Functionalization of Metal-Organic Framework Nanochannels for Water Transport and Purification

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Functionalization of Metal-Organic Framework Nanochannels for Water Transport and Purification

Li, F; Hanna, G; Yücesan, G; Yazaydin, AO; (2022) Functionalization of Metal-Organic Framework Nanochannels for Water Transport and Purification. ACS Applied Nano Materials , 6 (4) pp. 3003-3011. 10.1021/acsanm.2c05389. Green open access

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Abstract

Artificial water nanochannels (AWCs) have drawn great attention due to their potential use in water purification. Herein, we propose an AWC design, which is based on coordinatively functionalizing unsaturated metal sites found in metal-organic frameworks (MOFs) with one-dimensional nanochannels. As a computational demonstration, we consider two MOFs, namely, Ni-CPO-27 and Ni-CPO-54, and graft proline, imidazolecarboxylic acid, imidazolecarboxaldehyde, pyrazolecarboxylic acid, and pyrazole carbaldehyde molecules into the MOF nanochannels. To assess the strength of the molecule-metal binding, binding energies were calculated using density functional theory. The results indicate that the MOFs containing either proline or 2-imidazolecarboxylic acid form water-stable AWCs with binding energies twice that of the binding energy of water. To shed light on the water diffusion mechanism in the proline-Ni-CPO-27/54 and 2-imidazolecarboxylic-Ni-CPO-27/54 AWCs, molecular dynamics simulations were performed to calculate the mean-squared displacement of water molecules and nonbonded interaction energies between select pairs of atoms in water and coordinated molecules were analyzed. It was found that the fastest water diffusion occurs in proline-Ni-CPO-54 with a self-diffusion coefficient of 7.2 ± 0.5 × 10-8 cm2/s. In comparison, the fastest water self-diffusion coefficient reported in a carbon nanotube-based AWC is 9 × 10-6 cm2/s. Nonbonded interactions between specific atom pairs regulate water diffusion in the functionalized MOF nanochannels. In particular, the change in water mean-squared displacement with changing water loading correlates well with the nonbonded energies between the partially positively charged hydrogen atoms in water and the partially negatively charged oxygen and nitrogen atoms in the proline and 2-imidazolecarboxylic acid molecules. The results presented herein indicate that water-stable MOFs could perform well as AWCs, thereby lending support to the further design and synthesis of MOF-based AWCs for water purification.

Type:	Article
Title:	Functionalization of Metal-Organic Framework Nanochannels for Water Transport and Purification
Open access status:	An open access version is available from UCL Discovery
DOI:	10.1021/acsanm.2c05389
Publisher version:	https://doi.org/10.1021/acsanm.2c05389
Language:	English
Additional information:	This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Keywords:	artificial water nanochannels, metal−organic frameworks, aquaporins, water diffusion, molecular dynamics simulations
UCL classification:	UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI:	https://discovery.ucl.ac.uk/id/eprint/10166453