The eternal battle to combat global warming: (thio)urea as a CO2 wet scrubbing agent

文献情報

出版日 2020-04-24

DOI 10.1039/D0CP00629G

インパクトファクター 3.676

著者

Ala’a F. Eftaiha, Abdussalam K. Qaroush, Ahed W. Alsayyed, Feda’a Al-Qaisi, Fatima Alsoubani, Khaleel I. Assaf

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要旨

(Thio)Urea scaffolds are best known for their importance as intermediates in organic synthesis. In this work, a mechanistic study of the reaction between urea (U), (2-hydroxyethyl)urea (U-EtOH) and thiourea (tU)/NaH in DMSO with CO2 was carried out. While both U/tU reacted with CO2via a 1 : 2 mechanism through the formation of the keto (thio)carbamide–carboxylate adducts (k-U/tU-CO2− Na+), U-EtOH gave mixed CO2-adducts composed of organic carbonate and carbamide–carboxylate moieties (Na+-CO2-U-Et-OCO2− Na+). Moreover, we recorded for the first time, a new type of bond, namely sodium carbamimidothiocarbonate (e-tU-SCO2− Na+), upon bubbling CO2 in the DMSO solution of tU due to the persistence of the enol form (e-tU) and the better nucleophilicity of sulfur over nitrogen focal points. The reaction mechanisms were proven by 1D and 2D nuclear magnetic resonance (NMR) and ex situ attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopies. The stability of these bonds was studied following the changes in 1H-NMR as a function of temperature, which indicated the reversibility of these reactions. Furthermore, the proposed mechanisms were explored theoretically via density functional theory (DFT) calculations by analyzing the energetics of the anticipated products.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.