Insights into the Stability of Zeolitic Imidazolate Frameworks in Humid Acidic Environments from First-Principles Calculations
Abstract
Understanding the degradation mechanisms of zeolitic imidazolate frameworks (ZIFs) is crucial to improve their chemical stability and realize their potential industrial applications. In this work, we conduct a comprehensive study utilizing dispersion-corrected density functional theory calculations to investigate the chemical stability of bulk ZIFs and their external surfaces under conditions of acid-gas exposure. We examine the influence of steric factors such as topology and ligand functionalization on the relative chemical stability of prototypical ZIFs (ZIF-2 and ZIF-8), including their hypothetical polymorphs. We find that defect formation is more thermodynamically and kinetically favorable at ZIF external surfaces versus the bulk, and that both topology and ligand functionalization impact defect formation. In addition, we provide a detailed mechanism for the reaction of ZIFs with sulfurous and sulfuric acids, of which the latter serves as a catalyst in potential degradation reactions of ZIFs. We also provide information about the adsorption strength of a range of acid gases to defective ZIF structures, which can inform potential strategies to regenerate ZIFs and/or achieve defect engineering in these materials.
- Authors:
-
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering; Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry & Biochemistry
- Univ. of Wisconsin, Madison, WI (United States). Theoretical Chemistry Inst., and Dept. of Chemistry; Central South Univ., Changsha, Hunan (China). School of Minerals Processing and Bioengineering
- Univ. of Wisconsin, Madison, WI (United States). Theoretical Chemistry Inst., and Dept. of Chemistry
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1470287
- Grant/Contract Number:
- SC0012577
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 8; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (heterogeneous); defects; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)
Citation Formats
Han, Chu, Zhang, Chenyang, Tymińska, Nina, Schmidt, J. R., and Sholl, David S. Insights into the Stability of Zeolitic Imidazolate Frameworks in Humid Acidic Environments from First-Principles Calculations. United States: N. p., 2018.
Web. doi:10.1021/acs.jpcc.7b12058.
Han, Chu, Zhang, Chenyang, Tymińska, Nina, Schmidt, J. R., & Sholl, David S. Insights into the Stability of Zeolitic Imidazolate Frameworks in Humid Acidic Environments from First-Principles Calculations. United States. https://doi.org/10.1021/acs.jpcc.7b12058
Han, Chu, Zhang, Chenyang, Tymińska, Nina, Schmidt, J. R., and Sholl, David S. Mon .
"Insights into the Stability of Zeolitic Imidazolate Frameworks in Humid Acidic Environments from First-Principles Calculations". United States. https://doi.org/10.1021/acs.jpcc.7b12058. https://www.osti.gov/servlets/purl/1470287.
@article{osti_1470287,
title = {Insights into the Stability of Zeolitic Imidazolate Frameworks in Humid Acidic Environments from First-Principles Calculations},
author = {Han, Chu and Zhang, Chenyang and Tymińska, Nina and Schmidt, J. R. and Sholl, David S.},
abstractNote = {Understanding the degradation mechanisms of zeolitic imidazolate frameworks (ZIFs) is crucial to improve their chemical stability and realize their potential industrial applications. In this work, we conduct a comprehensive study utilizing dispersion-corrected density functional theory calculations to investigate the chemical stability of bulk ZIFs and their external surfaces under conditions of acid-gas exposure. We examine the influence of steric factors such as topology and ligand functionalization on the relative chemical stability of prototypical ZIFs (ZIF-2 and ZIF-8), including their hypothetical polymorphs. We find that defect formation is more thermodynamically and kinetically favorable at ZIF external surfaces versus the bulk, and that both topology and ligand functionalization impact defect formation. In addition, we provide a detailed mechanism for the reaction of ZIFs with sulfurous and sulfuric acids, of which the latter serves as a catalyst in potential degradation reactions of ZIFs. We also provide information about the adsorption strength of a range of acid gases to defective ZIF structures, which can inform potential strategies to regenerate ZIFs and/or achieve defect engineering in these materials.},
doi = {10.1021/acs.jpcc.7b12058},
journal = {Journal of Physical Chemistry. C},
number = 8,
volume = 122,
place = {United States},
year = {Mon Feb 05 00:00:00 EST 2018},
month = {Mon Feb 05 00:00:00 EST 2018}
}
Web of Science
Works referenced in this record:
Defects in Metal–Organic Frameworks: Challenge or Opportunity?
