Efficient extraction of inorganic selenium from water by a Zr metal–organic framework: investigation of volumetric uptake capacity and binding motifs
Abstract
Strict monitoring and control of selenium concentrations in freshwater supplies is critical to safeguarding human health and aquatic life. A handful of previously investigated sorbents exhibit noteworthy gravimetric (mg g -1) Se uptake capacities; however, often display insufficient volumetric (mg cm -3) capacities, thereby requiring large volumes of material for commercial implementation. In this paper, in pursuit of mitigating this material inefficiency, we investigated the selenite (SeO 3 2-) and selenate (SeO 4 2-) affinity of MOF-808, a Zr-based metal–organic framework with a high density of potential Se oxyanion binding sites. MOF-808 recorded exceptional volumetric and gravimetric Se oxyanion capacities of 133 mg g -1 (127 mg cm -3) and 118 mg g -1 (112 mg cm -3) for aqueous selenite and selenate, respectively. Single-crystal X-ray diffraction studies revealed that selenite and selenate can bind at the MOF node via two distinct binding motifs, an η 2μ 2 motif in which the oxyanion coordinates to two different metal atoms in a single node, and a μ 2 motif in which the oxyanion interacts with only a single metal atom. Finally and furthermore, powder X-ray diffraction (PXRD) patterns and N 2 adsorption/desorption isotherms confirm the retention of bulk crystallinity and porositymore »
- Authors:
-
[1];
[2];
[1];
[3]
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
- Concordia Univ., Montreal, QC (Canada). Dept. of Chemistry and Biochemistry
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. Dept. of Chemical and Biological Engineering; King Abdulaziz Univ., Jeddah (Saudi Arabia). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
- OSTI Identifier:
- 1468444
- Alternate Identifier(s):
- OSTI ID: 1463190
- Grant/Contract Number:
- NA0003763; ECCS-1542205
- Resource Type:
- Accepted Manuscript
- Journal Name:
- CrystEngComm
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 40; Journal ID: ISSN 1466-8033
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Drout, Riki J., Howarth, Ashlee J., Otake, Ken-ichi, Islamoglu, Timur, and Farha, Omar K. Efficient extraction of inorganic selenium from water by a Zr metal–organic framework: investigation of volumetric uptake capacity and binding motifs. United States: N. p., 2018.
Web. doi:10.1039/c8ce00992a.
Drout, Riki J., Howarth, Ashlee J., Otake, Ken-ichi, Islamoglu, Timur, & Farha, Omar K. Efficient extraction of inorganic selenium from water by a Zr metal–organic framework: investigation of volumetric uptake capacity and binding motifs. United States. doi:10.1039/c8ce00992a.
Drout, Riki J., Howarth, Ashlee J., Otake, Ken-ichi, Islamoglu, Timur, and Farha, Omar K. Tue .
"Efficient extraction of inorganic selenium from water by a Zr metal–organic framework: investigation of volumetric uptake capacity and binding motifs". United States. doi:10.1039/c8ce00992a. https://www.osti.gov/servlets/purl/1468444.
