NOx Adsorption and Optical Detection in Rare Earth Metal–Organic Frameworks
Abstract
Acid gases (e.g., NOx and SOx), commonly found in complex chemical and petrochemical streams, require material development for their selective adsorption and removal. Here, we report the NOx adsorption properties in a family of rare earth (RE) metal–organic frameworks (MOFs) materials. Fundamental understanding of the structure–property relationship of NOx adsorption in the RE-DOBDC materials platform was sought via a combined experimental and molecular modeling study. No structural change was noted following humid NOx exposure. Density functional theory (DFT) simulations indicated that H2O has a stronger affinity to bind with the metal center than NO2, while NO2 preferentially binds with the DOBDC ligands. Further modeling results indicate no change in binding energy across the RE elements investigated. Also, stabilization of the NO2 and H2O molecules following adsorption was noted, predicted to be due to hydrogen bonding between the framework ligands and the molecules and nanoconfinement within the MOF structure. This interaction also caused distinct changes in emission spectra, identified experimentally. As a result, calculations indicated that this is due to the adsorption of NO2 molecules onto the DOBDC ligand altering the electronic transitions and the resulting photoluminescent properties, a feature that has potential applications in future sensing technologies.
- Authors:
-
[1];
[2];
[3]
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Nanoscale Sciences Dept.
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Geochemistry Dept.
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Material, Physical, and Chemical Sciences Center
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1574696
- Report Number(s):
- SAND-2019-10906J
Journal ID: ISSN 1944-8244; 679413
- Grant/Contract Number:
- AC04-94AL85000
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 46; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; metal−organic frameworks; lanthanide; emission; density functional theory; NOx
Citation Formats
Sava Gallis, Dorina F., Vogel, Dayton J., Vincent, Grace A., Rimsza, Jessica M., and Nenoff, Tina M. NOx Adsorption and Optical Detection in Rare Earth Metal–Organic Frameworks. United States: N. p., 2019.
Web. doi:10.1021/acsami.9b16470.
Sava Gallis, Dorina F., Vogel, Dayton J., Vincent, Grace A., Rimsza, Jessica M., & Nenoff, Tina M. NOx Adsorption and Optical Detection in Rare Earth Metal–Organic Frameworks. United States. https://doi.org/10.1021/acsami.9b16470
Sava Gallis, Dorina F., Vogel, Dayton J., Vincent, Grace A., Rimsza, Jessica M., and Nenoff, Tina M. Mon .
"NOx Adsorption and Optical Detection in Rare Earth Metal–Organic Frameworks". United States. https://doi.org/10.1021/acsami.9b16470. https://www.osti.gov/servlets/purl/1574696.
@article{osti_1574696,
title = {NOx Adsorption and Optical Detection in Rare Earth Metal–Organic Frameworks},
author = {Sava Gallis, Dorina F. and Vogel, Dayton J. and Vincent, Grace A. and Rimsza, Jessica M. and Nenoff, Tina M.},
abstractNote = {Acid gases (e.g., NOx and SOx), commonly found in complex chemical and petrochemical streams, require material development for their selective adsorption and removal. Here, we report the NOx adsorption properties in a family of rare earth (RE) metal–organic frameworks (MOFs) materials. Fundamental understanding of the structure–property relationship of NOx adsorption in the RE-DOBDC materials platform was sought via a combined experimental and molecular modeling study. No structural change was noted following humid NOx exposure. Density functional theory (DFT) simulations indicated that H2O has a stronger affinity to bind with the metal center than NO2, while NO2 preferentially binds with the DOBDC ligands. Further modeling results indicate no change in binding energy across the RE elements investigated. Also, stabilization of the NO2 and H2O molecules following adsorption was noted, predicted to be due to hydrogen bonding between the framework ligands and the molecules and nanoconfinement within the MOF structure. This interaction also caused distinct changes in emission spectra, identified experimentally. As a result, calculations indicated that this is due to the adsorption of NO2 molecules onto the DOBDC ligand altering the electronic transitions and the resulting photoluminescent properties, a feature that has potential applications in future sensing technologies.},
doi = {10.1021/acsami.9b16470},
journal = {ACS Applied Materials and Interfaces},
number = 46,
volume = 11,
place = {United States},
year = {2019},
month = {10}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 8 works
Citation information provided by
Web of Science
Web of Science
Figures / Tables:
Figure 1: (a) N2 sorption isotherms for compounds 1-4 measured at 77K; (b) Powder x-ray diffraction data for pristine and NOx exposed compound 1 after 24 hrs.
