Unique design of superior metal-organic framework for removal of toxic chemicals in humid environment via direct functionalization of the metal nodes

Ga Young Cha, Hoje Chun, Do Young Hong, Jaegyeom Kim, Kyung Ho Cho, U. Hwang Lee, Jong San Chang, Sam Gon Ryu, Hae Wan Lee, Seung Joo Kim, Byungchan Han, Young Kyu Hwang

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Abstract

Unique chemical and thermal stabilities of a zirconium-based metal-organic framework (MOF) and its functionalized analogues play a key role to efficiently remove chemical warfare agents (ex., cyanogen chloride, CNCl) and simulant (dimethyl methylphosphonate, DMMP) as well as industrial toxic gas, ammonia (NH3). Herein, we for the first time demonstrate outstanding performance of MOF-808 for removal of toxic chemicals in humid environment via special design of functionalization of hydroxo species bridging Zr-nodes using a triethylenediamine (TEDA) to form ionic frameworks by gas phase acid-base reactions. In situ experimental analyses and first-principles density functional theory calculations unveil underlying mechanism on the selective deposition of TEDA on the Zr-bridging hydroxo sites (μ3-OH) in Zr-MOFs. The crystal structure of TEDA-grafted MOF-808 was confirmed using synchrotron X-ray powder diffraction (SXRPD). Furthermore, operando FT-IR spectra elucidate why the TEDA-grafted MOF-808 shows by far superior sorption efficiency to other MOF varieties. This work provides design principles and applications how to optimize MOFs for the preparation for versatile adsorbents using diamine grafting chemistry, which is also potentially applicable to various catalysis.

Original languageEnglish
Article number122857
JournalJournal of Hazardous Materials
Volume398
DOIs
Publication statusPublished - 2020 Nov 5

All Science Journal Classification (ASJC) codes

  • Environmental Engineering
  • Environmental Chemistry
  • Waste Management and Disposal
  • Pollution
  • Health, Toxicology and Mutagenesis

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    Cha, G. Y., Chun, H., Hong, D. Y., Kim, J., Cho, K. H., Lee, U. H., Chang, J. S., Ryu, S. G., Lee, H. W., Kim, S. J., Han, B., & Hwang, Y. K. (2020). Unique design of superior metal-organic framework for removal of toxic chemicals in humid environment via direct functionalization of the metal nodes. Journal of Hazardous Materials, 398, [122857]. https://doi.org/10.1016/j.jhazmat.2020.122857