2023年 第23卷 第4期
《工程（英文）》 >> 2023年 第23卷 第4期 doi: 10.1016/j.eng.2022.07.017
天然气提质过程中可有效回收丙烷和乙烷的高工业应用潜力金属有机框架材料
a Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic, Shenzhen 518055, China
b Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, NJ 08854, USA
c School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China
d Department of Physics & Center for Functional Materials, Wake Forest University, Winston-Salem, NC 27109, USA
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摘要
开发具有高吸收和选择性的高效吸附剂用于从天然气中分离和回收C2H6和C3H8是一项重要但具有挑战性的任务。在这项工作中，我们证明了高表面极性和合适孔径是协同提高分离性能的两个关键因素，例如，金属有机框架（MOF）-303 和MIL-160（MIL：拉瓦锡材料研究所）都具有一维（1D）开放通道，其具有高密度杂原子和所需的孔径（5~7 Å）。值得注意的是，MOF-303 在298 K和5 kPa 下对C3H8的吸收高达3.38 mmol∙g−1，C3H8/CH4 (5:85, V/V)理想吸附溶液理论（IAST）选择性为5114，在所有已报道的MOF中创下新高。此外，MOF-303 也显示出很高的C2H6吸收能力（在10 kPa 时）和C2H6/CH4 (10:85, V/V)选择性，分别达到1.59 mmol∙g−1和26。与MOF-303 相比，MIL-160 的孔径更大，1D通道内杂原子密度更低，因此其具有明显较低的吸收和选择性，但其值超过了大多数报道的MOF。密度泛函理论（DFT）的计算结果表明，高表面极性和合适的孔径能协同增强框架对C3H8和C2H6的亲和力，从而产生了对C3H8和C2H6的高负载能力和选择性。在95%的相对湿度（RH）下暴露一个月后，两种MOF均具有显著的湿度稳定性，且结构没有变化。此外，这两种化合物的合成都可以很容易地通过一锅反应来放大规模，从而获得约5 g 的高结晶度样品。最后，通过三元突破性实验、再生试验和循环评价，证明了MOF-303 和MIL-160 作为先进的吸附剂在高效分离C3H8/C2H6/CH4方面的巨大潜力。其优异的分离性能、高稳定性、低成本和良好的可扩展性，是天然气净化和回收C2H6和C3H8的理想吸附剂。
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