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Selective decontamination of the reactive air pollutant nitrous acid via node-linker cooperativity in a metal-organic framework.

ABSTRACT: Nitrous acid (HONO) is a reservoir of NO _x and an emerging pollutant having direct impacts on air quality, both in- and outdoors, as well as on human health. In this work, the amine-functionalized metal-organic framework (MOF), UiO-66-NH₂, was investigated due to its potential to selectively decontaminate nitrous acid at environmentally relevant concentrations. UiO-66-NH₂ proved to be effective in the removal of nitrous acid from a continuous gaseous stream. This is observed via the formation of an aryl diazonium salt that subsequently converts to a phenol with a concomitant release of nitrogen gas. This process is preceded via the formation of the nitrosonium cation (likely protonation from an acidic proton on the node). Thus, UiO-66-NH₂ is capable of selectively converting the pollutant nitrous acid to benign products.

SUBMITTER: McGrath DT

PROVIDER: S-EPMC6553375 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

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Selective decontamination of the reactive air pollutant nitrous acid via node-linker cooperativity in a metal-organic framework.

McGrath Devon T DT Ryan Michaela D MD MacInnis John J JJ VandenBoer Trevor C TC Young Cora J CJ Katz Michael J MJ

Chemical science 20190429 21

Nitrous acid (HONO) is a reservoir of NO x and an emerging pollutant having direct impacts on air quality, both in- and outdoors, as well as on human health. In this work, the amine-functionalized metal-organic framework (MOF), UiO-66-NH2, was investigated due to its potential to selectively decontaminate nitrous acid at environmentally relevant concentrations. UiO-66-NH2 proved to be effective in the removal of nitrous acid from a continuous gaseous strea ...[more]

PMID: 31293741

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Project description:Solvent-assisted ligand incorporation (SALI) of the ditopic linker 5-carboxy-3-(4-carboxybenzyl)thiazolium bromide [(H2PhTz)Br] into the zirconium metal-organic framework NU-1000 [Zr6O4(OH)8(H2O)4(TBAPy)2, where NU = Northwestern University and H4TBAPy = 1,3,6,8-tetrakis(p-benzoic-acid)pyrene], led to the SALIed NU-1000-PhTz material of minimal formula [Zr6O4(OH)6(H2O)2(TBAPy)2(PhTz)]Br. NU-1000-PhTz has been thoroughly characterized in the solid state. As confirmed by powder X-ray diffraction, this material keeps the same three-dimensional architecture of NU-1000 and the dicarboxylic extra linker bridges adjacent [Zr6] nodes ca. 8 Å far apart along the crystallographic c-axis. The functionalized MOF has a BET specific surface area of 1560 m2/g, and it is featured by a slightly higher thermal stability than its parent material (Tdec = 820 vs. 800 K, respectively). NU-1000-PhTz has been exploited for the capture and separation of two pollutant gases: carbon dioxide (CO2) and nitrous oxide (N2O). The high thermodynamic affinity for both gases [isosteric heat of adsorption (Qst) = 25 and 27 kJ mol-1 for CO2 and N2O, respectively] reasonably stems from the strong interactions between these (polar) "stick-like" molecules and the ionic framework. Intriguingly, NU-1000-PhTz shows an unprecedented temperature-dependent adsorption capacity, loading more N2O in the 298 K ≤ T ≤ 313 K range but more CO2 at temperatures falling out of this range. Grand canonical Monte Carlo simulations of the adsorption isotherms confirmed that the preferential adsorption sites of both gases are the triangular channels (micropores) in close proximity to the polar pillar. While CO2 interacts with the thiazolium ring in an "end-on" fashion through its O atoms, N2O adopts a "side-on" configuration through its three atoms simultaneously. These findings open new horizons in the discovery of functional materials that may discriminate between polluting gases through selective adsorption at different temperatures.

Dataset Information

Selective decontamination of the reactive air pollutant nitrous acid via node-linker cooperativity in a metal-organic framework.

Publications

Selective decontamination of the reactive air pollutant nitrous acid <i>via</i> node-linker cooperativity in a metal-organic framework.

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