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Fine-tuning covalent organic frameworks for structure-activity correlation via adsorption and catalytic studies.
- Source :
-
Journal of Colloid & Interface Science . Jul2024, Vol. 665, p988-998. 11p. - Publication Year :
- 2024
-
Abstract
- [Display omitted] In applications utilizing Covalent Organic Frameworks (COFs) for adsorption, the interplay between crystallinity (vis-à-vis surface area) and active sites still remains ambiguous. To address this, the present study introduces three isoreticular COFs—COP-N18 (covalent organic polymer with short-range order), COF-N18 (COF having long-range order), and COF-N27 (semicrystalline COF with pyridyl heteroatoms)—to explore this duality. Through systematic variations in structural order, pore volume, and pore-wall nitrogen content, we aim to establish a structure–activity relationship (SAR) for these COFs via adsorption and catalysis, using CO 2 and I 2 as probes. Our investigation highlights the positive influence of crystallinity, surface area, and pore volume in adsorption as well as catalysis. However, the presence of heteroatoms manifests complex behavior in CO 2 adsorption and CO 2 cycloaddition reactions with epoxides. COF-N18 and COF-N27 showed comparable CO 2 uptake capacities at different temperatures (273, 293, and 313 K) and ∼1 bar pressure. Additionally, CO 2 cycloaddition reactions were performed with substrates possessing different polarities (epichlorohydrin, 1,2-epoxydodecane) to elucidate the role of COF surface polarity. Further investigation into iodine adsorption was performed to understand the impact of COF structural features on the modes of adsorption and adsorption kinetics. Improvements in COF-crystallinity results in faster average iodine uptake rate at 80% (K 80% = 1.79 g/h) by COF-N18. Whereas, heteroatom doping slows down iodine adsorption kinetics (0.35 g/h) by prolonging the adsorption process up to 72 h. Overall, this study advances our understanding of COFs as adsorbents and catalysts, providing key insights into their SAR while emphasizing structural fine-tuning as a key factor for impactful environmental applications. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 00219797
- Volume :
- 665
- Database :
- Academic Search Index
- Journal :
- Journal of Colloid & Interface Science
- Publication Type :
- Academic Journal
- Accession number :
- 176546052
- Full Text :
- https://doi.org/10.1016/j.jcis.2024.03.077