高效分离同碳数烃的先进微孔膜：现状与挑战

doi:10.16085/j.issn.1000-6613.2023-0464

摘要/Abstract

摘要：

热法精馏分离同碳数烃混合物是当前石油化工行业中最耗能的过程之一。膜分离技术具有投资成本和操作费用低、节能降耗和集成度高等优点，可实现低能耗的膜法流程再造。以沸石分子筛和金属有机骨架材料（MOF）为代表的先进微孔膜较传统聚合物膜，具有更高的分离性能；渗透性和分离选择性可提升一至两个数量级，展现出优异的应用前景。本文综述了先进微孔膜在提升渗透性、分离选择性与分离过程稳定性3个方面的研究进展，深入探讨了膜层厚度、孔道取向、骨架柔性和晶间缺陷等微结构调控与同碳数烃分离性能间的构效关系。并且分析了面向同碳数烃高效分离应用的几种沸石膜和MOF膜面积放大制备的瓶颈问题，提出了晶种/成核位点均一性分布在先进微孔膜放大制备中的关键作用。最后对进一步加快新型先进微孔膜材料开发进程以应对石化行业多元化分离体系，以及加大膜工艺技术开发力度以匹配石化行业主流程工艺要求进行了展望。

关键词: 同碳数烃, 膜, 金属有机骨架, 沸石, 分离

Abstract:

Separation of hydrocarbon mixtures with the same carbon number by thermal distillation is one of the most energy-consuming processes in the petrochemical industry. The membrane separation technology can realize the reconstruction of membrane technology with low energy consumption due to the advantages of low investment and operating costs, high energy saving and high process integration degree. The advanced microporous membranes represented by zeolite and metal-organic framework materials have better separation performance than traditional polymers membrane, which can improve the permeability and selectivity by one or two orders of magnitude, and show excellent application prospects. This paper reviewed the progress of advanced microporous membranes in improving permeability, separation selectivity and separation process stability. The structure-activity relationship between the separation performance of hydrocarbon with the same carbon number and the microstructure regulation of membrane thickness, pore orientation, framework flexibility and intergranular defects was discussed in detail. The bottleneck problem of area scaling preparation of several zeolite films and MOF films for efficient separation of hydrocarbon with the same carbon number was analyzed, and the key role of homogeneity distributionof crystal seed/nucleation site in advanced microporous film scaling was proposed. Finally, it was expected to further accelerate the development of new advanced microporous membrane materials to cope with the diversified separation system in the petrochemical industry, and to increase the development of membrane technology to match the main process requirements in the petrochemical industry.

Key words: same-carbon-number hydrocarbon, membrane, metal-organic frameworks, zeolite, separation

中图分类号:

TQ028

潘宜昌, 周荣飞, 邢卫红. 高效分离同碳数烃的先进微孔膜：现状与挑战[J]. 化工进展, 2023, 42(8): 3926-3942.

PAN Yichang, ZHOU Rongfei, XING Weihong. Advanced microporous membranes for efficient separation of same-carbon-number hydrocarbon mixtures: State-of-the-art and challenges[J]. Chemical Industry and Engineering Progress, 2023, 42(8): 3926-3942.

图/表 14

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膜种类	制备方法	支撑体	厚度/µm	参考文献
沸石分子筛膜（MFI）	低温快速合成	α-氧化铝管	0.6	[19]
	二次生长	α-氧化铝片	0.3~0.4	[20]
	干凝胶法+微波法	氧化铝中空纤维	0.4	[25]
	无凝胶二次生长法	SiO₂片	0.2	[26]
	无凝胶二次生长法	烧结石英纤维	0.1	[30]
	微波二次生长法	α-氧化铝片	0.38	[31]
MOF膜（ZIF-8）	二次生长	α-氧化铝片	2.5	[32]
	电化学	阳极氧化铝片	0.2	[33]
	反扩散	Torlon中空纤维	2	[34]
	凝胶气相沉积	PVDF中空纤维	0.017	[35]
	界面诱导	聚砜	0.045	[36]

