Ultrasensitive and Selective Detection of Uranium by a Luminescent Terbium–Organic Framework

Lei, M.; Jia, Yuyu; Zhang, Wei; Xie, Jian; Xu, Zhijun; Wang, Yanlong; Du, Wei

doi:10.1021/acsami.1c16742

Cited by 29 publications

(15 citation statements)

References 63 publications

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“…The porosity of Eu-MTB was determined to be 58.6% based on the PLATON analysis. Note that our Tb-MTB with a structure similar to ionic Ln-MOF has been reported by Liu et al and Lei et al [45,46]. By replacing the pyrazine group of TPP unit with a phenyl ring, the geometry of the tetratopic carboxylate-based ligand can be fixed on a square and rectangular planar.…”

Section: Structural and Topologicalsupporting

confidence: 52%

Precise Design and Deliberate Tuning of Turn-On Fluorescence in Tetraphenylpyrazine-Based Metal−Organic Frameworks

Zheng

Zhang

et al. 2022

Research

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The manipulation on turn-on fluorescence in solid state materials attracts increasing interests owing to their widespread applications. Herein we report how the nonradiative pathways of tetraphenylpyrazine (TPP) units in metal−organic frameworks (MOFs) systems could be hindered through a topological design approach. Two MOFs single crystals of different topology were constructed via the solvothermal reaction of a TPP-based 4,4′,4″,4‴-(pyrazine-2,3,5,6-tetrayl) tetrabenzoic acid (H4TCPP) ligand and metal cations, and their mechanisms of formation have been explored. Compared with the innate low-frequency vibrational modes of flu net Tb-TCPP-1, such as phenyl ring torsions and pyrazine twists, Tb-TCPP-2 adopts a shp net, so the dihedral angle of pyrazine ring and phenyl arms is larger, and the center pyrazine ring in TPP unit is coplanar, which hinders the radiationless decay of TPP moieties in Tb-TCPP-2. Thereby Tb-TCPP-2 exhibits a larger blue-shifted fluorescence and a higher fluorescence quantum yield than Tb-TCPP-1, which is consistent with the reduced nonradiative pathways. Furthermore, Density functional theory (DFT) studies also confirmed aforementioned tunable turn-on fluorescence mechanism. Our work constructed TPP-type MOFs based on a deliberately topological design approach, and the precise design of turn-on fluorescence holds promise as a strategy for controlling nonradiative pathways.

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Section: Structural and Topologicalsupporting

confidence: 52%

Precise Design and Deliberate Tuning of Turn-On Fluorescence in Tetraphenylpyrazine-Based Metal−Organic Frameworks

Zheng

Zhang

et al. 2022

Research

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“…FT-IR and XPS spectra of U-ZIF-L-hemin-contained distinct peaks of OUO at 910 cm −1 (Figure 5D) and strong U 4f signals (4f 5/2 : 392.4 eV, 4f 7/2 : 381.7 eV, Figure 5E), confirming that uranium was present. The coordination of UO 2 2+ with the ZIF-L-hemin was suggested by the obvious redshift (∼50, 960 cm −1 for pristine uranyl nitrate 46,47 ) in FT-IR spectra (Figure 5D) and the considerably lower binding energies of U 4f in XPS spectra compared to pristine uranyl nitrate (Figure S16). Moreover, the UV−vis spectra data of ZIF-L-hemin showed a blueshift, indicating that the interaction between imidazole and hemin was blocked due to competing ligands of U (Figure 5F).…”

Section: Resultsmentioning

confidence: 97%

Insertion of Hemin into Metal–Organic Frameworks: Mimicking Natural Peroxidase Microenvironment for the Rapid Ultrasensitive Detection of Uranium

Zhou

Hao

et al. 2022

Anal. Chem.

