期刊
ACS APPLIED MATERIALS & INTERFACES
卷 8, 期 44, 页码 30294-30303出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.6b10890
关键词
luminescent metal-organic framework; heavy metal detection; heavy metal adsorption; ligand-based emission; isoreticular series
资金
- Department of Energy, Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-08ER-46491]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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 ilia interpenetration. All compounds crystallize in a body-centered tetragonal crystal system (space group I4(1)/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 (459,4-46 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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