低成本高稳定性K2Zn3[Fe(CN)6]2框架用于高效CO2/C2H2分离★

doi:10.6023/A26010036

化学学报 ›› 2026, Vol. 84 ›› Issue (5): 651-658.DOI: 10.6023/A26010036 上一篇下一篇

研究论文

低成本高稳定性K₂Zn₃[Fe(CN)₆]₂框架用于高效CO₂/C₂H₂分离^★

欧阳阳, 俱战锋^*(), 王文经, 杜顺福, 袁大强^*()

中国科学院福建物质结构研究所结构化学全国重点实验室福州 350002

投稿日期:2026-01-31 发布日期:2026-04-03
通讯作者: 俱战锋, 袁大强
作者简介:
★ “框架材料化学”专辑
基金资助:
国家自然科学基金(22275186); 国家自然科学基金(22275191); 中国科学院海西研究院自主部署项目(CXZX-2022-GH01); 中国科学院海西研究院自主部署项目(CXZX-2022-JQ11)

A Low-Cost and Highly Stable K₂Zn₃[Fe(CN)₆]₂ Framework for Efficient CO₂/C₂H₂ Separation^★

Yangyang Ou, Zhanfeng Ju^*(), Wenjing Wang, Shunfu Du, Daqiang Yuan^*()

State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China

Received:2026-01-31 Published:2026-04-03
Contact: Zhanfeng Ju, Daqiang Yuan
About author:
★ For the VSI “Chemistry of Framework Materials”.
Supported by:
National Natural Science Foundation of China(22275186); National Natural Science Foundation of China(22275191); Self-deployment Project Research Program of Haixi Institutes, Chinese Academy of Sciences(CXZX-2022-GH01); Self-deployment Project Research Program of Haixi Institutes, Chinese Academy of Sciences(CXZX-2022-JQ11)

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1. Supporting information-A26010036.pdf(2464KB)

摘要/Abstract

通过物理吸附分离法去除C₂H₂中的CO₂杂质具有节能优势, 但由于这两种气体的分子尺寸和物理性质极为接近, 给分离带来很大挑战性. 其中具有CO₂选择性的反向分离更为有效, 但是具有此性能的吸附剂十分稀缺. 另外, 吸附剂在分离过程中的稳定性、成本以及实际分离效率等问题均需考量. 本研究选用两种低成本、高稳定性的多孔配位框架材料Zn₃[Fe³⁺(CN)₆]₂ (ZnHCF)和K₂Zn₃[Fe²⁺(CN)₆]₂ (KZnHCF)来解决上述问题. 这两例材料的笼状孔道结构具备适宜的窗口尺寸, 可实现对CO₂的吸附性能优于C₂H₂. 在KZnHCF 中, 位于孔腔内部的 K⁺离子通过静电作用对进入孔道的CO₂与C₂H₂分子产生差异化定向作用, 显著提升了CO₂吸附量与分离选择性, 并在一定程度上缓解了吸附容量与选择性之间常见的此消彼长关系. 该材料在298 K条件下对CO₂的吸附量达到111.5 cm³•g⁻¹, 对等体积的CO₂/C₂H₂混合气体具备出色的CO₂选择性分离效果, 298 K、0.1 MPa条件下, 其理想吸附溶液理论(IAST)选择性为23.4. 更重要的是, 通过动态穿透实验发现, KZnHCF 可在较宽温度范围内保持高效的CO₂/C₂H₂分离性能. 在298 K条件下处理体积比50∶50的CO₂/C₂H₂混合气时, 该材料可一步法制备出纯度高于99.9%的C₂H₂, 动态吸附产率达1915 mmol•kg⁻¹, 仅略低于最新报道的最高纪录. 在323 K, 其吸附产率(1450 mmol•kg⁻¹)仍高于多数文献在298 K下报道的数值. KZnHCF 凭借优异的分离性能, 同时兼具高稳定性、可循环利用性、低成本及易规模化合成等优势, 成为潜在可应用于实际的高效CO₂/C₂H₂分离材料.