膜种类	制备方法	支撑体	厚度/µm	参考文献
沸石分子筛膜（MFI）	低温快速合成	α-氧化铝管	0.6	[19]
	二次生长	α-氧化铝片	0.3~0.4	[20]
	干凝胶法+微波法	氧化铝中空纤维	0.4	[25]
	无凝胶二次生长法	SiO₂片	0.2	[26]
	无凝胶二次生长法	烧结石英纤维	0.1	[30]
	微波二次生长法	α-氧化铝片	0.38	[31]
MOF膜（ZIF-8）	二次生长	α-氧化铝片	2.5	[32]
	电化学	阳极氧化铝片	0.2	[33]
	反扩散	Torlon中空纤维	2	[34]
	凝胶气相沉积	PVDF中空纤维	0.017	[35]
	界面诱导	聚砜	0.045	[36]

膜类型	支撑体类型	制备方法	膜面积/cm²		C₃H₆或n-C₄H₁₀渗透速率^①/10^-8mol·m^-2·s^-1·Pa^-1	分离因子	参考文献
膜类型	支撑体类型	制备方法	单个膜	膜组件	C₃H₆或n-C₄H₁₀渗透速率^①/10^-8mol·m^-2·s^-1·Pa^-1	分离因子	参考文献
沸石分子筛膜（MFI）	不锈钢管状支撑体	原位合成法	15.7	—	4	18	[86]
	α-Al₂O₃管状支撑体	二次生长法	94	—	1	78	[87]
	TiO₂管状支撑体	二次生长法	78.5	—	1.6	6	[88]
	α-Al₂O₃管状支撑体	二次生长法	180	3800	13	45	[93]
	19通道α-Al₂O₃支撑体	二次生长法	84	—	10.3	51	[94]
	19通道α-Al₂O₃支撑体	二次生长法	270	—	6.4	32	[94]
	61通道α-Al₂O₃支撑体	二次生长法	190	—	8.1	28	[95]
MOF膜（ZIF-8）	PVDF中空纤维	凝胶-气相沉积法	11.3	340	28	70	[35]
	陶瓷管状支撑体	晶种-二次生长法	24.5	—	1.3	67	[80]
	陶瓷管状支撑体	电化学合成法	—	—	0.6	63	[104]
	陶瓷管状支撑体	前体辅助生长法	25	157	1.08	55	[105]
	陶瓷平板支撑体	浸涂-热转换法	100	300	0.24	38	[106]

膜类型	支撑体类型	制备方法	膜面积/cm²		C₃H₆或n-C₄H₁₀渗透速率^①/10^-8mol·m^-2·s^-1·Pa^-1	分离因子	参考文献
膜类型	支撑体类型	制备方法	单个膜	膜组件	C₃H₆或n-C₄H₁₀渗透速率^①/10^-8mol·m^-2·s^-1·Pa^-1	分离因子	参考文献
沸石分子筛膜（MFI）	不锈钢管状支撑体	原位合成法	15.7	—	4	18	[86]
	α-Al₂O₃管状支撑体	二次生长法	94	—	1	78	[87]
	TiO₂管状支撑体	二次生长法	78.5	—	1.6	6	[88]
	α-Al₂O₃管状支撑体	二次生长法	180	3800	13	45	[93]
	19通道α-Al₂O₃支撑体	二次生长法	84	—	10.3	51	[94]
	19通道α-Al₂O₃支撑体	二次生长法	270	—	6.4	32	[94]
	61通道α-Al₂O₃支撑体	二次生长法	190	—	8.1	28	[95]
MOF膜（ZIF-8）	PVDF中空纤维	凝胶-气相沉积法	11.3	340	28	70	[35]
	陶瓷管状支撑体	晶种-二次生长法	24.5	—	1.3	67	[80]
	陶瓷管状支撑体	电化学合成法	—	—	0.6	63	[104]
	陶瓷管状支撑体	前体辅助生长法	25	157	1.08	55	[105]
	陶瓷平板支撑体	浸涂-热转换法	100	300	0.24	38	[106]

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