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首页> 外文期刊>ACS Sustainable Chemistry & Engineering >Unveiling the Molecular Mechanism of CO2 Capture in N-Methylethylenediamine-Grafted M2(dobpdc)
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Unveiling the Molecular Mechanism of CO2 Capture in N-Methylethylenediamine-Grafted M2(dobpdc)

机译：揭示在N-甲基乙基二胺接枝M2（DOBPDC）中CO 2捕获的分子机制

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摘要

For the first time, the adsorption properties and detailed microscopic mechanism of CO_(2) capture in N -methylethylenediamine (m-2) functionalized M_(2)(dobpdc) (dobpdc~(4–) = 4,4′-dioxidobiphenyl-3,3′-dicarboxylate; M = Mg, Sc–Zn) have been systematically investigated using van der Waals-corrected (vdW) density functional theory (DFT) calculations. Our results show that the m-2 binding energies in two binding modes via primary amine binding and secondary amine binding are similar. These binding energies range from 129/133 to 177/181 kJ/mol for 1°/2°-m-2-M_(2)(dobpdc) (M = Mg, Sc–Zn), providing a reasonable explanation for the experimental observations that 1°-amine-bound and 2°-amine-bound products coexist. For CO_(2) capture by 1°/2°-m-2-M_(2)(dobpdc), we have considered both the chain structures of the experimental configurations and the pair structures proposed by Planas et al. For each metal, the ammonium carbamate chain model is preferable to the carbamic acid pair model, and CO_(2)-1°-m-2-M_(2)(dobpdc) is more stable than CO_(2)-2°-m-2-M_(2)(dobpdc). The CO_(2) binding energies of chain-CO_(2)-1°-m-2-M_(2)(dobpdc) range from 45–102 kJ/mol. Moreover, the reaction path of CO_(2) capture in chain-1°-m-2-M_(2)(dobpdc) is described in detail in two parts. The first part is a proton transfer and nucleophilic addition between the CO_(2) and the metal-bound amine. This forms a zwitterion intermediate. The first step is found to be rate limiting with relatively high barriers of 0.62–1.44 eV. The second step is the rearrangement of the zwitterion intermediates with lower barriers (<0.50 eV). The present study provides detailed insights into the absorption of CO_(2) onto these materials. We hope that these results will provide inspiration for improved design of future CO_(2) capture materials.
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