@article{osti_1468444,
title = {Efficient extraction of inorganic selenium from water by a Zr metal–organic framework: investigation of volumetric uptake capacity and binding motifs},
author = {Drout, Riki J. and Howarth, Ashlee J. and Otake, Ken-ichi and Islamoglu, Timur and Farha, Omar K.},
abstractNote = {Strict monitoring and control of selenium concentrations in freshwater supplies is critical to safeguarding human health and aquatic life. A handful of previously investigated sorbents exhibit noteworthy gravimetric (mg g-1) Se uptake capacities; however, often display insufficient volumetric (mg cm-3) capacities, thereby requiring large volumes of material for commercial implementation. In this paper, in pursuit of mitigating this material inefficiency, we investigated the selenite (SeO32-) and selenate (SeO42-) affinity of MOF-808, a Zr-based metal–organic framework with a high density of potential Se oxyanion binding sites. MOF-808 recorded exceptional volumetric and gravimetric Se oxyanion capacities of 133 mg g-1 (127 mg cm-3) and 118 mg g-1 (112 mg cm-3) for aqueous selenite and selenate, respectively. Single-crystal X-ray diffraction studies revealed that selenite and selenate can bind at the MOF node via two distinct binding motifs, an η2μ2 motif in which the oxyanion coordinates to two different metal atoms in a single node, and a μ2 motif in which the oxyanion interacts with only a single metal atom. Finally and furthermore, powder X-ray diffraction (PXRD) patterns and N2 adsorption/desorption isotherms confirm the retention of bulk crystallinity and porosity after the uptake of Se oxyanions.},
doi = {10.1039/c8ce00992a},
journal = {CrystEngComm},
number = 40,
volume = 20,
place = {United States},
year = {2018},
month = {8}
}
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 4 works
Citation information provided by
Web of Science
Web of Science
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:
Adsorptive removal of Sb(V) from water using a mesoporous Zr-based metal–organic framework
journal, September 2018
- Rangwani, Sean; Howarth, Ashlee J.; DeStefano, Matthew R.
- Polyhedron, Vol. 151
Postsynthetic Tuning of Metal–Organic Frameworks for Targeted Applications
journal, February 2017
- Islamoglu, Timur; Goswami, Subhadip; Li, Zhanyong
- Accounts of Chemical Research, Vol. 50, Issue 4
Selenate Removal from Sulfate Containing Aqueous Solutions
journal, October 2005
- Jegadeesan, G.; Mondal, K.
- Environmental Technology, Vol. 26, Issue 10
Porous metal–organic-framework nanoscale carriers as a potential platform for drug delivery and imaging
journal, December 2009
- Horcajada, Patricia; Chalati, Tamim; Serre, Christian
- Nature Materials, Vol. 9, Issue 2
Identifying the Recognition Site for Selective Trapping of 99 TcO 4 – in a Hydrolytically Stable and Radiation Resistant Cationic Metal–Organic Framework
journal, October 2017
- Zhu, Lin; Sheng, Daopeng; Xu, Chao
- Journal of the American Chemical Society, Vol. 139, Issue 42
Adsorption mechanisms of selenium oxyanions at the aluminum oxide/water interface
journal, November 2006
- Peak, Derek
- Journal of Colloid and Interface Science, Vol. 303, Issue 2
Adsorption of selenite and selenate ions onto thiourea-formaldehyde resin
journal, May 2011
- Gezer, Nisa; Gülfen, Mustafa; Aydın, Ali Osman
- Journal of Applied Polymer Science, Vol. 122, Issue 2
Removal of selenate from water by chemical reduction
journal, January 1988
- Murphy, Andrew P.
- Industrial & Engineering Chemistry Research, Vol. 27, Issue 1
An Isoreticular Series of Metal-Organic Frameworks with Dendritic Hexacarboxylate Ligands and Exceptionally High Gas-Uptake Capacity
journal, June 2010
- Yuan, Daqiang; Zhao, Dan; Sun, Daofeng
- Angewandte Chemie International Edition, Vol. 49, Issue 31, p. 5357-5361
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
Superacidity in Sulfated Metal–Organic Framework-808
journal, September 2014
- Jiang, Juncong; Gándara, Felipe; Zhang, Yue-Biao
- Journal of the American Chemical Society, Vol. 136, Issue 37
Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage
journal, January 2002
- Eddaoudi, Mohamed; Kim, Jaheon; Rosi, Nathaniel
- Science, Vol. 295, Issue 5554, p. 469-472
Efficient and Selective Uptake of TcO 4 – by a Cationic Metal–Organic Framework Material with Open Ag + Sites
journal, March 2017
- Sheng, Daopeng; Zhu, Lin; Xu, Chao
- Environmental Science & Technology, Vol. 51, Issue 6
Carbon Dioxide Capture in Metal–Organic Frameworks
journal, September 2011
- Sumida, Kenji; Rogow, David L.; Mason, Jarad A.
