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Large-Scale, One-Pot Synthesis of Imine/ β-Ketoenamine-Linked COF Gels in Aqueous Systems for Wastewater Purification
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.ORCID iD: 0000-0001-6922-9477
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.ORCID iD: 0009-0002-4231-4254
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Nanotechnology and Functional Materials.ORCID iD: 0000-0002-1587-8073
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Water contamination by organic dyes, heavy metal ions, and nanoscale particles poses a severe threat to ecosystems and human health, necessitating the development of versatile and robust filtration materials. Covalent organic frameworks (COFs), with their high porosity, tunable surface chemistry, and structural diversity, offer unique opportunities for multifunctional water purification. Here, we report a facile, one-pot, and scalable aqueous synthesis of imine- and β-ketoenamine-linked COFs in the form of freestanding, mechanically robust gels. A total of 31 freestanding COF gels with different molecular structures were successfully obtained, including 25 that are highly crystalline and 6 that are less crystalline or amorphous. Systematic investigation of synthesis conditions revealed that the type of linkage and reaction temperature significantly influenced the gelation process: room temperature favored imine-linked COF gels, whereas elevated temperature promoted β- ketoenamine-linked COF formation. The resulting COF gels exhibited high surface areas (up to 2127 m²/g), tunable pore sizes, and robust elastic networks. Taking advantage of their hierarchical porosity and high stability, the COF gels were employed in a filtration system, which enabled efficient removal of diverse pollutants, including Rhodamine B, Cr³⁺ ions, and ultrafine particles under continuous flow. These findings establish aqueous synthesis and shaping of COF materials as multifunctional platforms for next-generation water purification, capable of efficiently removing diverse pollutants and suitable for applications in industrial wastewater treatment, environmental remediation, and potable water production.

National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-567643OAI: oai:DiVA.org:uu-567643DiVA, id: diva2:1999663
Available from: 2025-09-22 Created: 2025-09-22 Last updated: 2025-09-22
In thesis
1. Scalable Fabrication of Structured Covalent Organic Frameworks for Chemical Separation
Open this publication in new window or tab >>Scalable Fabrication of Structured Covalent Organic Frameworks for Chemical Separation
2025 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

 Large-scale chemical separations underpin modern industry yet consume 10–15% of global energy, driving the need to replace thermal operations with membrane- and sorbent-based alternatives of higher efficiency. This thesis advances covalent organic frameworks (COFs) toward practical deployment by focusing on scalable fabrication and processing routes that preserve performance while enabling industrial integration. The intrinsic advantages of COFs—uniform porosity, tunability, and stability—are outlined alongside application-driven requirements for separation materials and processes. For membranes, this entails ultrathin, defect-free active layers on robust supports compatible with continuous manufacturing; for sorbents, it requires short diffusion pathways, macroscopic structure, and low-cost, high-throughput fabrication. A critical survey of fabrication strategies identifies nanosheet assembly and support-infusion liquid–liquid interfacial polymerization as promising continuous routes for COF membranes, while highlighting time and footprint reduction as key issues for structured COF sorbent fabrication. Two novel, scalable fabrication strategies are introduced: (i) a precursor-casting method yielding continuous sub-micron β-ketoenamine COF films, adapted to manufacture thin-film composite membranes on polymeric substrates; and (ii) a gel-based approach for imine and β-ketoenamine COFs, producing hierarchically porous sorbents with rapid adsorption kinetics. To enable robust membrane evaluation, a low-cost pressure-driven filtration system was designed and constructed to support extended nanofiltration studies. The findings suggest that near-term industrial impact is most likely in organic-solvent nanofiltration and selective metal-ion adsorption, where COFs’ robustness and modularity provide distinct benefits. Practical constraints—including monomer cost, solvent use, and heating requirements—are examined with potential mitigation pathways. Collectively, the results outline design and manufacturing considerations that chart a pragmatic route from laboratory scale to industrial implementation of COF membranes and sorbents.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2025. p. 80
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 2592
Keywords
Covalent organic frameworks, Membrane separation, Scalable fabrication, Energy-efficient separations, COF synthesis, COF processing
National Category
Materials Chemistry Separation Processes
Research subject
Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-567805 (URN)978-91-513-2600-9 (ISBN)
Public defence
2025-11-07, Ångström 4101, Regementsvägen 10, Uppsala, 09:15 (English)
Opponent
Supervisors
Available from: 2025-10-16 Created: 2025-09-22 Last updated: 2025-10-16

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Kong, XueyingEliasson, KasperÅhlén, MichelleXu, Chao

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