All figures and tables
(9 total)
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
SO x /NO x Removal from Flue Gas Streams by Solid Adsorbents: A Review of Current Challenges and Future Directions
journal, August 2015
- Rezaei, Fateme; Rownaghi, Ali A.; Monjezi, Saman
- Energy & Fuels, Vol. 29, Issue 9
Nitrogen and sulphur chemistry in pressurised flue gas systems: A comparison of modelling and experiments
journal, January 2013
- Normann, Fredrik; Jansson, Erik; Petersson, Tobias
- International Journal of Greenhouse Gas Control, Vol. 12
Stability of Supported Amine Adsorbents to SO 2 and NO x in Postcombustion CO 2 Capture. 1. Single-Component Adsorption
journal, August 2013
- Rezaei, Fateme; Jones, Christopher W.
- Industrial & Engineering Chemistry Research, Vol. 52, Issue 34
Research Challenges in Avoiding “Showstoppers” in Developing Materials for Large-Scale Energy Applications
journal, October 2017
- Walton, Krista S.; Sholl, David S.
- Joule, Vol. 1, Issue 2
Selective Catalytic Reduction of NOx with N-Free Reductants
journal, January 1995
- Shelef, M.
- Chemical Reviews, Vol. 95, Issue 1
Simultaneous adsorption of SO2NOx from flue gases in a riser configuration
journal, December 2001
- Das, Asit K.; De Wilde, Juray; Heynderickx, Geraldine J.
- AIChE Journal, Vol. 47, Issue 12
SO2 and NO adsorption properties of activated carbons obtained from a pitch containing iron derivatives
journal, November 2001
- Davini, Paolo
- Carbon, Vol. 39, Issue 14
Adsorption equilibrium for sulfur dioxide, nitric oxide, carbon dioxide, nitrogen on 13X and 5A zeolites
journal, April 2012
- Deng, Hua; Yi, Honghong; Tang, Xiaolong
- Chemical Engineering Journal, Vol. 188
Computational screening of porous metal-organic frameworks and zeolites for the removal of SO 2 and NO x from flue gases
journal, April 2014
- Sun, Weizhen; Lin, Li-Chiang; Peng, Xuan
- AIChE Journal, Vol. 60, Issue 6
Selective O 2 Sorption at Ambient Temperatures via Node Distortions in Sc-MIL-100
journal, May 2016
- Sava Gallis, Dorina F.; Chapman, Karena W.; Rodriguez, Mark A.
- Chemistry of Materials, Vol. 28, Issue 10
Ab initio molecular dynamics determination of competitive O 2 vs. N 2 adsorption at open metal sites of M 2 (dobdc)
journal, January 2016
- Parkes, Marie V.; Greathouse, Jeffery A.; Hart, David B.
- Physical Chemistry Chemical Physics, Vol. 18, Issue 16
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
journal, March 2015
- Parkes, Marie V.; Sava Gallis, Dorina F.; Greathouse, Jeffery A.
- The Journal of Physical Chemistry C, Vol. 119, Issue 12
Enhanced O 2 Selectivity versus N 2 by Partial Metal Substitution in Cu-BTC
journal, March 2015
- Sava Gallis, Dorina F.; Parkes, Marie V.; Greathouse, Jeffery A.
- Chemistry of Materials, Vol. 27, Issue 6
Gas storage in porous metal–organic frameworks for clean energy applications
journal, January 2010
- Ma, Shengqian; Zhou, Hong-Cai
- Chem. Commun., Vol. 46, Issue 1
Selective gas adsorption and separation in metal–organic frameworks
journal, January 2009
- Li, Jian-Rong; Kuppler, Ryan J.; Zhou, Hong-Cai
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1477-1504
Metal–Organic Frameworks for Separations
journal, September 2011
- Li, Jian-Rong; Sculley, Julian; Zhou, Hong-Cai
- Chemical Reviews, Vol. 112, Issue 2, p. 869-932
Methane storage in metal–organic frameworks
journal, January 2014
- He, Yabing; Zhou, Wei; Qian, Guodong
- Chem. Soc. Rev., Vol. 43, Issue 16
Rational Design, Synthesis, Purification, and Activation of Metal−Organic Framework Materials
journal, August 2010
- Farha, Omar K.; Hupp, Joseph T.
