Journal
ADVANCED MATERIALS INTERFACES
Volume 9, Issue 16, Pages -Publisher
WILEY
DOI: 10.1002/admi.202200337
Keywords
2D materials; charge transfer; iodine capture; mechanical exfoliation; metal-organic nanosheets
Funding
- Science and Engineering Research Board (SERB), New Delhi [SB/S2/JCB-52/2014]
- SERB, New Delhi [SERB/CHM/2018575]
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A layered metal-organic framework (MOF), Cd-BPDP, was synthesized using a metal-assisted self-assembly method. The MOF was then exfoliated into porous 2D metal-organic nanosheets (MONs) through ultrasonication and mechanical grinding techniques. The resulting MONs showed significant iodine capture ability, attributed to the increased surface area, charge-transfer complex formation, and reinforced binding of iodine through charge transfer.
An electron-rich pi-conjugated organic linker H4BPDP (BPDP = biphenyl dipyrrole tetracarboxylic acid) is designed and subjected to metal-assisted self-assembly to afford a layered metal-organic framework (MOF), i.e., Cd-BPDP. Single crystal X-ray structure determination and analysis show that two corrugated layers of the MOF are intertwined to yield thick strands of porous 2D metal-organic nanosheets (MONs). It is shown that the latter can be delaminated by ultrasonication-induced liquid-phase exfoliation and mechanical grinding techniques, as evidenced by Tyndall light scattering and comprehensive microscopy investigations that include field emission scanning electron microscopy (FESEM), atomic force microscopy, and high-resolution transmission electron microscopy. The MONs accessed by grinding permit notable capture of iodine when compared to the bulk layered MOF, i.e., Cd-BPDP; the extent of iodine capture can be correlated with the magnitude exfoliation, which is essentially determined by the duration of grinding. The observed notable iodine capture is attributed to i) a large increase in surface area with exfoliation, ii) ability of the e-rich pi-conjugated organic linker to form a charge-transfer complex with iodine, and iii) the presence of free and uncoordinated carboxylic acids of the linker that reinforce binding of iodine through charge transfer. Thus, a notable capture of iodine by 2D MONs generated by mechanical exfoliation of a layered MOF constructed from an e-rich pi-extended organic linker is compellingly demonstrated.
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