- Chemical Reviews, Vol. 112, Issue 2, p. 724-781
Rapid Simultaneous Removal of Toxic Anions [HSeO 3 ] − , [SeO 3 ] 2– , and [SeO 4 ] 2– , and Metals Hg 2+ , Cu 2+ , and Cd 2+ by MoS 4 2– Intercalated Layered Double Hydroxide
journal, August 2017
- Ma, Lijiao; Islam, Saiful M.; Xiao, Chengliang
- Journal of the American Chemical Society, Vol. 139, Issue 36
Review of 15 years of research on ecotoxicology and remediation of land contaminated by agricultural drainage sediment rich in selenium
journal, March 2004
- Wu, Lin
- Ecotoxicology and Environmental Safety, Vol. 57, Issue 3
Towards the use of metal–organic frameworks for water reuse: a review of the recent advances in the field of organic pollutants removal and degradation and the next steps in the field
journal, January 2015
- Dias, Elton M.; Petit, Camille
- Journal of Materials Chemistry A, Vol. 3, Issue 45
High Efficiency Adsorption and Removal of Selenate and Selenite from Water Using Metal–Organic Frameworks
journal, June 2015
- Howarth, Ashlee J.; Katz, Michael J.; Wang, Timothy C.
- Journal of the American Chemical Society, Vol. 137, Issue 23
Water Purification: Adsorption over Metal-Organic Frameworks
journal, February 2016
- Li, Siqing; Chen, Yifa; Pei, Xiaokun
- Chinese Journal of Chemistry, Vol. 34, Issue 2
Evaluation of Brønsted acidity and proton topology in Zr- and Hf-based metal–organic frameworks using potentiometric acid–base titration
journal, January 2016
- Klet, Rachel C.; Liu, Yangyang; Wang, Timothy C.
- Journal of Materials Chemistry A, Vol. 4, Issue 4
Hydrogen storage in metal–organic frameworks
journal, January 2009
- Murray, Leslie J.; Dincă, Mircea; Long, Jeffrey R.
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1294-1314
Superior capability of MgAl2O4 for selenite removal from contaminated groundwater during its reconstruction of layered double hydroxides
journal, April 2017
- Tian, Na; Zhou, Zhaoxin; Tian, Xike
- Separation and Purification Technology, Vol. 176
Introduction to Metal–Organic Frameworks
journal, September 2011
- Zhou, Hong-Cai; Long, Jeffrey R.; Yaghi, Omar M.
- Chemical Reviews, Vol. 112, Issue 2, p. 673-674
A series of isoreticular chiral metal–organic frameworks as a tunable platform for asymmetric catalysis
journal, July 2010
- Ma, Liqing; Falkowski, Joseph M.; Abney, Carter
- Nature Chemistry, Vol. 2, Issue 10
Metal–Organic Framework Materials as Chemical Sensors
journal, September 2011
- Kreno, Lauren E.; Leong, Kirsty; Farha, Omar K.
- Chemical Reviews, Vol. 112, Issue 2, p. 1105-1125
Role of assisted natural remediation in environmental cleanup
journal, October 2004
- Adriano, D. C.; Wenzel, W. W.; Vangronsveld, J.
- Geoderma, Vol. 122, Issue 2-4
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
Selective Selenate Adsorption on Cationated Amino-Functionalized MCM-41
journal, November 2003
- Yokoi, Toshiyuki; Tatsumi, Takashi; Yoshitake, Hideaki
- Bulletin of the Chemical Society of Japan, Vol. 76, Issue 11
Efficient Capture of Perrhenate and Pertechnetate by a Mesoporous Zr Metal–Organic Framework and Examination of Anion Binding Motifs
journal, January 2018
- Drout, Riki J.; Otake, Kenichi; Howarth, Ashlee J.
- Chemistry of Materials, Vol. 30, Issue 4
Probing the correlations between the defects in metal–organic frameworks and their catalytic activity by an epoxide ring-opening reaction
journal, January 2016
- Liu, Yangyang; Klet, Rachel C.; Hupp, Joseph T.
