TY - JOUR
T1 - Balancing Pore Accessibility and Hydrophobicity for Enhanced Perfluorooctanoic Acid Removal
T2 - A Case Study on NU-1000
AU - Alkhatib, Nour
AU - Yazaydin, A. Ozgur
AU - Kirmizialtin, Serdal
N1 - Publisher Copyright:
© 2025 The Authors. Published by American Chemical Society.
PY - 2025/6/10
Y1 - 2025/6/10
N2 - Perfluorooctanoic acid (PFOA), a persistent pollutant from the PFCA class, poses significant environmental and health risks due to its resistance to degradation. Metal-organic frameworks (MOFs) offer a promising solution for removing PFOA from water; however, the mechanisms underlying PFOA uptake and the optimization of MOFs for this application remain unclear. In this study, we explore the adsorption mechanism of PFOA on NU-1000, a zirconium-based MOF, using molecular dynamics (MD) simulations conducted in an explicit water environment to replicate realistic conditions. Our findings, consistent with experimental observations, provide atomistic insights into PFOA adsorption, identifying hydrophobic interactions as key drivers of its removal. Leveraging these insights, we propose two functionalization strategies using the SALI method. Among these, NU-F, the MOF functionalized with fluorobenzoate ligands, exhibits superior PFOA uptake across all tested concentrations, achieving a higher removal efficiency and faster adsorption kinetics. The enhanced performance of NU-F is attributed to its optimal balance of hydrophobic interactions and efficient pore utilization. This study underscores the importance of rational functionalization in MOF design for environmental remediation and offers a promising pathway for developing advanced adsorbents targeting PFOA and other PFCAs pollutants.
AB - Perfluorooctanoic acid (PFOA), a persistent pollutant from the PFCA class, poses significant environmental and health risks due to its resistance to degradation. Metal-organic frameworks (MOFs) offer a promising solution for removing PFOA from water; however, the mechanisms underlying PFOA uptake and the optimization of MOFs for this application remain unclear. In this study, we explore the adsorption mechanism of PFOA on NU-1000, a zirconium-based MOF, using molecular dynamics (MD) simulations conducted in an explicit water environment to replicate realistic conditions. Our findings, consistent with experimental observations, provide atomistic insights into PFOA adsorption, identifying hydrophobic interactions as key drivers of its removal. Leveraging these insights, we propose two functionalization strategies using the SALI method. Among these, NU-F, the MOF functionalized with fluorobenzoate ligands, exhibits superior PFOA uptake across all tested concentrations, achieving a higher removal efficiency and faster adsorption kinetics. The enhanced performance of NU-F is attributed to its optimal balance of hydrophobic interactions and efficient pore utilization. This study underscores the importance of rational functionalization in MOF design for environmental remediation and offers a promising pathway for developing advanced adsorbents targeting PFOA and other PFCAs pollutants.
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U2 - 10.1021/acs.chemmater.5c00246
DO - 10.1021/acs.chemmater.5c00246
M3 - Article
AN - SCOPUS:105006937101
SN - 0897-4756
VL - 37
SP - 4027
EP - 4037
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 11
ER -