Three Robust Isoreticular Metal–Organic Frameworks with High-Performance Selective CO 2 Capture and Separation

作者：Wen Li, Xinyao Liu, Xueyue Yu, Borong Zhang, Chao Ji, Zhaohui Shi, Lirong Zhang, Yunling Liu · 发表于：Inorganic Chemistry · 年份：2023 · DOI：10.1021/acs.inorgchem.3c02851 · 被引用次数：14 · 研究领域：Metal-Organic Frameworks: Synthesis and Applications、Covalent Organic Framework Applications、Carbon Dioxide Capture Technologies

Based on the hard-soft acid base (HSAB) theory, three robust isoreticular metal–organic frameworks (MOFs) with nia topology were successfully synthesized by solvothermal reaction {[In 3 O(BHB)(H 2 O) 3 ]NO 3 ·3DMA ( JLU-MOF110(In) ), [Fe 3 O(BHB)(H 2 O) 3 ]NO 3 ( JLU-MOF110(Fe) ), and [Fe 2 NiO(BHB)(H 2 O) 3 ] ( JLU-MOF110(FeNi) ) (DMA = N, N -dimethylacetamide, H 6 BHB = 4,4″-benzene-1,3,5-triyl-hexabenzoic acid)}. Both JLU-MOF110(In) and JLU-MOF110(Fe) are cationic frameworks, and their BET surface areas are 301 and 446 m 2 /g, respectively. By modification of the components of metal clusters, JLU-MOF110(FeNi) features a neutral framework, and the BET surface area is increased up to 808 m 2 /g. All three MOF materials exhibit high chemical and thermal stability. JLU-MOF110(In) remains stable for 24 h at pH values ranging from 1 to 11, while JLU-MOF110(Fe) and JLU-MOF110(FeNi) persist to be stable for 24 h at pH from 1 to 12. JLU-MOF110(In) exhibits thermal stability up to 350 °C, whereas JLU-MOF110(Fe) and JLU-MOF(FeNi) can be stable up to 300 °C. Thanks to the microporous cage-based structure and abundant open metal sites, JLU-MOF110(In), JLU-MOF110(Fe), and JLU-MOF110(FeNi) have excellent CO 2 capture capacity (28.0, 51.5, and 99.6 cm 3 /g, respectively, under 298 K and 1 bar). Interestingly, the ideal adsorption solution theory results show that all three MOFs exhibit high separation selectivity toward CO 2 over N 2 (35.2, 43.2, and 43.2 for CO 2 /N 2 = 0.15/0.85) and CO...