Prediction of Reactive Nitrous Acid Formation in Rare‐Earth MOFs via ab initio Molecular Dynamics

Vogel, Dayton J.; Rimsza, Jessica M.; Nenoff, Tina M.

doi:10.1002/ange.202102956

Prediction of Reactive Nitrous Acid Formation in Rare‐Earth MOFs via ab initio Molecular Dynamics

Journal Article · Thu Apr 08 00:00:00 EDT 2021 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202102956· OSTI ID:1775157

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Nanoscale Sciences Department Sandia National Laboratories Albuquerque NM 87185 USA
Geochemistry Department Sandia National Laboratories Albuquerque NM 87185 USA
Material, Physical, and Chemical Sciences Sandia National Laboratories Albuquerque NM 87185 USA

Abstract

Reactive gas formation in pores of metal–organic frameworks (MOFs) is a known mechanism of framework destruction; understanding those mechanisms for future durability design is key to next generation adsorbents. Herein, an extensive set of ab initio molecular dynamics (AIMD) simulations are used for the first time to predict competitive adsorption of mixed acid gases (NO ₂ and H ₂ O) and the in‐pore reaction mechanisms for a series of rare earth (RE)‐DOBDC MOFs. Spontaneous formation of nitrous acid (HONO) is identified as a result of deprotonation of the MOF organic linker, DOBDC. The unique DOBDC coordination to the metal clusters allows for proton transfer from the linker to the NO ₂ without the presence of H ₂ O and may be a factor in DOBDC MOF durability. This is a previously unreported mechanisms of HONO formation in MOFs. With the presented methodology, prediction of future gas interactions in new nanoporous materials can be achieved.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0012577

OSTI ID:: 1775157

Alternate ID(s):: OSTI ID: 1775158

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 20 Vol. 133; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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