Screening of Ionic Liquids for Efficient CO₂ Cycloaddition Catalysis under Mild Condition: A Combined Machine Learning and DFT Approach

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 19, 2024

The industrial application of ionic liquid-catalyzed CO2 cycloaddition reactions is impeded by harsh conditions. We propose a novel approach that utilizes machine learning and density functional theory (DFT) to overcome this challenge. By training regression algorithms on data set 10,174 experimental points, we developed predictive model for solubility in liquids. random forest (RF) exhibited exceptional accuracy, enabling the prediction 1624 newly generated Subsequent validation confirmed efficacy RF model. Moreover, employing DFT calculation, identified four liquids with high low energy barriers catalytic reactions, presenting promising candidates efficient epichlorohydrin under mild This study showcases streamlined catalyst discovery integrating methods, offering pathway toward sustainable utilization.

Language: Английский

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De novo assembly of frustrated Lewis pair bearing metal‐organic frameworks for atmospheric CO₂ cycloaddition

AIChE Journal, Journal Year: 2023, Volume and Issue: 70(4)

Published: Dec. 22, 2023

Abstract Porous frustrated Lewis pairs (FLPs) have been demonstrated as cutting‐edge heterogeneous catalysts in acidic–basic catalysis, which, yet faces great challenges synthesis. Herein, we propose a one‐step de novo assembly strategy for constructing porous FLPs by capping monodentate ionic liquids (ILs) on metal clusters during the synthesis of metal–organic frameworks (MOFs). The ILs makes adjacent sites MOFs transforming to coordinatively‐unsaturated acids, producing containing basic Cl − ions from and sites. distribution framework endows with large surface areas (up 2125 m 2 g −1 ), open channels good stability. behave unprecedented activity atmospheric CO activation coupling epoxides (25–40°C, 1 bar, without cocatalyst). This exhibits universality synthesizing different kinds ILs, paving facile approach designing high‐efficiency catalysts.

Language: Английский

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CO₂ to Cyclic Carbonate: A Mechanistic Insight of a Benign Route Using Zinc(II) Salophen Complexes

European Journal of Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 27(6)

Published: Dec. 16, 2023

Abstract Zinc(II) Schiff base complexes with different substituents at 5, 5’ positions have been synthesized to study the effect of electronic environment metal towards cycloaddition reaction between CO 2 and epoxide. The characterized by FT‐IR, XPS, NMR, spectroscopy, LC–MS, TGA. We used density functional theory structure Zn(II) modelled spectra mechanism catalysis. Results obtained from DFT LC–MS indicate dimeric structures for all except ZnL4. monomeric ZnL4 has strongest electron withdrawing group, i. e., −NO along two labile water molecules attached Zn center. exhibit good moderate yield styrene carbonate under solvent‐free conditions a relatively low temperature 80 °C, pressure ~1 atm. best achieved Different rate‐determining steps are captured studies complexes. Without taking any preventing measure dimerization attaching bulky t Bu groups, lesser catalytic amounts shown yields cyclic 53–74 %, depending on nature substituent present.

Language: Английский

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The Synthesis of Nitrogen- and Oxygen-Containing Heterocyclic Scaffolds Assisted by Ionic Liquids: A 2022 Literature Survey

Synlett, Journal Year: 2023, Volume and Issue: 35(14), P. 1648 - 1668

Published: Oct. 30, 2023

Abstract Heterocycles have gained recognition as vital components in approved drugs, drawing substantial attention from the scientific community. Ionic liquids (ILs) been utilized for their transformative roles heterocycle synthesis, showcasing distinctive properties that are pivotal diverse chemical transformations, while also acting effective catalysts and offering safer alternatives to volatile organic solvents. This account delves into synthesis of nitrogen- oxygen-containing heterocyclic structures, employing various ILs such ammonium, cholinium, DABCO-based, DBU-based, guanidinium-based, imidazolium, phosphonium, pyridinium, other miscellaneous examples. They proven indispensable facilitating reactions like Fischer indole Biginelli reaction, Knoevenagel condensations many more. Notably, recyclability serves a valuable asset, aiding completion intricate synthetic pathways, multicomponent reactions, one-pot syntheses, ultimately enhancing yields. account, covering literature published 2022, seeks guide researchers selecting suitable specific enable aza- and/or oxa-heterocycles. The described advancements represent promising prospects drug development applications within domain chemistry.

Language: Английский

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A mechanistic study on coupling of CO₂ and epoxide mediated by guanidine/TBAI catalysts

New Journal of Chemistry, Journal Year: 2023, Volume and Issue: 48(2), P. 920 - 932

Published: Dec. 1, 2023

Guanidine acted as H-bond donor to activate styrene oxide by (N)H⋯O interaction, facilitating epoxide ring-opening.

Language: Английский

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