G5 Doctoral dissertation (article)
Exploring the applicability of amine-containing metal-organic frameworks on direct air capture of carbon dioxide (2024)
Amiineja sisältävien metalliorgaanisten verkkorakenteiden soveltuvuus hiilidioksidin talteenottoon suoraan ilmasta


Mahajan, S. (2024). Exploring the applicability of amine-containing metal-organic frameworks on direct air capture of carbon dioxide [Doctoral dissertation]. University of Jyväskylä. JYU Dissertations, 819. https://urn.fi/URN:ISBN:978-952-86-0280-4


JYU authors or editors


Publication details

All authors or editors: Mahajan, Shreya

eISBN: 978-952-86-0280-4

Journal or series: JYU Dissertations

eISSN: 2489-9003

Publication year: 2024

Number in series: 819

Number of pages in the book: 1 verkkoaineisto (69 sivua, 50 sivua useina numerointijaksoina, 3 numeroimatonta sivua)

Publisher: University of Jyväskylä

Place of Publication: Jyväskylä

Publication country: Finland

Publication language: English

Persistent website address: https://urn.fi/URN:ISBN:978-952-86-0280-4

Publication open access: Openly available

Publication channel open access: Open Access channel


Abstract

Negative emission technologies (NETs), such as direct air capture (DAC), hold substantial potential in limiting planetary warming. Among the various CO2-capturing materials being explored, a promising class of porous crystalline materials, such as metal–organic frameworks (MOFs), have come out ahead as potentially customizable materials for selectively capturing atmospheric CO2. The thesis's first section covers the most recent achievements made in developing MOFs for DAC potential. It provides a detailed account of structural approaches, examines MOFs' DAC performance under different conditions, and discusses the CO2 adsorption pathways. The second section of the thesis encapsulates the key results published in three journal articles related to this work.
The results and discussion section detail the preparation of an amino-triazole-based N-rich bent ligand and the structural determination of its sixteen new molecular salts, each assisted by different anions. Several characterization techniques were employed to fully understand these anion-templated supramolecular assemblies, which are self-assembled by a combination of noncovalent interactions, constituting different protonation sites and a versatile spectrum of conformations of the bent ligand. The amino-triazole-based ligand was further utilized in constructing a series of MOFs, namely, MOF-1-Zn, MOF-2-Zn, and MOF-3-Zn. This was achieved using the mixed-linker strategy, combining the selected ligand with a carboxylate linker to introduce basic functionalities (–NH2) and polarizable sulfur atoms onto the MOF pores. In addition to examining the CO2 capture capabilities of the MOFs, we systematically investigated the dynamic behavior of the pillared-layer MOF, MOF-2-Zn, in a single-crystal-to-single-crystal (SC-to-SC) manner during solvent exchange and removal processes. The latter part of the thesis focuses on utilizing amine-tethered MOF for capturing CO2, aiming to understand long-term material behavior and performance when employed under realistic DAC working conditions. The results presented in this study highlight various obstacles facing the practical implementation of studied amine-tethered MOF for DAC. These challenges include kinetic limitations and inadequate hydrolytic stability, emphasizing that these critical aspects should be focused more on developing practical DAC materials.


Keywords: carbon capture and storage; carbon dioxide; sorption; recovery (recapture); air; amines; ligands; doctoral dissertations

Free keywords: Direct Air Capture (DAC); metal-organic frameworks (MOF); noncovalent interactions; single-crystal to-single-crystal transformation; CO2 adsorptio


Contributing organizations


Ministry reporting: Yes

VIRTA submission year: 2024


Last updated on 2024-14-10 at 15:09