2022, Номер 10(41), С. 13835 - 13848

Опубликована: Сен. 29, 2022

High anthropogenic CO2 emissions are among the main causes of climate change. Herein, we investigate use for synthesis organic cyclic carbonates on metal-free nitrogen-doped carbon catalysts obtained from chitosan, chitin, and shrimp shell wastes, both in batch continuous flow (CF). The were characterized by N2 physisorption, CO2-temperature-programmed desorption, X-ray photoelectron spectroscopy, scanning electron microscopy, CNHS elemental analysis, all reactivity tests run absence solvents. Under conditions, catalyst calcination chitin exhibited excellent performance conversion epichlorohydrin (selected as a model epoxide), resulting corresponding carbonate with 96% selectivity at complete conversion, 150 °C 30 bar CO2, 4 h. On other hand, CF regime, quantitative >99% achieved °C, using waste. Remarkably, material displayed an outstanding stability over reaction time 180 min. robustness synthetized was confirmed their good operational reusability: ca. (75 ± 3)% initial achieved/retained systems, after six recycles. Also, additional experiments proved that successful different terminal internal epoxides.

Язык: Английский

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Safer Polyurethane Foams with Cyclic Carbonates

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(20)

Опубликована: Янв. 13, 2023

Abstract Polyurethanes (PUs) are a class of materials usually synthesized from isocyanates, diols, and water. Water is essential for producing carbon dioxide (CO 2 ) which used the self‐blowing foams. Due to safety concerns with production alternative chemistries have been evaluated cyclic carbonate systems shown great promise. In recent advancement by Bourguignon, Grignard, Detrembleur, diamine system capable generating CO through hydrolysis carbonate‐based monomer. The authors demonstrate that simple variation monomer wide range physical thermo‐mechanical properties were achievable. This work represents significant step towards safer more environmentally friendly PUs.

Язык: Английский

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Sustainable valorisation of renewables through dialkyl carbonates and isopropenyl esters

Green Chemistry, Год журнала: 2023, Номер 25(13), С. 4878 - 4911

Опубликована: Янв. 1, 2023

This review showcases the most recent application of commercially relevant linear and alkylene organic carbonates a representative enol ester, isopropenyl acetate (iPAc), for chemical upgrading renewable-based compounds biopolymers.

Язык: Английский

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Transformations of Carbon Dioxide under Homogeneous Catalysis Conditions (A Review)

Petroleum Chemistry, Год журнала: 2022, Номер 62(1), С. 1 - 39

Опубликована: Янв. 1, 2022

Язык: Английский

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Atomically Dispersed Dual Metal Sites Boost the Efficiency of Olefins Epoxidation in Tandem with CO₂ Cycloaddition

Nano Letters, Год журнала: 2022, Номер 22(20), С. 8381 - 8388

Опубликована: Сен. 20, 2022

Tandem catalysis provides an economical and energy-efficient process for the production of fine chemicals. In this work, we demonstrate that a rationally synthesized carbon-based catalyst with atomically dispersed dual Fe–Al sites (ADD-Fe-Al) achieves superior catalytic activity one-pot oxidative carboxylation olefins (conversion ∼97%, selectivity ∼91%), where yield target product over ADD-Fe-Al is at least 62% higher than monometallic counterparts. The kinetic results reveal excellent performance arises from synergistic effect between Fe (oxidation site) Al (cycloaddition site), efficient CO2 cycloaddition epoxides in presence (3.91 wt %) positively shifts oxidation equilibrium to olefin epoxidation (0.89 %). This work not only offers advanced but also opens up avenue rational design multifunctional catalysts tandem reactions future.

Язык: Английский

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Multi-step oxidative carboxylation of olefins with carbon dioxide by combining electrochemical and 3D-printed flow reactors

Green Chemistry, Год журнала: 2023, Номер 25(23), С. 9934 - 9940

Опубликована: Янв. 1, 2023

Olefin electrooxidation is combined with CO 2 cycloaddition to produce cyclic carbonates using 3D-printed reactors in continuous flow.

Язык: Английский

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