Haris Muhammad, Aziz Arif, Sohail Muhammad, Sardar Waseem
College of Power and Energy Engineering, Harbin Engineering University, Harbin, 150001, People's Republic of China.
College of Physics and Optoelectronics Engineering, Harbin Engineering University, Harbin, 150001, People's Republic of China.
Environ Sci Pollut Res Int. 2025 May;32(21):12681-12699. doi: 10.1007/s11356-025-36464-7. Epub 2025 May 5.
Post-combustion CO capture offers a promising solution for reducing carbon from power plants and marine emissions. By capturing CO from exhaust gases, it helps lessen the environmental impact. This paper evaluates the comparative performance of a hybrid blend of such absorbents as N-methyldiethanolamine (MDEA), ethanolamine (MEA), tetraethylenepentamine (TEPA), aminomethylpropanol (AMP), and piperazine (PZ) for CO capture, with emphasis on imitations of the flue gases for a marine engine. MDEA was taken as a base amine, while the percentages of MEA, TEPA, AMP, and PZ were taken in variable proportions to optimize absorption, desorption, and cyclic CO capacity. The absorbents were tested under simulated marine engine flue gas conditions with exposure to NO to test their performance and robustness in real-world CO capture scenarios. The highest initial CO absorption capacity was recorded for the TEPA + MDEA mixture; however, the presence of NO causes a serious decrease in this absorption. Under identical conditions, an opposite effect-that is, the increase of its CO absorption-was found in the AMP + MDEA mixture, pointing out how complex interactions between blend composition and gas contaminants are. Density functional theory (DFT) calculations were obtained with frontier molecular orbital (FMO) analysis, natural bond orbital (NBO) analysis, electron density difference (EDD) mappings, and non-covalent interaction (NCI) analysis. FMO analysis of the adsorption of CO showed a decrease in highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) energy gaps, potentially signifying higher reactivity. Relevant charge transfer from CO to the blends was evidenced by NBO analysis, which is consistent with the outcomes of EDD and NCI analyses that indicated non-bonding van der Waals interactions between CO and absorbent components. The study throws new light on mixed absorbents for post-combustion CO capture and emphasizes the role of computational techniques in understanding molecular interactions, energy dynamics, and bonding mechanisms, thus assisting the design of advanced absorbents for sustainable CO capture technologies.
燃烧后二氧化碳捕集为减少发电厂和船舶排放的碳提供了一个有前景的解决方案。通过从废气中捕集二氧化碳，有助于减轻对环境的影响。本文评估了N-甲基二乙醇胺（MDEA）、乙醇胺（MEA）、四乙烯五胺（TEPA）、氨基甲基丙醇（AMP）和哌嗪（PZ）等吸收剂的混合混合物用于二氧化碳捕集的比较性能，重点是模拟船舶发动机的烟气。以MDEA作为基础胺，MEA、TEPA、AMP和PZ的百分比采用可变比例以优化吸收、解吸和循环二氧化碳容量。吸收剂在模拟船舶发动机烟气条件下进行测试，并暴露于NO中，以测试它们在实际二氧化碳捕集场景中的性能和稳定性。TEPA+MDEA混合物的初始二氧化碳吸收能力最高；然而，NO的存在会导致这种吸收严重下降。在相同条件下，在AMP+MDEA混合物中发现了相反的效果，即其二氧化碳吸收增加，这指出了混合成分与气体污染物之间的相互作用是多么复杂。通过前沿分子轨道（FMO）分析、自然键轨道（NBO）分析、电子密度差（EDD）映射和非共价相互作用（NCI）分析获得了密度泛函理论（DFT）计算结果。CO吸附的FMO分析表明最高占据分子轨道-最低未占据分子轨道（HOMO-LUMO）能隙减小，这可能意味着更高的反应活性。NBO分析证明了从CO到混合物的相关电荷转移，这与EDD和NCI分析结果一致，后者表明CO与吸收剂成分之间存在非键范德华相互作用。该研究为燃烧后二氧化碳捕集的混合吸收剂提供了新的思路，并强调了计算技术在理解分子相互作用、能量动力学和键合机制方面的作用，从而有助于设计用于可持续二氧化碳捕集技术的先进吸收剂。