- Chemical Communications, Vol. 52, Issue 50
Metal-organic frameworks (MOFs) in water filtration membranes for desalination and other applications
journal, June 2018
- Kadhom, Mohammed; Deng, Baolin
- Applied Materials Today, Vol. 11
Metal–organic frameworks for applications in remediation of oxyanion/cation-contaminated water
journal, January 2015
- Howarth, Ashlee J.; Liu, Yangyang; Hupp, Joseph T.
- CrystEngComm, Vol. 17, Issue 38
Design and synthesis of an exceptionally stable and highly porous metal-organic framework
journal, November 1999
- Li, Hailian; Eddaoudi, Mohamed; M., O'Keeffe
- Nature, Vol. 402, Issue 6759, p. 276-279
Metal–organic frameworks for the removal of toxic industrial chemicals and chemical warfare agents
journal, January 2017
- Bobbitt, N. Scott; Mendonca, Matthew L.; Howarth, Ashlee J.
- Chemical Society Reviews, Vol. 46, Issue 11
Aquatic selenium pollution is a global environmental safety issue
journal, September 2004
- Lemly, A. Dennis
- Ecotoxicology and Environmental Safety, Vol. 59, Issue 1
Adsorption of selenite and selenate by nanocrystalline aluminum oxide, neat and impregnated in chitosan beads
journal, March 2014
- Yamani, Jamila S.; Lounsbury, Amanda W.; Zimmerman, Julie B.
- Water Research, Vol. 50
Adsorption mechanism of selenate and selenite on the binary oxide systems
journal, September 2009
- Chan, Ya Ting; Kuan, Wen Hui; Chen, Tsan Yao
- Water Research, Vol. 43, Issue 17
Structure and hydrogen bonding of the hydrated selenite and selenate ions in aqueous solution
journal, January 2014
- Eklund, Lars; Persson, Ingmar
- Dalton Trans., Vol. 43, Issue 17
Selenium Sequestration in a Cationic Layered Rare Earth Hydroxide: A Combined Batch Experiments and EXAFS Investigation
journal, July 2017
- Zhu, Lin; Zhang, Linjuan; Li, Jie
- Environmental Science & Technology, Vol. 51, Issue 15
Science and technology for water purification in the coming decades
journal, March 2008
- Shannon, Mark A.; Bohn, Paul W.; Elimelech, Menachem
- Nature, Vol. 452, Issue 7185, p. 301-310
Experimental and theoretical study on selenate uptake to zirconium metal–organic frameworks: Effect of defects and ligands
journal, December 2017
- Li, Jie; Liu, Yang; Wang, Xiangxue
- Chemical Engineering Journal, Vol. 330
An Isoreticular Series of Metal-Organic Frameworks with Dendritic Hexacarboxylate Ligands and Exceptionally High Gas-Uptake Capacity
journal, June 2010
- Yuan, Daqiang; Zhao, Dan; Sun, Daofeng
- Angewandte Chemie, Vol. 122, Issue 31
Works referencing / citing this record:
CCDC 1843055: Experimental Crystal Structure Determination: New Structure undergoing enhancement
IFAGII : Space Group: F d 3 m (227), Cell: a 35.286(9)Å b 35.286(9)Å c 35.286(9)Å, α 90° β 90° γ 90°
dataset, June 2018
- Drout, Riki J.; Howarth, Ashlee J.; Otake, Ken-ichi
- The Cambridge Crystallographic Data Centre, 3D viewer; 1 diagram
CCDC 1843056: Experimental Crystal Structure Determination: IFAGEE : catena-[(μ-benzene-1,3,5-tricarboxylato)-tetrakis(μ-oxido)-tris(selenato)-tri-hafnium]
dataset, June 2018
- Drout, Riki; Howarth, Ashlee; Otake, Ken-ichi
- Cambridge Structural Database (CSD)
An Isoreticular Series of Metal-Organic Frameworks with Dendritic Hexacarboxylate Ligands and Exceptionally High Gas-Uptake Capacity