journal, August 2015
- Sholl, David S.; Lively, Ryan P.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 17
Engineering Copper Carboxylate Functionalities on Water Stable Metal–Organic Frameworks for Enhancement of Ammonia Removal Capacities
journal, February 2017
- Joshi, Jayraj N.; Garcia-Gutierrez, Erika Y.; Moran, Colton M.
- The Journal of Physical Chemistry C, Vol. 121, Issue 6
Defect-Engineered Metal-Organic Frameworks
journal, June 2015
- Fang, Zhenlan; Bueken, Bart; De Vos, Dirk E.
- Angewandte Chemie International Edition, Vol. 54, Issue 25
The surface chemistry of metal–organic frameworks
journal, January 2015
- McGuire, Christina V.; Forgan, Ross S.
- Chemical Communications, Vol. 51, Issue 25
MOF positioning technology and device fabrication
journal, January 2014
- Falcaro, Paolo; Ricco, Raffaele; Doherty, Cara M.
- Chem. Soc. Rev., Vol. 43, Issue 16
The Chemistry and Applications of Metal-Organic Frameworks
journal, August 2013
- Furukawa, H.; Cordova, K. E.; O'Keeffe, M.
- Science, Vol. 341, Issue 6149, p. 1230444-1230444
Gas Separation Properties of Metal Organic Framework (MOF-5) Membranes
journal, April 2012
- Zhao, Zhenxia; Ma, Xiaoli; Kasik, Alexandra
- Industrial & Engineering Chemistry Research, Vol. 52, Issue 3
Adsorption and Diffusion of CO 2 and CH 4 in Zeolitic Imidazolate Framework-8: Effect of Structural Flexibility
journal, April 2014
- Zhang, Liling; Wu, Gang; Jiang, Jianwen
- The Journal of Physical Chemistry C, Vol. 118, Issue 17
The first example of commensurate adsorption of atomic gas in a MOF and effective separation of xenon from other noble gases
journal, January 2014
- Wang, Hao; Yao, Kexin; Zhang, Zhijuan
- Chemical Science, Vol. 5, Issue 2, p. 620-624
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
MOF Crystal Chemistry Paving the Way to Gas Storage Needs: Aluminum-Based soc -MOF for CH 4 , O 2 , and CO 2 Storage
journal, October 2015
- Alezi, Dalal; Belmabkhout, Youssef; Suyetin, Mikhail
- Journal of the American Chemical Society, Vol. 137, Issue 41
A 3-D diamondoid MOF catalyst based on in situ generated [Cu(L) 2 ] N-heterocyclic carbene (NHC) linkers: hydroboration of CO 2
journal, January 2014
- Burgun, Alexandre; Crees, Rachel S.; Cole, Marcus L.
- Chem. Commun., Vol. 50, Issue 79
Amorphous metal–organic frameworks for drug delivery
journal, January 2015
- Orellana-Tavra, Claudia; Baxter, Emma F.; Tian, Tian
- Chemical Communications, Vol. 51, Issue 73
Metal–Organic Frameworks as Efficient Materials for Drug Delivery
journal, September 2006
- Horcajada, Patricia; Serre, Christian; Vallet-Regí, María
- Angewandte Chemie International Edition, Vol. 45, Issue 36, p. 5974-5978
Chemical, thermal and mechanical stabilities of metal–organic frameworks
journal, February 2016
- Howarth, Ashlee J.; Liu, Yangyang; Li, Peng
- Nature Reviews Materials, Vol. 1, Issue 3
Water Stability and Adsorption in Metal–Organic Frameworks
journal, September 2014
- Burtch, Nicholas C.; Jasuja, Himanshu; Walton, Krista S.
