通过竞争性氢键相互作用合理设计用于 HCl 吸收的高效低共熔溶剂,Physical Chemistry Chemical Physics

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通过竞争性氢键相互作用合理设计用于 HCl 吸收的高效低共熔溶剂
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-10-14 , DOI: 10.1039/d2cp03418b
Lin Feng _{1,

2} , Shuyi Li _{1,

2} , Chunxi Li _{1,

2,

3} , Hong Meng ₄ , Yingzhou Lu ₂ , Hongwei Fan ₂

Affiliation

高效吸收剂的设计是工业尾气中氯化氢（HCl）回收和资源化利用的前提。在此，设计了一系列基于 1-丁基-3-甲基咪唑鎓氯化物 (BmimCl) 的深共晶溶剂 (DESs)，并从其结构、碱度、自由体积、分子间相互作用能和吸收焓。详细探讨了HCl溶解过程中相互作用能与相变的关系。BmimCl-TAA（硫代乙酰胺）（1:1）由于其高自由体积、合适的吸收焓以及 BmimCl 与 TAA 或 HCl 之间更紧密的氢键 (HB) 相互作用而显示出高可逆溶解度。通过FT-IR和NMR光谱以及量子化学计算验证了HCl的溶解机理和HB网络的动态演化。结果表明，正是竞争性HB相互作用促进了HCl的溶解，降低了吸收焓，呈现可逆吸收。与BmimCl相比，HCl在BmimCl-TAA（1:1）中的吸收焓降低了25%，可逆溶解度提高了150%。HCl 在 BmimCl-TAA (1 : 1) 中的可逆溶解度高达 0.51 gg 1）降低25%，可逆溶解度提高150%。HCl 在 BmimCl-TAA (1 : 1) 中的可逆溶解度高达 0.51 gg 1）降低25%，可逆溶解度提高150%。HCl 在 BmimCl-TAA (1 : 1) 中的可逆溶解度高达 0.51 gg^-1 (1.76 mol mol^-1 )在303.15 K和101.3 kPa下，并且吸收剂可以通过减压加热容易地再生。这项工作为合理设计 DES 以有效和可逆地吸收 HCl 和其他极性气体提供了新的见解。

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Rational design of efficient deep eutectic solvents for HCl absorption through their competitive H-bonding interactions

The design of an efficient absorbent is the premise for recovery and resource utilization of hydrogen chloride (HCl) from its industrial tail gases. Herein, a series of 1-butyl-3-methylimidazolium chloride (BmimCl) based-deep eutectic solvents (DESs) were designed and the solubility behavior for HCl was studied in terms of their structure, basicity, free volume, intermolecular interaction energy, and absorption enthalpy. The relationship between the interaction energy and the phase change in the HCl dissolution process was explored in detail. BmimCl-TAA (thioacetamide) (1 : 1) shows high reversible solubility due to its high free volume, suitable absorption enthalpy, and closer H-bonding (HB) interactions between BmimCl and TAA or HCl. The dissolution mechanism of HCl and the dynamic evolution of the HB network were verified by FT-IR and NMR spectra and quantum chemical calculations. The results show that it is the competitive HB interaction that promotes the dissolution of HCl, reduces the absorption enthalpy, and renders a reversible absorption. Compared with BmimCl, the absorption enthalpy of HCl in BmimCl-TAA (1 : 1) is reduced by 25% and the reversible solubility increased 150%. The reversible solubility of HCl in BmimCl-TAA (1 : 1) is as high as 0.51 g g⁻¹ (1.76 mol mol⁻¹) at 303.15 K and 101.3 kPa, and the absorbent can be regenerated facilely by heating under reduced pressure. This work provides new insights into the rational design of DES for efficient and reversible absorption of HCl and other polar gases.

更新日期：2022-10-14

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