Molecular insights into the in situ early-stage assembly of metal–organic frameworks on cellulose nanofibrils

Zhang, Kailong; Smith, Micholas Dean; Li, Mi

doi:10.1039/d4ta05512h

Title: Molecular insights into the in situ early-stage assembly of metal–organic frameworks on cellulose nanofibrils

Journal Article · 06 November 2024 · Journal of Materials Chemistry. A

DOI: https://doi.org/10.1039/d4ta05512h · OSTI ID:2480013

Zhang, Kailong ^[1]; Smith, Micholas Dean ^[1];

^[1]

University of Tennessee, Knoxville, TN (United States)

The integration of metal–organic frameworks (MOFs) into renewable matrices, including those derived from cellulose, to create cellulose/MOF hybrids has attracted significant interest due to the synergistic combination of cellulosic biopolymer properties and MOFs' multifunctional features. The interfacial interactions between cellulose and MOF not only ensure stable bonding, but ultimately also determine the bulk physical properties of the macroscopic composites. However, the mechanistic understanding of the in situ assembly between the two materials remains unclear. In this study, we employ a combination study of synthesis, experimental characterization, and molecular dynamics simulations to explore the early-stage assembly of a cellulose/MOF hybrid. Our results revealed that the growth of MOF clusters on the 2,2,6,6-tetramethyl-1-piperidinyloxy oxidized cellulose nanofibrils (TOCNF) follows an inhomogeneous sequential transformation pathway. The carboxylates of TOCNF form coordination-like bonds with the metal ions, while the hydroxyl groups of TOCNF form hydrogen bonds with MOF ligands. These interactions provide the initial nucleation sites that mediate the growth of MOF clusters and also guide the assembly of larger MOF clusters onto the TOCNF substrate. In conclusion, the fundamental insights into the in situ assembly of MOF nanoparticles on cellulosic substrates are essential for the rational design of high-performance materials with tailored morphology and optimized properties.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); South-Eastern Regional Sun Grant Center

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2480013

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 47 Vol. 12; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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