Scale-up synthesis and shaping of MIL-160(Al) applicable for efficient CO2 adsorption and separation

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology Pub Date : 2024-12-15 DOI:10.1016/j.seppur.2024.131091

Mengkun Wang , Haijun Guo , Can Wang , Lian Xiong , Xuefang Chen , Fen Peng , Shimiao Yao , Hailong Li , Hairong Zhang , Xinde Chen

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引用次数: 0

Abstract

The scale-up preparation and shaping of Metal-Organic Frameworks (MOFs) is crucial for achieving its industrial application for CO₂ capture. In this work, MIL-160(Al)-5L powder was successfully produced in a 5 L reactor with an environmentally friendly and easy route under mild conditions, and then shaped into cylindrical particles via a simple extrusion method using dilute nitric acid as the binder. Mechanical performance tests indicated that the average crushing stress of the particles was 1.45 MPa, which slightly exceeded that of the commercial molecular sieve Zeolite-13X. Characterization of the MIL-160(Al)-5L powder and its shaped particles using XRD, FTIR, and BET analysis revealed there are no significant structural changes compared to experimental MIL-160(Al) except only a 5.93 % decrease in BET surface area for the shaped particles. Equilibrium adsorption isotherms for CO₂, CH₄, and N₂ at 298 K and 273 K were well fitted to the Langmuir-Freundlich model. The CO₂ adsorption capacity of the MIL-160(Al)-5L powder and its shaped particles were 3.13 mmol/g and 2.97 mmol/g at 298 K, respectively. Ideal adsorption solution theory (IAST) calculations indicated similar selectivity for CO₂/CH₄ and CO₂/N₂ across all samples. Breakthrough experiments demonstrated that the shaped sample possesses stable dynamic adsorption capacity and separation performance for simulated biogas, and its structural integrity is maintained after five consecutive breakthrough-regeneration cycles. Comparison with other shaped MOFs also highlights the advantages of low binder cost, superior mechanical, and adsorption properties, which suggests that MIL-160(Al) has shown potential applications prospect in CO₂ capture and gas separation. This work also provides a promising preparation method for developing stable and shaped MOFs for industrial applications.

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MIL-160（Al）的放大合成和成型，适用于高效的CO2吸附和分离

金属有机框架（MOFs）的规模化制备和成型对于实现二氧化碳捕集的工业应用至关重要。本研究在温和条件下，采用环保简便的方法，在 5 L 反应器中成功制备出 MIL-160(Al)-5L 粉末，然后以稀硝酸为粘合剂，通过简单的挤压方法将其成型为圆柱形颗粒。机械性能测试表明，颗粒的平均压碎应力为 1.45 兆帕，略高于商用分子筛 Zeolite-13X 的压碎应力。利用 XRD、傅立叶变换红外光谱和 BET 分析法对 MIL-160(Al)-5L 粉末及其成型颗粒进行表征后发现，与实验用 MIL-160(Al) 相比，除了成型颗粒的 BET 表面积减少了 3.72% 之外，其他结构没有发生显著变化。在 298 K 和 273 K 下，CO2、CH4 和 N2 的平衡吸附等温线与 Langmuir-Freundlich 模型拟合良好。在 298 K 时，MIL-160(Al)-5L 粉末及其异形颗粒对 CO2 的吸附量分别为 3.13 mmol/g 和 2.97 mmol/g。理想吸附溶液理论（IAST）计算表明，所有样品对 CO2/CH4 和 CO2/N2 的选择性相似。突破实验表明，该异型样品对模拟沼气具有稳定的动态吸附能力和分离性能，并且在连续五次突破-再生循环后仍能保持结构的完整性。与其他异型 MOFs 的比较也表明，MIL-160(Al) 具有粘合剂成本低、机械性能和吸附性能优越等优点，在二氧化碳捕集和气体分离方面具有潜在的应用前景。这项研究还为开发稳定的异型 MOFs 工业应用提供了一种可行的制备方法。

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来源期刊

Separation and Purification Technology 工程技术-工程：化工

CiteScore

14.00

自引率

12.80%

发文量

2347

审稿时长

43 days

期刊介绍： Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.