- Chemical Reviews, Vol. 114, Issue 20, p. 10575-10612
Tuning the Kinetic Water Stability and Adsorption Interactions of Mg-MOF-74 by Partial Substitution with Co or Ni
journal, December 2015
- Jiao, Yang; Morelock, Cody R.; Burtch, Nicholas C.
- Industrial & Engineering Chemistry Research, Vol. 54, Issue 49
Characterization and properties of Zn/Co zeolitic imidazolate frameworks vs. ZIF-8 and ZIF-67
journal, January 2017
- Zhou, Kui; Mousavi, Bibimaryam; Luo, Zhixiong
- Journal of Materials Chemistry A, Vol. 5, Issue 3
The effect of water adsorption on the structure of the carboxylate containing metal–organic frameworks Cu-BTC, Mg-MOF-74, and UiO-66
journal, January 2013
- DeCoste, Jared B.; Peterson, Gregory W.; Schindler, Bryan J.
- Journal of Materials Chemistry A, Vol. 1, Issue 38
Tuning the moisture stability of metal–organic frameworks by incorporating hydrophobic functional groups at different positions of ligands
journal, January 2011
- Ma, Deyun; Li, Yingwei; Li, Zhong
- Chemical Communications, Vol. 47, Issue 26
Mixed-Linker Hybrid Superpolyhedra for the Production of a Series of Large-Pore Iron(III) Carboxylate Metal-Organic Frameworks
journal, April 2013
- Chevreau, Hubert; Devic, Thomas; Salles, Fabrice
- Angewandte Chemie International Edition, Vol. 52, Issue 19
Moisture-Resistant and Superhydrophobic Metal−Organic Frameworks Obtained via Postsynthetic Modification
journal, April 2010
- Nguyen, Joseph G.; Cohen, Seth M.
- Journal of the American Chemical Society, Vol. 132, Issue 13
Synergistic Effects of Water and SO 2 on Degradation of MIL-125 in the Presence of Acid Gases
journal, November 2016
- Mounfield, William P.; Han, Chu; Pang, Simon H.
- The Journal of Physical Chemistry C, Vol. 120, Issue 48
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
Interactions of SO 2 -Containing Acid Gases with ZIF-8: Structural Changes and Mechanistic Investigations
journal, November 2016
- Bhattacharyya, Souryadeep; Pang, Simon H.; Dutzer, Michael R.
- The Journal of Physical Chemistry C, Vol. 120, Issue 48
Facet-Specific Stability of ZIF-8 in the Presence of Acid Gases Dissolved in Aqueous Solutions
journal, September 2016
- Pang, Simon H.; Han, Chu; Sholl, David S.
- Chemistry of Materials, Vol. 28, Issue 19
Chemical structure, network topology, and porosity effects on the mechanical properties of Zeolitic Imidazolate Frameworks
journal, May 2010
- Tan, J. C.; Bennett, T. D.; Cheetham, A. K.
