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Extended MOF-74-Type Variant with an Azine Linkage: Efficient Direct Air Capture and One-Pot Synthesis.
Choe, Jong Hyeak; Kim, Hyojin; Yun, Hongryeol; Kurisingal, Jintu Francis; Kim, Namju; Lee, Donggyu; Lee, Yong Hoon; Hong, Chang Seop.
Afiliación
  • Choe JH; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
  • Kim H; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
  • Yun H; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
  • Kurisingal JF; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
  • Kim N; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
  • Lee D; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
  • Lee YH; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
  • Hong CS; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea.
J Am Chem Soc ; 146(28): 19337-19349, 2024 Jul 17.
Article en En | MEDLINE | ID: mdl-38953459
ABSTRACT
Direct air capture (DAC) shows considerable promise for the effective removal of CO2; however, materials applicable to DAC are lacking. Among metal-organic framework (MOF) adsorbents, diamine-Mg2(dobpdc) (dobpdc4- = 4,4-dioxidobiphenyl-3,3'-dicarboxylate) effectively removes low-pressure CO2, but the synthesis of the organic ligand requires high temperature, high pressure, and a toxic solvent. Besides, it is necessary to isolate the ligand for utilization in the synthesis of the framework. In this study, we synthesized a new variant of extended MOF-74-type frameworks, M2(hob) (M = Mg2+, Co2+, Ni2+, and Zn2+; hob4- = 5,5'-(hydrazine-1,2-diylidenebis(methanylylidene))bis(2-oxidobenzoate)), constructed from an azine-bonded organic ligand obtained through a facile condensation reaction at room temperature. Functionalization of Mg2(hob) with N-methylethylenediamine, N-ethylethylenediamine, and N,N'-dimethylethylenediamine (mmen) enables strong interactions with low-pressure CO2, resulting in top-tier adsorption capacities of 2.60, 2.49, and 2.91 mmol g-1 at 400 ppm of CO2, respectively. Under humid conditions, the CO2 capacity was higher than under dry conditions due to the presence of water molecules that aid in the formation of bicarbonate species. A composite material combining mmen-Mg2(hob) and polyvinylidene fluoride, a hydrophobic polymer, retained its excellent adsorption performance even after 7 days of exposure to 40% relative humidity. In addition, the one-pot synthesis of Mg2(hob) from a mixture of the corresponding monomers is achieved without separate ligand synthesis steps; thus, this framework is suitable for facile large-scale production. This work underscores that the newly synthesized Mg2(hob) and its composites demonstrate significant potential for DAC applications.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2024 Tipo del documento: Article Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2024 Tipo del documento: Article Pais de publicación: Estados Unidos