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

doi:10.1021/acsami.6b10890

Title: Highly Efficient Luminescent Metal–Organic Framework for the Simultaneous Detection and Removal of Heavy Metals from Water

Journal Article · Thu Oct 13 00:00:00 EDT 2016 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.6b10890· OSTI ID:1436604

Rudd, Nathan D. ^[1]; Wang, Hao ^[1]; Fuentes-Fernandez, Erika M. A. ^[2]; Teat, Simon J. ^[3]; Chen, Feng ^[4]; Hall, Gene ^[1]; Chabal, Yves J. ^[2]; Li, Jing ^[1]

Rutgers Univ., Piscataway, NJ (United States). Dept. of Chemistry and Chemical Biology
Univ. of Texas-Dallas, Richardson, TX (United States). Dept. of Materials Science and Engineering
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Rider Univ., Lawrenceville, NJ (United States). Dept. of Chemistry, Biochemistry and Physics

For this work, 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⁺ K_SV value for LMOF-263 (55,017 M^-1) is the highest among LMOFs reported to date, and the Hg²⁺ K_SV 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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Horiba, Ltd., Kyoto (Japan)

Grant/Contract Number:: AC02-05CH11231; FG02-08ER-46491

OSTI ID:: 1436604

Journal Information:: ACS Applied Materials and Interfaces, Vol. 8, Issue 44; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Highly Efficient Luminescent Metal–Organic Framework for the Simultaneous Detection and Removal of Heavy Metals from Water

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