- Proceedings of the National Academy of Sciences, Vol. 107, Issue 22
Investigating the Intrinsic Ethanol/Water Separation Capability of ZIF-8: An Adsorption and Diffusion Study
journal, March 2013
- Zhang, Ke; Lively, Ryan P.; Zhang, Chen
- The Journal of Physical Chemistry C, Vol. 117, Issue 14
Diffusive separation of propylene/propane with ZIF-8 membranes
journal, January 2014
- Hara, Nobuo; Yoshimune, Miki; Negishi, Hideyuki
- Journal of Membrane Science, Vol. 450
In Situ Synthesis of Thin Zeolitic–Imidazolate Framework ZIF-8 Membranes Exhibiting Exceptionally High Propylene/Propane Separation
journal, July 2013
- Kwon, Hyuk Taek; Jeong, Hae-Kwon
- Journal of the American Chemical Society, Vol. 135, Issue 29
A high-performance supercapacitor cell based on ZIF-8-derived nanoporous carbon using an organic electrolyte
journal, January 2016
- Salunkhe, Rahul R.; Young, Christine; Tang, Jing
- Chemical Communications, Vol. 52, Issue 26
ZIF-derived porous carbon: a promising supercapacitor electrode material
journal, January 2014
- Zhang, Peng; Sun, Fang; Shen, Zhigang
- Journal of Materials Chemistry A, Vol. 2, Issue 32
Metal−Organic Frameworks as Sensors: A ZIF-8 Based Fabry−Pérot Device as a Selective Sensor for Chemical Vapors and Gases
journal, June 2010
- Lu, Guang; Hupp, Joseph T.
- Journal of the American Chemical Society, Vol. 132, Issue 23
Recovery of Acid-Gas-Degraded Zeolitic Imidazolate Frameworks by Solvent-Assisted Crystal Redemption (SACRed)
journal, September 2017
- Jayachandrababu, Krishna C.; Bhattacharyya, Souryadeep; Chiang, Yadong
- ACS Applied Materials & Interfaces, Vol. 9, Issue 40
Computational Characterization of Defects in Metal–Organic Frameworks: Spontaneous and Water-Induced Point Defects in ZIF-8
journal, January 2016
- Zhang, Chenyang; Han, Chu; Sholl, David S.
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 3
Computational Model and Characterization of Stacking Faults in ZIF-8 Polymorphs
journal, November 2016
- Han, Rebecca; Sholl, David S.
- The Journal of Physical Chemistry C, Vol. 120, Issue 48
Liquid metal–organic frameworks
journal, October 2017
- Gaillac, Romain; Pullumbi, Pluton; Beyer, Kevin A.
- Nature Materials, Vol. 16, Issue 11
External Surface of Zeolite Imidazolate Frameworks Viewed Ab Initio: Multifunctionality at the Organic−Inorganic Interface
journal, November 2009
- Chizallet, Céline; Bats, Nicolas
- The Journal of Physical Chemistry Letters, Vol. 1, Issue 1
Characterization of the Thermodynamic Stability of Solvated Metal–Organic Framework Polymorphs Using Molecular Simulations
journal, September 2013
- Gee, Jason A.; Sholl, David S.
- The Journal of Physical Chemistry C, Vol. 117, Issue 40
Thermal and mechanical stability of zeolitic imidazolate frameworks polymorphs
journal, December 2014
- Bouëssel du Bourg, Lila; Ortiz, Aurélie U.; Boutin, Anne
- APL Materials, Vol. 2, Issue 12
Zeolitic imidazole frameworks: structural and energetics trends compared with their zeolite analogues
journal, January 2009
- Lewis, Dewi W.; Ruiz-Salvador, A. Rabdel; Gómez, Ariel
- CrystEngComm, Vol. 11, Issue 11
Experimental and Theoretical Evaluation of the Stability of True MOF Polymorphs Explains Their Mechanochemical Interconversions
journal, June 2017
- Akimbekov, Zamirbek; Katsenis, Athanassios D.; Nagabhushana, G. P.
- Journal of the American Chemical Society, Vol. 139, Issue 23
Ionic Liquid/Metal–Organic Framework Composites for H 2 S Removal from Natural Gas: A Computational Exploration
journal, February 2015
- Li, Zhengjie; Xiao, Yuanlong; Xue, Wenjuan
- The Journal of Physical Chemistry C, Vol. 119, Issue 7
Acid Gas Adsorption on Metal–Organic Framework Nanosheets as a Model of an “All-Surface” Material
journal, February 2017
- Howe, Joshua D.; Liu, Yang; Flores, Luis
- Journal of Chemical Theory and Computation, Vol. 13, Issue 3
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
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
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
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
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
Reversible work transition state theory: application to dissociative adsorption of hydrogen
journal, February 1995
- Mills, Gregory; Jónsson, Hannes; Schenter, Gregory K.
