铵和磷离子液体的二氧化碳化学吸附：量子化学计算,The Journal of Physical Chemistry B

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铵和磷离子液体的二氧化碳化学吸附：量子化学计算
The Journal of Physical Chemistry B ( IF 2.8 ) Pub Date : 2022-07-14 , DOI: 10.1021/acs.jpcb.2c02968
Vitaly V Chaban ₁

Affiliation

碳捕获和储存是一项重要的技术努力，旨在通过对抗全球变暖来改善生态。目前的工作研究了由含有非质子杂环阴离子 2-氰基吡咯烷的铵基和鏻基离子液体引起CO ₂化学吸附的反应路径。我们举例说明 2 mol CO ₂每 1 mol 的气体清除剂理论上可以被这种离子液体固定。阳离子和阴离子都参与化学吸附。相应的标准焓和势能是适度负的。正如竞争途径的模拟所揭示的，化学吸附反应是通过将质子从阳离子提供给阴离子开始的。阳离子结构中的双共价键出现。涉及鏻基阳离子的所有反应的障碍相对较小，有利于所考虑的吸附剂的实际应用。由于四烷基铵叶立德固有的不稳定性，铵基阳离子的性能不太理想。对鏻叶立德在反应机理中的作用进行了仔细的描述。非质子阴离子作为 CO 的性能₂清除剂不受抗衡离子化学特性的影响。确定的空间屏障的基本高度强调了模拟反应物质的整个结构以获得化学吸附的可靠描述的必要性。报告的结果促进了对季铵基和鏻基 2-氰基吡咯内酯的出色 CO ₂吸附性能的基本理解。

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Carbon Dioxide Chemisorption by Ammonium and Phosphonium Ionic Liquids: Quantum Chemistry Calculations

Carbon capture and storage is an important technological endeavor aiming to improve the ecology by combating global warming. The present work investigates reaction paths that are responsible for CO₂ chemisorption by the ammonium- and phosphonium-based ionic liquids containing an aprotic heterocyclic anion 2-cyanopyrrolide. We exemplify that 2 mol of CO₂ per 1 mol of the gas scavenger can be theoretically fixed by such ionic liquids. Both the cation and anion participate in the chemisorption. The corresponding standard enthalpies and potential energies are moderately negative. The chemisorption reaction, as revealed by the simulations of competing pathways, is started by the donation of the proton from the cation to the anion. The double covalent bond in the cation’s structure emerges. The barriers to all reactions involving the phosphonium-based cation are relatively small and favor practical applications of the considered sorbents. The performance of the ammonium-based cation is less favorable due to the inherent instability of the tetraalkylammonium ylide. The role of phosphonium ylide in the mechanism of the reaction is carefully characterized. The performance of the aprotic anion as a CO₂ scavenger is unaffected by the chemical identity of the counterion. The essential heights of the identified steric barriers underline the necessity to simulate the entire structures of the reacting species to obtain a reliable description of chemisorption. The reported results foster a fundamental understanding of the outstanding CO₂ sorption performance of the quaternary ammonium- and phosphonium-based 2-cyanopyrrolides.

更新日期：2022-07-14

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