Research progress on zeolite for CO2-N2-CH4 sieving separation

doi:10.16085/j.issn.1000-6613.2024-0803

Abstract

Abstract:

Facing the global challenges of energy shortage and increasing greenhouse effect, the development of gas separation technology based on molecular sieving principle is of great significance for reducing energy consumption and alleviating greenhouse effect. This sieving technology shows great potential for realizing CO₂ capture in flue gas and N₂ removal from natural gas, and it is challenging to realize effective molecular sieving of CO₂, N₂ and CH₄ molecules due to the similarity of physical properties among these gases. In this paper, based on the flexibility of zeolite frameworks (both rigid and flexible) and their sieving characteristics, molecular sieving was categorized into three separation mechanisms: size sieving mechanism (the most common sieving based on molecular size differences), molecular trapdoor mechanism and framework breathing-gated cation synergistic mechanism. The article comprehensively illustrated the constitutive relationships between zeolite framework types, framework rigidity (flexibility) and pore-blocking groups (including the type, number and position of equilibrium cations) with their performance in the sieve separation of CO₂, N₂, and CH₄ gases.

Key words: moleclar sieves, separation, carbon dioxide, nitrogen, methane

摘要：

面对能源短缺与温室效应加剧的全球性挑战，开发基于分子筛分原理的气体分离技术对降低能源消耗和缓解温室效应具有重要意义。这种筛分技术在烟气中实现CO₂捕集以及从天然气中脱除N₂方面展现出较大潜力，由于CO₂、N₂和CH₄分子之间的物理性质相似，实现这3种气体的有效分子筛分充满挑战。本文基于沸石骨架（包括刚性骨架和柔性骨架）的灵活性及其筛分特征，将分子筛分归纳为3种分离机制：尺寸筛分机制（基于分子尺寸差异最常见的筛分方式）、分子陷阱门机制以及骨架呼吸-门控阳离子协同机制。本文全面阐述了沸石骨架类型、骨架刚（柔）性以及孔隙阻塞基团（包括平衡阳离子的类型、数量和位置）和其与CO₂、N₂和CH₄气体筛分分离性能之间的构效关系。

关键词: 分子筛, 分离, 二氧化碳, 氮气, 甲烷

CLC Number:

TQ028.1

TANG Xuan, BAI Xiaowei, ZHANG Feifei, LI Jinping, YANG Jiangfeng. Research progress on zeolite for CO₂-N₂-CH₄ sieving separation[J]. Chemical Industry and Engineering Progress, 2025, 44(7): 3938-3949.

唐轩, 白晓炜, 张飞飞, 李晋平, 杨江峰. 沸石分子筛用于CO₂-N₂-CH₄筛分分离的研究进展[J]. 化工进展, 2025, 44(7): 3938-3949.

Figures/Tables 10

References 68

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气体分子	分子量	沸点/K	极化率/cm³	四极矩/esu·cm²	动力学直径/Å
CO₂	44	216.6	29.11×10^-25	4.30×10^-26	3.30
N₂	28	77.3	17.40×10^-25	1.52×10^-26	3.64
CH₄	16	111.7	25.93×10^-25	0	3.80

气体分子	分子量	沸点/K	极化率/cm³	四极矩/esu·cm²	动力学直径/Å
CO₂	44	216.6	29.11×10^-25	4.30×10^-26	3.30
N₂	28	77.3	17.40×10^-25	1.52×10^-26	3.64
CH₄	16	111.7	25.93×10^-25	0	3.80

筛分机制	窗口灵活性	特点	最大窗口环数	拓扑结构	骨架密度	典型材料
尺寸筛分机制	刚性	孔隙阻塞基团的类型、数量和位置	8	KFI	15.0T/1000Å³（1.49g/cm³）	K-ZK-5
			10	HEU	17.5T/1000Å³（1.75g/cm³）	Na⁺和Ca²⁺型斜发沸石
			12	MOR	17.0T/1000Å³（1.69g/cm³）	铁掺杂的丝光沸石
分子陷阱门机制	刚性	客体分子和孔隙阻塞基团相互作用的差异	8	CHA	15.1T/1000Å³（1.50g/cm³）	K-chabazite和Cs-chabazite
				MWF	16.1T/1000Å³（1.60g/cm³）	NaTEA-ZSM-25和K-ZSM-25
				LTA	14.2T/1000Å³（1.41g/cm³）	\|Na_10.2KCs_0.8\|-LTA和NaK-ZK-4
骨架呼吸-门控阳离子协同机制	柔性	柔性窗口协同孔隙阻塞基团迁移	8	—	2.20g/cm³	Sr-ETS-4和Ba-ETS-4
				MER	16.4T/1000Å³（1.63g/cm³）	Na-MER-2.3、K-MER-2.3和Rb-MER-2.3
				GIS	16.4T/1000Å³（1.64g/cm³）	Na-GIS-2.8和Na-GIS-3.0
				PHI	16.4T/1000Å³（1.63g/cm³）	Cs-PHI-2.5
				RHO	14.5T/1000Å³（1.44g/cm³）	Na-RHO、K-RHO和Cs-RHO

筛分机制	窗口灵活性	特点	最大窗口环数	拓扑结构	骨架密度	典型材料
尺寸筛分机制	刚性	孔隙阻塞基团的类型、数量和位置	8	KFI	15.0T/1000Å³（1.49g/cm³）	K-ZK-5
			10	HEU	17.5T/1000Å³（1.75g/cm³）	Na⁺和Ca²⁺型斜发沸石
			12	MOR	17.0T/1000Å³（1.69g/cm³）	铁掺杂的丝光沸石
分子陷阱门机制	刚性	客体分子和孔隙阻塞基团相互作用的差异	8	CHA	15.1T/1000Å³（1.50g/cm³）	K-chabazite和Cs-chabazite
				MWF	16.1T/1000Å³（1.60g/cm³）	NaTEA-ZSM-25和K-ZSM-25
				LTA	14.2T/1000Å³（1.41g/cm³）	\|Na_10.2KCs_0.8\|-LTA和NaK-ZK-4
骨架呼吸-门控阳离子协同机制	柔性	柔性窗口协同孔隙阻塞基团迁移	8	—	2.20g/cm³	Sr-ETS-4和Ba-ETS-4
				MER	16.4T/1000Å³（1.63g/cm³）	Na-MER-2.3、K-MER-2.3和Rb-MER-2.3
				GIS	16.4T/1000Å³（1.64g/cm³）	Na-GIS-2.8和Na-GIS-3.0
				PHI	16.4T/1000Å³（1.63g/cm³）	Cs-PHI-2.5
				RHO	14.5T/1000Å³（1.44g/cm³）	Na-RHO、K-RHO和Cs-RHO

Research progress on zeolite for CO₂-N₂-CH₄ sieving separation

沸石分子筛用于CO₂-N₂-CH₄筛分分离的研究进展

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