- Accounts of Chemical Research, Vol. 43, Issue 8, p. 1166-1175
Why hybrid porous solids capture greenhouse gases?
journal, January 2011
- Férey, Gérard; Serre, Christian; Devic, Thomas
- Chem. Soc. Rev., Vol. 40, Issue 2
Progress in adsorption-based CO 2 capture by metal–organic frameworks
journal, January 2012
- Liu, Jian; Thallapally, Praveen K.; McGrail, B. Peter
- Chem. Soc. Rev., Vol. 41, Issue 6
High-Throughput Screening of Metal–Organic Frameworks for CO 2 Separation
journal, March 2012
- Han, Sangil; Huang, Yougui; Watanabe, Taku
- ACS Combinatorial Science, Vol. 14, Issue 4
Interactions of NO 2 with Zr-Based MOF: Effects of the Size of Organic Linkers on NO 2 Adsorption at Ambient Conditions
journal, December 2012
- Ebrahim, Amani M.; Levasseur, Benoit; Bandosz, Teresa J.
- Langmuir, Vol. 29, Issue 1
Effect of amine modification on the properties of zirconium–carboxylic acid based materials and their applications as NO2 adsorbents at ambient conditions
journal, April 2014
- Ebrahim, Amani M.; Bandosz, Teresa J.
- Microporous and Mesoporous Materials, Vol. 188
A UiO-66 analogue with uncoordinated carboxylic acids for the broad-spectrum removal of toxic chemicals
journal, January 2015
- DeCoste, Jared B.; Demasky, Tyler J.; Katz, Michael J.
- New Journal of Chemistry, Vol. 39, Issue 4
Extraordinary NO 2 Removal by the Metal-Organic Framework UiO-66-NH 2
journal, April 2016
- Peterson, Gregory W.; Mahle, John J.; DeCoste, Jared B.
- Angewandte Chemie International Edition, Vol. 55, Issue 21
Interaction of Acid Gases SO 2 and NO 2 with Coordinatively Unsaturated Metal Organic Frameworks: M-MOF-74 (M = Zn, Mg, Ni, Co)
journal, May 2017
- Tan, Kui; Zuluaga, Sebastian; Wang, Hao
- Chemistry of Materials, Vol. 29, Issue 10
Exceptional chemical and thermal stability of zeolitic imidazolate frameworks
journal, June 2006
- Park, K. S.; Ni, Z.; Cote, A. P.
- Proceedings of the National Academy of Sciences, Vol. 103, Issue 27, p. 10186-10191
Acid Gas Stability of Zeolitic Imidazolate Frameworks: Generalized Kinetic and Thermodynamic Characteristics
journal, May 2018
- Bhattacharyya, Souryadeep; Han, Rebecca; Kim, Wun-Gwi
- Chemistry of Materials, Vol. 30, Issue 12
Stability of Zeolitic Imidazolate Frameworks in NO 2
journal, January 2019
- Bhattacharyya, Souryadeep; Han, Rebecca; Joshi, Jayraj N.
- The Journal of Physical Chemistry C, Vol. 123, Issue 4
Isoreticular rare earth fcu -MOFs for the selective removal of H 2 S from CO 2 containing gases
journal, September 2017
- Bhatt, Prashant M.; Belmabkhout, Youssef; Assen, Ayalew H.
- Chemical Engineering Journal, Vol. 324
Responsive Lanthanide Coordination Polymer for Hydrogen Sulfide
journal, November 2013
- Liu, Baoxia; Chen, Yang
- Analytical Chemistry, Vol. 85, Issue 22
A highly selective on–off–on responsive lanthanide( iii ) based probe for recognition of copper and hydrogen sulfide
journal, January 2016
- Yip, Yuk-Wang; Law, Ga-Lai; Wong, Wing-Tak
- Dalton Transactions, Vol. 45, Issue 3
Multifunctional, Tunable Metal–Organic Framework Materials Platform for Bioimaging Applications
journal, June 2017
- Sava Gallis, Dorina F.; Rohwer, Lauren E. S.; Rodriguez, Mark A.
