硅基离子液体微颗粒强化气体捕集与转化的研究进展

doi:10.11949/0438-1157.20230531

摘要/Abstract

摘要：

解决工业过程污染气体的过量排放问题，具有重要的科学和环境意义。离子液体（ILs）作为室温呈液态的绿色溶剂，在气体捕集转化方面具有独特的优势，但天然的高黏度特性严重阻碍了其工业应用。本团队基于多年研究发现，不执拗于大幅降低离子液体的黏度，而顺其自然，通过“微颗粒化”技术，实现离子液体于准静止状态的高效利用，是离子液体适应工业化的有效路径之一。鉴于此，综述了以二氧化硅（SiO₂）为介质的离子液体微颗粒，及其衍生的离子液体纳-微界面反应单元在气体捕集（VOCs和CO₂）和CO₂转化方面的应用研究进展，探讨了微颗粒化离子液体体系较传统体系的特性优势，并分析了离子液体“微颗粒化”的应用前景及工业可行性。

关键词: 离子液体, 气体捕集, CO₂转换, 微尺度, 二氧化硅

Abstract:

It is of great scientific and environmental significance to solve the problem of excessive discharge of polluting gases in industrial processes. Ionic liquids (ILs), being green solvents in a liquid state at room temperature, possess unique advantages in gas capture and conversion. However, their inherent high viscosity poses a major challenge for industrial applications. Based on years of research, our team has discovered that instead of significantly reducing the viscosity of ILs, an effective approach to adapt them for industrial use is through the utilization of "micro particulation" technology, enabling efficient deployment of ionic liquids in a quasi-stationary state. In view of this, the research progress on the application of ionic liquid micro particles with silica as a medium and its derived ILs nano-micro interface reaction units for gas capture and conversion is reviewed, the characteristic advantages of micro particulated IL systems over conventional systems are discussed, and the "micro particulation" of ILs is analyzed. The application prospects and industrial feasibility of "micro particulation" of ILs are discussed.

Key words: ionic liquids, gas capture, CO₂ conversion, microscale, silica

中图分类号:

TQ 028.8

陈美思, 陈威达, 李鑫垚, 李尚予, 吴有庭, 张锋, 张志炳. 硅基离子液体微颗粒强化气体捕集与转化的研究进展[J]. 化工学报, 2023, 74(9): 3628-3639.

Meisi CHEN, Weida CHEN, Xinyao LI, Shangyu LI, Youting WU, Feng ZHANG, Zhibing ZHANG. Advances in silicon-based ionic liquid microparticle enhanced gas capture and conversion[J]. CIESC Journal, 2023, 74(9): 3628-3639.

图/表 11

图1 “干离子液体”的宏观及微观形态[28]

Fig.1 Macroscopic and microscopic morphology of a “dry ionic liquid”

图2 D-IL的宏观图像及高效的VOCs捕集效率[40]

Fig.2 The macroscopic image of D-IL and efficient VOCs capture efficiency[40]

图3 不同的硅基离子液体微颗粒孔隙形态[43]

Fig.3 Different pore morphologies of silica-based microparticles[43]

图4 [N2222][Gly]@SBA-15硅基离子液体微颗粒通过化学协同作用形成超微孔结构[45] (1 Å=10-10 m)

Fig. 4 [N2222][Gly]@SBA-15 silica-based microparticles form ultra-microporous structures through chemical synergy[45]

图5 [N1111][Gly]-EG硅基离子液体微颗粒形貌特征及其优异的捕集性能[48]

Fig.5 The morphological characteristics of [N1111][Gly]-EG silica-based microparticles and its capture rate[48]

表1 硅基离子液体微颗粒与纯离子液体CO2吸收量的比较

Table1 Comparison of CO2 uptake between silica-based ionic liquid microparticles and pure ionic liquid

吸收剂	吸收量/（mol/kg）	吸收条件	文献
[Bmim][HSO₄]	0.3	CO₂: 12 ml/min；25℃	[49]
[Bmim][HSO₄]-SiO₂	0.53	CO₂: 12 ml/min；25℃	[49]
[Bmim][BF₄]	0.24	CO₂: 12 ml/min；25℃	[44]
[Bmim][BF₄]-SiO₂	0.51
[Bmim][PF₆]	0.09
[Bmim][PF₆]-SiO₂	0.36
[Bmim][TfO]	0.28
[Bmim][TfO]-SiO₂	0.43
[Bmim][Tf₂N]	0.12
[Bmim][Tf₂N]-SiO₂	0.45

图6 纳-微界面反应单元催化强化CO2环加成反应[78]

Fig. 6 The catalysis intensification of CO2 cycloaddition in NMRUs[78]

表2 不同底物参与环加成反应的动力学比较

Table 2 Comparison of the kinetics of different substrates involved in cycloaddition reactions

反应底物	反应条件	转化率/%，转化时间/h
反应底物	反应条件	硅基[C₁C₆Im][HCO₃]微颗粒	[C₁C₆Im][HCO₃]体系
氧化苯乙烯	60 ℃ 0.4 MPa	96.08%，22.5 h	96.08%，65 h
环氧氯丙烷		97%，10 h	97%，23.3 h
烯丙基缩水甘油醚		95%，14.5 h	95%，31.2 h
环氧己烷		69%，26.5 h	51%，26.5 h
环氧环己烷		9.1%，25 h	4%，25 h

图7 NMRUs的微界面效应[78]

Fig.7 The micro interfacial effect of NMRUs[78]

图8 [C3C4Im][HCO3]-SiO2的合成路线

Fig.8 Schematic diagram of the synthesis of [C3C4Im][HCO3]-silica

表3 环加成反应中硅基离子液体微颗粒的催化性能

Table 3 Catalytic performance of silica-based IL microparticles in cycloaddition reactions

反应底物	反应温度	转化率/%，转化时间/h，CO₂分压
反应底物	反应温度	硅基[C₁C₆Im][HCO₃]微颗粒	[C₃C₄Im][HCO₃]-SiO₂微颗粒
氧化苯乙烯	60℃	96.08%，22.5 h，0.4 MPa	95%，12 h，0.3 MPa
环氧氯丙烷		97%，10 h，0.4 MPa	95.3%，2.5 h，0.3 MPa
烯丙基缩水甘油醚		95%，14.5 h，0.4 MPa	93.4%，10.2 h，0.3 MPa

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