Yang Shan-Qing, Xing Bo, Wang Lu-Lu, Zhou Lei, Zhang Fei-Yang, Li Yi-Long, Hu Tong-Liang
School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin 300350, China.
Chem Bio Eng. 2024 Feb 1;1(3):245-251. doi: 10.1021/cbe.3c00073. eCollection 2024 Apr 25.
Porous solid adsorbents for CH/CO separation are generally confronted with poor stability, high cost, or high regeneration energy, which largely inhibit their industrial implementation. A desired adsorbent material for practical implementation should exhibit a good balance between low cost, high stability, scale-up production feasibility, and good separation performance. An effective strategy is herein explored based on reticular chemistry through embedding methyl groups in a prototype microporous metal-organic framework (MOF) featuring low cost and high stability to effectively separate an CH/CO mixture. The anchored methyl groups on the pore surfaces could strongly boost the CH packing density and specifically enhance the CH/CO separation performance, as distinctly established by single-component gas sorption isotherms. The CAU-10-CH material exhibits an excellent CH packing density of 486 g L and high adsorption differences between CH and CO uptake (147%), outperforming the prototype benchmark material CAU-10-H (392 g L and 53%). The highly selective adsorption of CH over CO was achieved by a lower CH adsorption enthalpy (25.18 kJ mol) compared to that with unfunctionalized CAU-10-H. In addition, dynamic column breakthrough experiments further confirm CAU-10-CH's efficient separation performance for the CH/CO mixture. CAU-10-CH accomplishes the benchmark balance between cost, stability, scale-up, and separation performance for CH/CO separation, establishing its promise for industrial implementation. This approach could further facilitate the development of advanced MOF adsorbents to address challenging separation processes. Thus, this study paves the route for the practical implementations of MOF materials in the gas adsorption and separation field.
用于CH/CO分离的多孔固体吸附剂通常面临稳定性差、成本高或再生能量高的问题,这在很大程度上阻碍了它们的工业应用。一种适用于实际应用的理想吸附剂材料应在低成本、高稳定性、放大生产可行性和良好的分离性能之间取得良好平衡。本文基于网状化学探索了一种有效策略,通过在具有低成本和高稳定性的原型微孔金属有机框架(MOF)中嵌入甲基来有效分离CH/CO混合物。孔表面锚定的甲基可以显著提高CH的堆积密度,并特别增强CH/CO的分离性能,这通过单组分气体吸附等温线得到了明确证实。CAU-10-CH材料表现出优异的CH堆积密度,为486 g/L,CH和CO吸附量之间的吸附差异很大(147%),优于原型基准材料CAU-10-H(392 g/L和53%)。与未功能化的CAU-10-H相比,CH的吸附焓较低(25.18 kJ/mol),从而实现了CH对CO的高选择性吸附。此外,动态柱穿透实验进一步证实了CAU-10-CH对CH/CO混合物的高效分离性能。CAU-10-CH在CH/CO分离的成本、稳定性、放大生产和分离性能之间实现了基准平衡,展现了其工业应用前景。这种方法可以进一步促进先进MOF吸附剂的开发,以解决具有挑战性的分离过程。因此,本研究为MOF材料在气体吸附和分离领域的实际应用铺平了道路。