- ACS Applied Materials & Interfaces, Vol. 9, Issue 27
A New Zirconium Inorganic Building Brick Forming Metal Organic Frameworks with Exceptional Stability
journal, October 2008
- Cavka, Jasmina Hafizovic; Jakobsen, Søren; Olsbye, Unni
- Journal of the American Chemical Society, Vol. 130, Issue 42, p. 13850-13851
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 49, Issue 20, p. 14251-14269
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008
- Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I.
- Physical Review Letters, Vol. 100, Issue 13
Defect and Linker Effects on the Binding of Organophosphorous Compounds in UiO-66 and Rare-Earth MOFs
journal, November 2018
- Harvey, Jacob A.; Greathouse, Jeffery A.; Sava Gallis, Dorina F.
- The Journal of Physical Chemistry C, Vol. 122, Issue 47
Assessing Hubbard-corrected AM05+U and PBEsol+U density functionals for strongly correlated oxides CeO 2 and Ce 2 O 3
journal, January 2016
- Weck, Philippe F.; Kim, Eunja
- Physical Chemistry Chemical Physics, Vol. 18, Issue 38
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010
- Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
- The Journal of Chemical Physics, Vol. 132, Issue 15
Effect of the damping function in dispersion corrected density functional theory
journal, March 2011
- Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars
- Journal of Computational Chemistry, Vol. 32, Issue 7
H 2 O Adsorption/Desorption in MOF-74: Ab Initio Molecular Dynamics and Experiments
journal, May 2015
- Li, Yunsong; Wang, Xinjiang; Xu, Dongyan
- The Journal of Physical Chemistry C, Vol. 119, Issue 23
Role of Lead Vacancies for Optoelectronic Properties of Lead-Halide Perovskites
journal, December 2017
- Vogel, Dayton J.; Inerbaev, Talgat M.; Kilin, Dmitri S.
- The Journal of Physical Chemistry C, Vol. 122, Issue 10
First-Principles Treatment of Photoluminescence in Semiconductors
journal, December 2015
- Vogel, Dayton J.; Kilin, Dmitri S.
- The Journal of Physical Chemistry C, Vol. 119, Issue 50
Photoinduced Single- and Multiple-Electron Dynamics Processes Enhanced by Quantum Confinement in Lead Halide Perovskite Quantum Dots
journal, June 2017
- Vogel, Dayton J.; Kryjevski, Andrei; Inerbaev, Talgat
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 13
Reaction of NO 2 with Zn and ZnO: Photoemission, XANES, and Density Functional Studies on the Formation of NO 3
journal, January 2000
- Rodriguez, José A.; Jirsak, Tomas; Dvorak, Joseph
- The Journal of Physical Chemistry B, Vol. 104, Issue 2
Chemistry of NO2 on CeO2 and MgO: Experimental and theoretical studies on the formation of NO3
journal, June 2000
- Rodriguez, José A.; Jirsak, Tomas; Sambasivan, Sharadha
- The Journal of Chemical Physics, Vol. 112, Issue 22
Thermal Decomposition of Nitrogen Dioxide
journal, February 1956
- Rosser, Willis A.; Wise, Henry
- The Journal of Chemical Physics, Vol. 24, Issue 2
A precise solution of the rotation bending Schrödinger equation for a triatomic molecule with application to the water molecule
journal, January 1979
- Hoy, A. R.; Bunker, P. R.
- Journal of Molecular Spectroscopy, Vol. 74, Issue 1
A proposal for the structuring of water
journal, January 2000
- Chaplin, M. F.
- Biophysical Chemistry, Vol. 83, Issue 3
The structure of the ice Ih by neutron diffraction
journal, October 1983
- Kuhs, W. F.; Lehmann, M. S.
- The Journal of Physical Chemistry, Vol. 87, Issue 21
Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.