journal, June 2010
- Yuan, Daqiang; Zhao, Dan; Sun, Daofeng
- Angewandte Chemie International Edition, Vol. 49, Issue 31, p. 5357-5361
Adsorption of selenite and selenate ions onto thiourea-formaldehyde resin
journal, May 2011
- Gezer, Nisa; Gülfen, Mustafa; Aydın, Ali Osman
- Journal of Applied Polymer Science, Vol. 122, Issue 2
Water Purification: Adsorption over Metal-Organic Frameworks
journal, February 2016
- Li, Siqing; Chen, Yifa; Pei, Xiaokun
- Chinese Journal of Chemistry, Vol. 34, Issue 2
Metal-organic frameworks (MOFs) in water filtration membranes for desalination and other applications
journal, June 2018
- Kadhom, Mohammed; Deng, Baolin
- Applied Materials Today, Vol. 11
Experimental and theoretical study on selenate uptake to zirconium metal–organic frameworks: Effect of defects and ligands
journal, December 2017
- Li, Jie; Liu, Yang; Wang, Xiangxue
- Chemical Engineering Journal, Vol. 330
Role of assisted natural remediation in environmental cleanup
journal, October 2004
- Adriano, D. C.; Wenzel, W. W.; Vangronsveld, J.
- Geoderma, Vol. 122, Issue 2-4
Adsorption mechanisms of selenium oxyanions at the aluminum oxide/water interface
journal, November 2006
- Peak, Derek
- Journal of Colloid and Interface Science, Vol. 303, Issue 2
Adsorptive removal of Sb(V) from water using a mesoporous Zr-based metal–organic framework
journal, September 2018
- Rangwani, Sean; Howarth, Ashlee J.; DeStefano, Matthew R.
- Polyhedron, Vol. 151
Superior capability of MgAl2O4 for selenite removal from contaminated groundwater during its reconstruction of layered double hydroxides
journal, April 2017
- Tian, Na; Zhou, Zhaoxin; Tian, Xike
- Separation and Purification Technology, Vol. 176
Adsorption mechanism of selenate and selenite on the binary oxide systems
journal, September 2009
- Chan, Ya Ting; Kuan, Wen Hui; Chen, Tsan Yao
- Water Research, Vol. 43, Issue 17
Adsorption of selenite and selenate by nanocrystalline aluminum oxide, neat and impregnated in chitosan beads
journal, March 2014
- Yamani, Jamila S.; Lounsbury, Amanda W.; Zimmerman, Julie B.
- Water Research, Vol. 50
Postsynthetic Tuning of Metal–Organic Frameworks for Targeted Applications
journal, February 2017
- Islamoglu, Timur; Goswami, Subhadip; Li, Zhanyong
- Accounts of Chemical Research, Vol. 50, Issue 4
Efficient Capture of Perrhenate and Pertechnetate by a Mesoporous Zr Metal–Organic Framework and Examination of Anion Binding Motifs
journal, January 2018
- Drout, Riki J.; Otake, Kenichi; Howarth, Ashlee J.
- Chemistry of Materials, Vol. 30, Issue 4
Efficient and Selective Uptake of TcO 4 – by a Cationic Metal–Organic Framework Material with Open Ag + Sites
journal, March 2017
- Sheng, Daopeng; Zhu, Lin; Xu, Chao
- Environmental Science & Technology, Vol. 51, Issue 6
Selenium Sequestration in a Cationic Layered Rare Earth Hydroxide: A Combined Batch Experiments and EXAFS Investigation
journal, July 2017
- Zhu, Lin; Zhang, Linjuan; Li, Jie
- Environmental Science & Technology, Vol. 51, Issue 15
Metal–Organic Framework Materials as Chemical Sensors
journal, September 2011
- Kreno, Lauren E.; Leong, Kirsty; Farha, Omar K.
