Zirconium‐Based Metal–Organic Frameworks with Free Hydroxy Groups for Enhanced Perfluorooctanoic Acid Uptake in Water

Liang, Rong‐Ran; Yang, Yihao; Han, Zongsu; Bakhmutov, Vladimir I.; Rushlow, Joshua; Fu, Yubin; Wang, Kun‐Yu; Zhou, Hong‐Cai

doi:10.1002/adma.202407194

Zirconium‐Based Metal–Organic Frameworks with Free Hydroxy Groups for Enhanced Perfluorooctanoic Acid Uptake in Water (in EN)

Journal Article · Wed Jun 19 00:00:00 EDT 2024 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202407194· OSTI ID:2377866

Liang, Rong‐Ran ^[1]; Yang, Yihao ^[1]; Han, Zongsu ^[1]; Bakhmutov, Vladimir I. ^[1]; Rushlow, Joshua ^[1]; Fu, Yubin ^[2]; Wang, Kun‐Yu ^[1]; ^[1]

Texas A & M Univ., College Station, TX (United States)
Technische Univ. Dresden (Germany); Max Planck Institute of Microstructure Physics, Weinberg (Germany)

Perfluorooctanoic acid (PFOA) is a highly recalcitrant organic pollutant, and its bioaccumulation severely endangers human health. While various methods are developed for PFOA removal, the targeted design of adsorbents with high efficiency and reusability remains largely unexplored. Here, in this work, the rational design and synthesis of two novel zirconium‐based metal‒organic frameworks (MOFs) bearing free ortho‐hydroxy sites, namely noninterpenetrated PCN‐1001 and twofold interpenetrated PCN‐1002, are presented. Single crystal analysis of the pure ligand reveals that intramolecular hydrogen bonding plays a pivotal role in directing the formation of MOFs with free hydroxy groups. Furthermore, the transformation from PCN‐1001 to PCN‐1002 is realized. Compared to PCN‐1001, PCN‐1002 displays higher chemical stability due to interpenetration, thereby demonstrating an exceptional PFOA adsorption capacity of up to 632 mg g⁻¹ (1.53 mmol g⁻¹), which is comparable to the reported record values. Moreover, PCN‐1002 shows rapid kinetics, high selectivity, and long‐life cycles in PFOA removal tests. Solid‐state nuclear magnetic resonance results and density functional theory calculations reveal that multiple hydrogen bonds between the free ortho‐hydroxy sites and PFOA, along with Lewis acid‐base interaction, work collaboratively to enhance PFOA adsorption.

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Research Organization:: Texas A & M Univ., College Station, TX (United States). Texas A & M AgriLife Research

Sponsoring Organization:: USDOE; USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: FE0032108

OSTI ID:: 2377866

Alternate ID(s):: OSTI ID: 2475699
OSTI ID: 2575780

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 33 Vol. 36; ISSN 1521-4095; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: EN

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collaborative adsorption
free hydroxy groups
interpenetration
metal-organic frameworks
perfluorooctanoic acid uptake

Zirconium‐Based Metal–Organic Frameworks with Free Hydroxy Groups for Enhanced Perfluorooctanoic Acid Uptake in Water (in EN)

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