关键词: 多孔框架, 二氧化碳选择性, 逆向, 分离, 低成本

Removal of CO₂ impurity from C₂H₂ by physical-adsorption separation is energy-saving but extremely challenging because the two gases have very similar molecular dimensions and physicochemical properties. CO₂-selective (inverse) separation is more efficient, yet suitable adsorbents are scarce. Moreover, the stability, cost, and practical efficiency of adsorbents for gas separation must be addressed. This work employs two low-cost, stable porous coordination frameworks—Zn₃[Fe³⁺(CN)₆]₂ (ZnHCF) and K₂Zn₃[Fe²⁺(CN)₆]₂ (KZnHCF)—to overcome these obstacles. Their cage-like pore structures possess appropriate window sizes, enabling selective adsorption of CO₂ over C₂H₂. In KZnHCF, the K⁺ ions residing in the cavities electrostatically orient incoming CO₂ or C₂H₂ molecules differently, markedly enhancing CO₂ uptake and selectivity and partially mitigating the usual trade-off between capacity and selectivity. The material exhibits a remarkable saturated CO₂ adsorption capacity of 111.5 cm³•g⁻¹ at 298 K, and high CO₂-selective performance for 1∶1 (V/V) CO₂/C₂H₂ mixture, with an ideal adsorption solution theory (IAST) selectivity of 23.4 at 298 K and 0.1 MPa. More importantly, dynamic breakthrough experiments demonstrate that KZnHCF maintains highly efficient CO₂/C₂H₂ separation over a broad temperature range. From 50/50 (V/V) CO₂/C₂H₂ mixture at 298 K, the process yields C₂H₂ of >99.9 % purity with a dynamic productivity of 1915 mmol•kg⁻¹ in a single step—only slightly below the newly reported record. At 323 K, the productivity (1450 mmol•kg⁻¹) remains higher than most reported values at 298 K. This outstanding separation performance, combined with excellent stability, recyclability, low-cost, and facile scalable synthesis, positions KZnHCF as a promising adsorbent for efficient CO₂/C₂H₂ separation in practical applications.

Key words: porous framework, CO₂-selective, inverse, separation, low-cost

引用此文

欧阳阳, 俱战锋, 王文经, 杜顺福, 袁大强. 低成本高稳定性K₂Zn₃[Fe(CN)₆]₂框架用于高效CO₂/C₂H₂分离^★[J]. 化学学报, 2026, 84(5): 651-658.

Yangyang Ou, Zhanfeng Ju, Wenjing Wang, Shunfu Du, Daqiang Yuan. A Low-Cost and Highly Stable K₂Zn₃[Fe(CN)₆]₂ Framework for Efficient CO₂/C₂H₂ Separation^★[J]. Acta Chimica Sinica, 2026, 84(5): 651-658.

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图/表 5

Scheme 1. Syntheses of ZnHCF and KZnHCF

Figure 1. (a) The porous framework of ZnHCF, (b) ellipsoidal cavities of ZnHCF, (c) Zeolite-like structure of KZnHCF, K ions as counter ions distribute in the cavities of the porous framework, (d) ellipsoidal cavities of KZnHCF

Figure 2. (a) Chemial stability of KZnHCF proved by PXRD, toward acid, base, and other condition. (b) Stability of KZnHCF proved by PXRD, immersed in diverse organic solution for 7 d. (c) The sucessfully prepared 1.235 kg of KZnHCF

Figure 3. (a) CO2 and C2H2 adsorption isotherms for ZnHCF and KZnHCF at 298 K. (b) Comparison of CO2 and C2H2 uptakes among CO2-selective adsorbents at 298 K and 0.01 MPa. (c) IAST selectivity of ZnHCF and KZnHCF for CO2/C2H2 (V/V, 50/50) at 298 K and 0.1 MPa. (d) Separation performance of KZnHCF for equimolar CO2/C2H2 mixtures compared with other CO2-selective adsorbents at room temperature

Figure 4. Experimental column breakthrough curves for (a) an equimolar CO2/C2H2 mixture and (b) cycling tests of the equimolar CO2/C2H2 mixture (solid symbols: C2H2, open symbols: CO2) in a column packed with KZnHCF at 298 K and 0.1 MPa. (c) Comparision of C2H2 productivity with the reported CO2-selective asorbents at 298 K and 0.1 MPa, including the producivity on KZnHCF at 313 K and 323 K. (d) Experimental column breakthrough curves for an equimolar CO2/C2H2 mixture under diverse temperature on KZnHCF

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低成本高稳定性K₂Zn₃[Fe(CN)₆]₂框架用于高效CO₂/C₂H₂分离^★

A Low-Cost and Highly Stable K₂Zn₃[Fe(CN)₆]₂ Framework for Efficient CO₂/C₂H₂ Separation^★

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