- Chemical Reviews, Vol. 112, Issue 2, p. 1105-1125
Carbon Dioxide Capture in Metal–Organic Frameworks
journal, September 2011
- Sumida, Kenji; Rogow, David L.; Mason, Jarad A.
- Chemical Reviews, Vol. 112, Issue 2, p. 724-781
Introduction to Metal–Organic Frameworks
journal, September 2011
- Zhou, Hong-Cai; Long, Jeffrey R.; Yaghi, Omar M.
- Chemical Reviews, Vol. 112, Issue 2, p. 673-674
Removal of selenate from water by chemical reduction
journal, January 1988
- Murphy, Andrew P.
- Industrial & Engineering Chemistry Research, Vol. 27, Issue 1
Superacidity in Sulfated Metal–Organic Framework-808
journal, September 2014
- Jiang, Juncong; Gándara, Felipe; Zhang, Yue-Biao
- Journal of the American Chemical Society, Vol. 136, Issue 37
High Efficiency Adsorption and Removal of Selenate and Selenite from Water Using Metal–Organic Frameworks
journal, June 2015
- Howarth, Ashlee J.; Katz, Michael J.; Wang, Timothy C.
- Journal of the American Chemical Society, Vol. 137, Issue 23
Rapid Simultaneous Removal of Toxic Anions [HSeO 3 ] − , [SeO 3 ] 2– , and [SeO 4 ] 2– , and Metals Hg 2+ , Cu 2+ , and Cd 2+ by MoS 4 2– Intercalated Layered Double Hydroxide
journal, August 2017
- Ma, Lijiao; Islam, Saiful M.; Xiao, Chengliang
- Journal of the American Chemical Society, Vol. 139, Issue 36
Identifying the Recognition Site for Selective Trapping of 99 TcO 4 – in a Hydrolytically Stable and Radiation Resistant Cationic Metal–Organic Framework
journal, October 2017
- Zhu, Lin; Sheng, Daopeng; Xu, Chao
- Journal of the American Chemical Society, Vol. 139, Issue 42
Design and synthesis of an exceptionally stable and highly porous metal-organic framework
journal, November 1999
- Li, Hailian; Eddaoudi, Mohamed; M., O'Keeffe
- Nature, Vol. 402, Issue 6759, p. 276-279
Science and technology for water purification in the coming decades
journal, March 2008
- Shannon, Mark A.; Bohn, Paul W.; Elimelech, Menachem
- Nature, Vol. 452, Issue 7185, p. 301-310
A series of isoreticular chiral metal–organic frameworks as a tunable platform for asymmetric catalysis
journal, July 2010
- Ma, Liqing; Falkowski, Joseph M.; Abney, Carter
- Nature Chemistry, Vol. 2, Issue 10
Porous metal–organic-framework nanoscale carriers as a potential platform for drug delivery and imaging
journal, December 2009
- Horcajada, Patricia; Chalati, Tamim; Serre, Christian
- Nature Materials, Vol. 9, Issue 2
Hydrogen storage in metal–organic frameworks
journal, January 2009
- Murray, Leslie J.; Dincă, Mircea; Long, Jeffrey R.
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1294-1314
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 framework materials as catalysts
journal, January 2009
- Lee, JeongYong; Farha, Omar K.; Roberts, John
- Chemical Society Reviews, Vol. 38, Issue 5, p. 1450-1459
Selenate Removal from Sulfate Containing Aqueous Solutions
journal, October 2005
- Jegadeesan, G.; Mondal, K.
- Environmental Technology, Vol. 26, Issue 10
Systematic Design of Pore Size and Functionality in Isoreticular MOFs and Their Application in Methane Storage
journal, January 2002
- Eddaoudi, Mohamed; Kim, Jaheon; Rosi, Nathaniel
- Science, Vol. 295, Issue 5554, p. 469-472
Selective Selenate Adsorption on Cationated Amino-Functionalized MCM-41
journal, November 2003
- Yokoi, Toshiyuki; Tatsumi, Takashi; Yoshitake, Hideaki
- Bulletin of the Chemical Society of Japan, Vol. 76, Issue 11