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/anie.202102956

Title: 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 (International Edition)

DOI:https://doi.org/10.1002/anie.202102956· OSTI ID:1775005

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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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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)

Grant/Contract Number:: AC04-94AL85000; SC0012577; NA0003525

OSTI ID:: 1775005

Alternate ID(s):: OSTI ID: 1775007; OSTI ID: 1778047

Report Number(s):: SAND-2021-3859J

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Vol. 60 Journal Issue: 20; ISSN 1433-7851

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

Country of Publication:: Germany

Language:: English

References (38)

NO _x Adsorption and Optical Detection in Rare Earth Metal–Organic Frameworks Sava Gallis, Dorina F.; Vogel, Dayton J.; Vincent, Grace A. ACS Applied Materials & Interfaces, Vol. 11, Issue 46 https://doi.org/10.1021/acsami.9b16470	journal	October 2019
Effect of Metal in M ₃ (btc) ₂ and M ₂ (dobdc) MOFs for O ₂ /N ₂ Separations: A Combined Density Functional Theory and Experimental Study Parkes, Marie V.; Sava Gallis, Dorina F.; Greathouse, Jeffery A. The Journal of Physical Chemistry C, Vol. 119, Issue 12 https://doi.org/10.1021/jp511789g	journal	March 2015
Book review of “Lanthanide metal-organic frameworks” Borovkov, Victor Frontiers in Chemistry, Vol. 3 https://doi.org/10.3389/fchem.2015.00050	journal	August 2015
Luminescent Properties of DOBDC Containing MOFs: The Role of Free Hydroxyls Henkelis, Susan E.; Rademacher, David; Vogel, Dayton J. ACS Applied Materials & Interfaces, Vol. 12, Issue 20 https://doi.org/10.1021/acsami.0c02829	journal	April 2020
Pollution characteristics and potential sources of nitrous acid (HONO) in early autumn 2018 of Beijing Jia, Chenhui; Tong, Shengrui; Zhang, Wenqian Science of The Total Environment, Vol. 735 https://doi.org/10.1016/j.scitotenv.2020.139317	journal	September 2020
Topologically guided tuning of Zr-MOF pore structures for highly selective separation of C6 alkane isomers Wang, Hao; Dong, Xinglong; Lin, Junzhong Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04152-5	journal	May 2018
Defects and disorder in metal organic frameworks Cheetham, Anthony K.; Bennett, Thomas D.; Coudert, François-Xavier Dalton Transactions, Vol. 45, Issue 10 https://doi.org/10.1039/C5DT04392A	journal	January 2016
Magnetic Tunability in RE-DOBDC MOFs via NO _x Acid Gas Adsorption Henkelis, Susan E.; Huber, Dale L.; Vogel, Dayton J. ACS Applied Materials & Interfaces, Vol. 12, Issue 17 https://doi.org/10.1021/acsami.0c01813	journal	April 2020
Multifunctional, Tunable Metal–Organic Framework Materials Platform for Bioimaging Applications Sava Gallis, Dorina F.; Rohwer, Lauren E. S.; Rodriguez, Mark A. ACS Applied Materials & Interfaces, Vol. 9, Issue 27 https://doi.org/10.1021/acsami.7b05859	journal	June 2017
Nitrogen and sulphur chemistry in pressurised flue gas systems: A comparison of modelling and experiments Normann, Fredrik; Jansson, Erik; Petersson, Tobias International Journal of Greenhouse Gas Control, Vol. 12 https://doi.org/10.1016/j.ijggc.2012.11.012	journal	January 2013
Interaction of Acid Gases SO ₂ and NO ₂ with Coordinatively Unsaturated Metal Organic Frameworks: M-MOF-74 (M = Zn, Mg, Ni, Co) Tan, Kui; Zuluaga, Sebastian; Wang, Hao Chemistry of Materials, Vol. 29, Issue 10 https://doi.org/10.1021/acs.chemmater.7b00005	journal	May 2017