- Surface Science, Vol. 324, Issue 2-3
A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
- Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
journal, December 2000
- Henkelman, Graeme; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22
The energy landscapes of zeolitic imidazolate frameworks (ZIFs): towards quantifying the presence of substituents on the imidazole ring
journal, January 2012
- Baburin, Igor A.; Leoni, Stefano
- J. Mater. Chem., Vol. 22, Issue 20
Polymorphism/pseudopolymorphism of metal–organic frameworks composed of zinc( ii ) and 2-methylimidazole: synthesis, stability, and application in gas storage
journal, January 2016
- Lo, Yang; Lam, Chon Hei; Chang, Chao-Wen
- RSC Advances, Vol. 6, Issue 92
Stability of ZIF-8 membranes and crystalline powders in water at room temperature
journal, July 2015
- Zhang, Huifeng; Liu, Defei; Yao, Ying
- Journal of Membrane Science, Vol. 485
Crystal-Size-Dependent Structural Transitions in Nanoporous Crystals: Adsorption-Induced Transitions in ZIF-8
journal, August 2014
- Zhang, Chen; Gee, Jason A.; Sholl, David S.
- The Journal of Physical Chemistry C, Vol. 118, Issue 35
Dichotomous adsorption behaviour of dyes on an amino-functionalised metal–organic framework, amino-MIL-101(Al)
journal, January 2014
- Haque, Enamul; Lo, Victor; Minett, Andrew I.
- J. Mater. Chem. A, Vol. 2, Issue 1
Zeolitic imidazolate metal organic framework ZIF-8 with ultra-high adsorption capacity bound tetracycline in aqueous solution
journal, January 2015
- Wu, Chun-sheng; Xiong, Zhen-hu; Li, Chen
- RSC Advances, Vol. 5, Issue 100
Development and Evaluation of Porous Materials for Carbon Dioxide Separation and Capture
journal, October 2011
- Bae, Youn-Sang; Snurr, Randall Q.
- Angewandte Chemie International Edition, Vol. 50, Issue 49
Metal–organic framework materials as catalysts
journal, January 2009
- Lee, JeongYong; Farha, Omar K.; Roberts, John
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1450-1459
A Chemical Route to Activation of Open Metal Sites in the Copper-Based Metal–Organic Framework Materials HKUST-1 and Cu-MOF-2
journal, July 2015
- Kim, Hong Ki; Yun, Won Seok; Kim, Min-Bum
- Journal of the American Chemical Society, Vol. 137, Issue 31
Works referencing / citing this record:
Metal–Organic Frameworks Based Nano/Micro/Millimeter‐Sized Self‐Propelled Autonomous Machines
journal, January 2019
- Khezri, Bahareh; Pumera, Martin
- Advanced Materials, Vol. 31, Issue 14
Structure and electronic properties of rare earth DOBDC metal–organic-frameworks
journal, January 2019
- Vogel, Dayton J.; Sava Gallis, Dorina F.; Nenoff, Tina M.
- Physical Chemistry Chemical Physics, Vol. 21, Issue 41
Light-controllable systems based on TiO 2 -ZIF-8 composites for targeted drug release: communicating with tumour cells
journal, January 2019
- Sharsheeva, Aziza; Iglin, Vadim A.; Nesterov, Pavel V.
- Journal of Materials Chemistry B, Vol. 7, Issue 43
High Surface Proton Conduction in Nanostructured ZIF-8
journal, September 2019
- Muñoz-Gil,
- Nanomaterials, Vol. 9, Issue 10