Integration of Metal-Organic Frameworks with Electrospun Fibers for Heavy Metal Removal and Carbon Dioxide Capture

The increasing levels of atmospheric CO2 and the widespread contamination of water sources with toxic heavy metals represent two of the most pressing environmental challenges of the 21st century. Efficient and scalable materials capable of capturing CO2 and removing pollutants such as Pb(II) and Cu(II) are urgently needed to mitigate climate change and safeguard public health. In this context, advanced porous materials such as metal–organic frameworks (MOFs) have gained significant attention due to their exceptionally high surface area, tunable porosity, and structural versatility. However, the practical use of MOFs remains limited by their powder form, which complicates processing and application in separation systems. Electrospinning, a versatile and scalable technique for producing nanofibrous membranes with high surface-to-volume ratio, offers a promising strategy to immobilize MOFs in structured and processable forms. This thesis investigates the integration of MOFs with electrospun polymer fibers to develop multifunctional composites for CO2 adsorption and heavy metal removal. Two approaches were explored: direct electrospinning of pre-synthesized MOFs with polymer solutions and in situ growth of MOFs on electrospun mats. For the first time, CALF-20, a Zn-based MOF originally designed for CO2 capture, was incorporated into polyacrylonitrile (PAN) fibers via direct electrospinning. The resulting composites showed high structural integrity with up to 60 wt.% loading and demonstrated excellent removal capacities for Pb(II) and Cu(II), achieving 248.3 mg/g and 128.2 mg/g, respectively. In situ growth of ZIF-67 on electrospun PAN and PVDF fibers was systematically investigated, revealing that solvent type, precursor concentration, and synthesis time strongly influenced particle morphology, crystallinity, and CO2 adsorption performance. Furthermore, the novel in situ growth of CALF-20 on PAN fibers was successfully demonstrated, providing improved accessibility of MOF active sites and enhanced CO2 capture compared to direct electrospinning. Overall, this research introduces new strategies for integrating MOFs with electrospun nanofibers and establishes their advantages over MOFs in powder form or traditional mixed-matrix membranes. By addressing key challenges related to stability, processability, and performance, this work advances the development of scalable MOF–fiber composites as promising materials for next-generation environmental remediation technologies.

Name thesis:degree_name

Doctor of Philosophy (PhD)

Discipline thesis:degree_discipline

Engineering – Chemical & Petroleum

Grantor

Schulich School of Engineering

Year dc:date.issued

2026

Author dc:creator

• Melo, Guilherme Henrique França

Advisor dc:contributor.advisor

• Sundararaj, Uttandaraman

Committee members dc:contributor.committeemember

• Lu, Qingye Gemma
• Shimizu, George Kisa Hayashi

• electrospinning
• metal-organic framework
• MOF
• CO2 capture
• heavy metal removal

Statement dc:rights

• Unless otherwise indicated, this material is protected by copyright and has been made available with authorization from the copyright owner. You may use this material in any way that is permitted by the Copyright Act or through licensing that has been assigned to the document. For uses that are not allowable under copyright legislation or licensing, you are required to seek permission.

Language dc:language.iso

en

DOI

https://dx.doi.org/10.11575/PRISM/51039

OAI identifier oai:identifier

oai:ucalgary.scholaris.ca:1880/124029