SO _x /NO _x Removal from Flue Gas Streams by Solid Adsorbents: A Review of Current Challenges and Future Directions Rezaei, Fateme; Rownaghi, Ali A.; Monjezi, Saman Energy & Fuels, Vol. 29, Issue 9 https://doi.org/10.1021/acs.energyfuels.5b01286	journal	August 2015
Predictive Acid Gas Adsorption in Rare Earth DOBDC Metal–Organic Frameworks via Complementary Cluster and Periodic Structure Models Vogel, Dayton J.; Lee, Zachary R.; Hanson, Caitlin A. The Journal of Physical Chemistry C, Vol. 124, Issue 49 https://doi.org/10.1021/acs.jpcc.0c08282	journal	November 2020
H ₂ O Adsorption/Desorption in MOF-74: Ab Initio Molecular Dynamics and Experiments Li, Yunsong; Wang, Xinjiang; Xu, Dongyan The Journal of Physical Chemistry C, Vol. 119, Issue 23 https://doi.org/10.1021/acs.jpcc.5b02069	journal	May 2015
Actinide-based MOFs: a middle ground in solution and solid-state structural motifs Dolgopolova, Ekaterina A.; Rice, Allison M.; Shustova, Natalia B. Chemical Communications, Vol. 54, Issue 50 https://doi.org/10.1039/C7CC09780H	journal	January 2018
MOFs for CO ₂ capture and separation from flue gas mixtures: the effect of multifunctional sites on their adsorption capacity and selectivity Zhang, Zhijuan; Zhao, Yonggang; Gong, Qihan Chem. Commun., Vol. 49, Issue 7 https://doi.org/10.1039/C2CC35561B	journal	January 2013
Sources of atmospheric nitrous acid: State of the science, current research needs, and future prospects Spataro, Francesca; Ianniello, Antonietta Journal of the Air & Waste Management Association, Vol. 64, Issue 11 https://doi.org/10.1080/10962247.2014.952846	journal	August 2014
Synergistic Reaction of SO2 with NO2 in Presence of H2O and NH3: A Potential Source of Sulfate Aerosol Wang, Zehua; Zhang, Chenxi; Lv, Guochun International Journal of Molecular Sciences, Vol. 20, Issue 15 https://doi.org/10.3390/ijms20153746	journal	July 2019
Elucidating the Breathing of the Metal–Organic Framework MIL-53(Sc) with ab Initio Molecular Dynamics Simulations and in Situ X-ray Powder Diffraction Experiments Chen, Linjiang; Mowat, John P. S.; Fairen-Jimenez, David Journal of the American Chemical Society, Vol. 135, Issue 42 https://doi.org/10.1021/ja403453g	journal	June 2013
Recent advances in gas storage and separation using metal–organic frameworks Li, Hao; Wang, Kecheng; Sun, Yujia Materials Today, Vol. 21, Issue 2 https://doi.org/10.1016/j.mattod.2017.07.006	journal	March 2018
Stability of Supported Amine Adsorbents to SO ₂ and NO _x in Postcombustion CO ₂ Capture. 1. Single-Component Adsorption Rezaei, Fateme; Jones, Christopher W. Industrial & Engineering Chemistry Research, Vol. 52, Issue 34 https://doi.org/10.1021/ie4019116	journal	August 2013
Structure and electronic properties of rare earth DOBDC metal–organic-frameworks Vogel, Dayton J.; Sava Gallis, Dorina F.; Nenoff, Tina M. Physical Chemistry Chemical Physics, Vol. 21, Issue 41 https://doi.org/10.1039/C9CP04038B	journal	January 2019
Metal–Organic Frameworks for Separations Li, Jian-Rong; Sculley, Julian; Zhou, Hong-Cai Chemical Reviews, Vol. 112, Issue 2, p. 869-932 https://doi.org/10.1021/cr200190s	journal	September 2011
Research Challenges in Avoiding “Showstoppers” in Developing Materials for Large-Scale Energy Applications Walton, Krista S.; Sholl, David S. Joule, Vol. 1, Issue 2 https://doi.org/10.1016/j.joule.2017.06.005	journal	October 2017
Efficient MOF-based degradation of organophosphorus compounds in non-aqueous environments Sava Gallis, Dorina F.; Harvey, Jacob A.; Pearce, Charles J. Journal of Materials Chemistry A, Vol. 6, Issue 7 https://doi.org/10.1039/C7TA10794C	journal	January 2018
