Cation-assisted interactions between N-heterocycles and CO2

文献情報

出版日 2015-05-12

DOI 10.1039/C5CP01793A

インパクトファクター 3.676

著者

Huarong Tang, Dongmei Lu, Chao Wu

原文を見る

要旨

Cation-assisted interactions between N-containing heterocycles (NHCs) and CO2 have been systematically studied by using density functional theory (DFT). For neutral and anionic (non-carbenoid) NHCs, the effects of monovalent cations (i.e., alkali metal ions) are moderate to small (the NHC–CO2 binding energy change, ΔBE usually < 25 kJ mol−1). However, for NHC carbenes, due to their strong basicity, the effects are strong (ΔBE > 60 kJ mol−1) and the monovalent cations play a critical role in the single carboxylation of dicarbenes with CO2. In comparison, divalent alkali earth metal cations, due to both their smaller sizes and higher formal charges, exhibit a much stronger influence (ΔBE > 100 kJ mol−1). Divalent cations should be incorporated into next generation CO2 capture reagents. Other aspects including the reaction potential energy surface (PES), orbital-based analyses of interactions, substitution effects, and the reactivity descriptors (cation size, reacting N lone pair orbital energy, etc.) have been discussed in detail as well.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

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