Abstract
We have designed and synthesized an isoreticular series of luminescent metal-organic frameworks (LMOFs) by incorporating a strongly emissive molecular fluorophore and functionally diverse colinkers into Zn-based structures. The three-dimensional porous networks of LMOF-261, -262, and -263 represent a unique/new type of nets, classified as a 2-nodal, (4,4)-c net (mot-e type) with 4-fold, class IIIa interpenetration. All compounds crystallize in a body-centered tetragonal crystal system (space group I41/a). A systematic study has been implemented to analyze their interactions with heavy metals. LMOF-263 exhibits impressive water stability, high porosity, and strong luminescence, making it an excellent candidate as a fluorescent chemical sensor and adsorbent for aqueous contaminants. It is extremely responsive to toxic heavy metals at a parts per billion level (3.3 ppb Hg2+, 19.7 ppb Pb2+) and demonstrates high selectivity for heavy metals over light metals, with detection ratios of 167.4 and 209.5 for Hg2+/Ca2+ and Hg2+/Mg2+, respectively. Mixed-metal adsorption experiments also show that LMOF-263 selectively adsorbs Hg2+ over other heavy metal ions in addition to light metals. The Pb2+ KSV value for LMOF-263 (55,017 M-1) is the highest among LMOFs reported to date, and the Hg2+ KSV value is the second highest (459,446 M-1). LMOF-263 exhibits a maximum adsorption capacity of 380 mg Hg2+/g. The Hg2+ adsorption process follows pseudo-second-order kinetics, removing 99.1% of the metal within 30 min. An in situ XPS study provides insight to help understand the interaction mechanism between Hg2+ and LMOF-263. No other MOFs have demonstrated such a high performance in both the detection and the capture of Hg2+ from aqueous solution.
| Original language | English |
|---|---|
| Pages (from-to) | 30294-30303 |
| Number of pages | 10 |
| Journal | ACS Applied Materials and Interfaces |
| Volume | 8 |
| Issue number | 44 |
| DOIs | |
| Publication status | Published - Nov 9 2016 |
Fingerprint
Keywords
- heavy metal adsorption
- heavy metal detection
- isoreticular series
- ligand-based emission
- luminescent metal-organic framework
ASJC Scopus subject areas
- Materials Science(all)
Cite this
Highly Efficient Luminescent Metal-Organic Framework for the Simultaneous Detection and Removal of Heavy Metals from Water. / Rudd, Nathan D.; Wang, Hao; Fuentes-Fernandez, Erika M.A.; Teat, Simon J.; Chen, Feng; Hall, Gene; Chabal, Yves J.; Li, Jing.
In: ACS Applied Materials and Interfaces, Vol. 8, No. 44, 09.11.2016, p. 30294-30303.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Highly Efficient Luminescent Metal-Organic Framework for the Simultaneous Detection and Removal of Heavy Metals from Water
AU - Rudd, Nathan D.
AU - Wang, Hao
AU - Fuentes-Fernandez, Erika M.A.
AU - Teat, Simon J.
AU - Chen, Feng
AU - Hall, Gene
AU - Chabal, Yves J.
AU - Li, Jing
PY - 2016/11/9
Y1 - 2016/11/9
N2 - We have designed and synthesized an isoreticular series of luminescent metal-organic frameworks (LMOFs) by incorporating a strongly emissive molecular fluorophore and functionally diverse colinkers into Zn-based structures. The three-dimensional porous networks of LMOF-261, -262, and -263 represent a unique/new type of nets, classified as a 2-nodal, (4,4)-c net (mot-e type) with 4-fold, class IIIa interpenetration. All compounds crystallize in a body-centered tetragonal crystal system (space group I41/a). A systematic study has been implemented to analyze their interactions with heavy metals. LMOF-263 exhibits impressive water stability, high porosity, and strong luminescence, making it an excellent candidate as a fluorescent chemical sensor and adsorbent for aqueous contaminants. It is extremely responsive to toxic heavy metals at a parts per billion level (3.3 ppb Hg2+, 19.7 ppb Pb2+) and demonstrates high selectivity for heavy metals over light metals, with detection ratios of 167.4 and 209.5 for Hg2+/Ca2+ and Hg2+/Mg2+, respectively. Mixed-metal adsorption experiments also show that LMOF-263 selectively adsorbs Hg2+ over other heavy metal ions in addition to light metals. The Pb2+ KSV value for LMOF-263 (55,017 M-1) is the highest among LMOFs reported to date, and the Hg2+ KSV value is the second highest (459,446 M-1). LMOF-263 exhibits a maximum adsorption capacity of 380 mg Hg2+/g. The Hg2+ adsorption process follows pseudo-second-order kinetics, removing 99.1% of the metal within 30 min. An in situ XPS study provides insight to help understand the interaction mechanism between Hg2+ and LMOF-263. No other MOFs have demonstrated such a high performance in both the detection and the capture of Hg2+ from aqueous solution.
AB - We have designed and synthesized an isoreticular series of luminescent metal-organic frameworks (LMOFs) by incorporating a strongly emissive molecular fluorophore and functionally diverse colinkers into Zn-based structures. The three-dimensional porous networks of LMOF-261, -262, and -263 represent a unique/new type of nets, classified as a 2-nodal, (4,4)-c net (mot-e type) with 4-fold, class IIIa interpenetration. All compounds crystallize in a body-centered tetragonal crystal system (space group I41/a). A systematic study has been implemented to analyze their interactions with heavy metals. LMOF-263 exhibits impressive water stability, high porosity, and strong luminescence, making it an excellent candidate as a fluorescent chemical sensor and adsorbent for aqueous contaminants. It is extremely responsive to toxic heavy metals at a parts per billion level (3.3 ppb Hg2+, 19.7 ppb Pb2+) and demonstrates high selectivity for heavy metals over light metals, with detection ratios of 167.4 and 209.5 for Hg2+/Ca2+ and Hg2+/Mg2+, respectively. Mixed-metal adsorption experiments also show that LMOF-263 selectively adsorbs Hg2+ over other heavy metal ions in addition to light metals. The Pb2+ KSV value for LMOF-263 (55,017 M-1) is the highest among LMOFs reported to date, and the Hg2+ KSV value is the second highest (459,446 M-1). LMOF-263 exhibits a maximum adsorption capacity of 380 mg Hg2+/g. The Hg2+ adsorption process follows pseudo-second-order kinetics, removing 99.1% of the metal within 30 min. An in situ XPS study provides insight to help understand the interaction mechanism between Hg2+ and LMOF-263. No other MOFs have demonstrated such a high performance in both the detection and the capture of Hg2+ from aqueous solution.
KW - heavy metal adsorption
KW - heavy metal detection
KW - isoreticular series
KW - ligand-based emission
KW - luminescent metal-organic framework
UR - http://www.scopus.com/inward/record.url?scp=84994744888&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84994744888&partnerID=8YFLogxK
U2 - 10.1021/acsami.6b10890
DO - 10.1021/acsami.6b10890
M3 - Article
VL - 8
SP - 30294
EP - 30303
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
SN - 1944-8244
IS - 44
ER -