Selective gas adsorption and separation in metal–organic frameworks Li, Jian-Rong; Kuppler, Ryan J.; Zhou, Hong-Cai Chemical Society Reviews, Vol. 38, Issue 5, p. 1477-1504 https://doi.org/10.1039/b802426j	journal	January 2009
Interactions of NO ₂ with Zr-Based MOF: Effects of the Size of Organic Linkers on NO ₂ Adsorption at Ambient Conditions Ebrahim, Amani M.; Levasseur, Benoit; Bandosz, Teresa J. Langmuir, Vol. 29, Issue 1 https://doi.org/10.1021/la302869m	journal	December 2012
Density Functional Theory Study of Hydrogen Adsorption in a Ti-Decorated Mg-Based Metal-Organic Framework-74 Suksaengrat, Pitphichaya; Amornkitbamrung, Vittaya; Srepusharawoot, Pornjuk ChemPhysChem, Vol. 17, Issue 6 https://doi.org/10.1002/cphc.201500981	journal	January 2016
Rotational Dynamics of Linkers in Metal–Organic Frameworks Gonzalez-Nelson, Adrian; Coudert, François-Xavier; van der Veen, Monique Nanomaterials, Vol. 9, Issue 3 https://doi.org/10.3390/nano9030330	journal	March 2019
Thermochemistry for enthalpies and reaction paths of nitrous acid isomers Asatryan, Rubik; Bozzelli, Joseph W.; Simmie, John M. International Journal of Chemical Kinetics, Vol. 39, Issue 7 https://doi.org/10.1002/kin.20247	journal	January 2007
Formation of nitrous acid and nitric oxide in the heterogeneous dark reaction of nitrogen dioxide and water vapor in a smog chamber Sakamaki, Fumio; Hatakeyama, Shiro; Akimoto, Hajime International Journal of Chemical Kinetics, Vol. 15, Issue 10 https://doi.org/10.1002/kin.550151006	journal	October 1983
Rotational dynamics of the organic bridging linkers in metal–organic frameworks and their substituent effects on the rotational energy barrier Pakhira, Srimanta RSC Advances, Vol. 9, Issue 65 https://doi.org/10.1039/C9RA01288E	journal	January 2019
Defect and Linker Effects on the Binding of Organophosphorous Compounds in UiO-66 and Rare-Earth MOFs Harvey, Jacob A.; Greathouse, Jeffery A.; Sava Gallis, Dorina F. The Journal of Physical Chemistry C, Vol. 122, Issue 47 https://doi.org/10.1021/acs.jpcc.8b06198	journal	November 2018
Ab initio molecular dynamics determination of competitive O ₂ vs. N ₂ adsorption at open metal sites of M ₂ (dobdc) Parkes, Marie V.; Greathouse, Jeffery A.; Hart, David B. Physical Chemistry Chemical Physics, Vol. 18, Issue 16 https://doi.org/10.1039/C6CP00768F	journal	January 2016
Competitive Coadsorption of CO ₂ with H ₂ O, NH ₃ , SO ₂ , NO, NO ₂ , N ₂ , O ₂ , and CH ₄ in M-MOF-74 (M = Mg, Co, Ni): The Role of Hydrogen Bonding Tan, Kui; Zuluaga, Sebastian; Gong, Qihan Chemistry of Materials, Vol. 27, Issue 6 https://doi.org/10.1021/acs.chemmater.5b00315	journal	March 2015
Covalent radii revisited Cordero, Beatriz; Gómez, Verónica; Platero-Prats, Ana E. Dalton Transactions, Issue 21 https://doi.org/10.1039/b801115j	journal	January 2008
Tuned Hydrogen Bonding in Rare-Earth Metal–Organic Frameworks for Design of Optical and Electronic Properties: An Exemplar Study of Y–2,5-Dihydroxyterephthalic Acid Vogel, Dayton J.; Nenoff, Tina M.; Rimsza, Jessica M. ACS Applied Materials & Interfaces, Vol. 12, Issue 4 https://doi.org/10.1021/acsami.9b20513	journal	January 2020
Selective decontamination of the reactive air pollutant nitrous acid via node-linker cooperativity in a metal–organic framework McGrath, Devon T.; Ryan, Michaela D.; MacInnis, John J. Chemical Science, Vol. 10, Issue 21 https://doi.org/10.1039/C9SC01357A	journal	January 2019

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