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Constructing enzyme-like active sites in mimic enzyme systems is critical for achieving catalytic performances comparable to natural enzymes and can shed light on the natural development of enzymes. In this study, we described a specific hemin-based mimetic enzyme, which was facilely synthesized by the assembly of zeolitic imidazolate framework-L (ZIF-L) and hemin. The obtained hemin-based mimetic enzyme (denoted as ZIF-L-hemin) displayed enhanced peroxidase activity compared to free hemin in solution. Such excellent activity originated from the ZIF-L framework mimicking the active site cavity microenvironment of horseradish peroxidase in terms of axially coordinated histidine and distal histidine. Additionally, the constructed peroxidase mimetic was extremely resistant to a variety of severe circumstances that would normally denature natural enzymes. These characteristics made ZIF-L-hemin a potential platform for the colorimetric sensor of uranium (UO 2 2+ ) with wide linear ranges (0.25−40 μM) and low limits of detection (0.079 μM). Moreover, the detection mechanism demonstrated that the coordination of uranyl ion with imidazole of ZIF-L-hemin reduced the catalytic efficiency of ZIF-L-hemin. The current work not only proposed a novel approach for fabricating artificial peroxidase but also offered facile colorimetric methods for selective radionuclide detection.

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“…As a new class of hybrid materials assembled from metal nodes and organic linkers, metal–organic frameworks (MOFs) are scientifically compelling in gas storage, separation, sensing, catalysis, and so forth. − Their tunability in terms of chemical composition and structure renders MOFs as promising candidate materials for radionuclide sensing. − Incorporating photoluminescent (PL) metal centers or organic phosphors within the frameworks endows sensing capacities of MOFs toward the target radionuclides via emission alteration of the host. , Furthermore, phosphors can be orderly and spatially distributed in rigid luminescent MOFs, eliminating luminescence quenching induced by agglomeration and boosting the detection sensitivity. , In addition, the feasible in-and-out channels and tailorable binding site of MOFs allow for sensing of target radionuclides with high selectivity. , However, only a few MOFs for sensing of UO 2 2+ have been documented. − Those for detection of the I – anion have been barely reported, and the most relevant cases thus far include Ln 2 Zn(L) 3 (H 2 O) 4 ](NO 3 ) 2 (Ln = Eu or Tb), [Eu 4 (OH) 4 (tcbpp) 2 (H 2 O) 9 ]Cl 8 , Cd 2.5 (PDA)(tz) 3 , and Tb(cpia)(H 2 O) 2 . − Moreover, the hydrolytic stability, a key parameter of the chemosensor for practical applications under environmentally relevant conditions, was not investigated in most studies. − …”

Section: Introductionmentioning

confidence: 99%

Hydrolytically Stable Zr-Based Metal–Organic Framework as a Highly Sensitive and Selective Luminescent Sensor of Radionuclides

Wang

Zhu

et al. 2022

Inorg. Chem.

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Effective detections of radionuclides including uranium and its predominant fission products, for example, iodine, are highly desired owing to their radiotoxicity and potential threat to human health. However, traditional analytical techniques of radionuclides are instrument-demanding, and chemosensors targeted for sensitization of radionuclides remain limited. In this regard, we report a sensitive and selective sensor of UO 2 2+ and I − based on the unique quenching behavior of a luminescent Zr-based metal−organic framework, Zr 6 O 4 (OH) 4 (OH) 6 (H 2 O) 6 (TCPE) 1.5 • (H 2 O) 24 (C 3 H 7 NO) 9 (Zr-TCPE). Immobilization of the luminescent tetrakis(4-carboxyphenyl)ethylene (TCPE 4− ) linkers by Zr 6 nodes enhances the photoluminescence quantum yield of Zr-TCPE, which facilitates the effective sensing of radionuclides in a "turn-off" manner. Moreover, Zr-TCPE can sensitively and selectively recognize UO 2 2+ and I − ions with the lowest limits of detection of 0.67 and 0.87 μg/kg, respectively, of which the former one is much lower than the permissible value (30 μg/L) defined by the U.S. EPA. In addition, Zr-TCPE features excellent hydrolytic stability and can withstand pH conditions ranging from 3 to 11. To facilitate real-world applications, we have further fabricated polyvinylidene fluoride-integrating Zr-TCPE as luminescence-based sensor membranes for on-site sensing of UO 2 2+ and I − .

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Ultrasensitive and Selective Detection of Uranium by a Luminescent Terbium–Organic Framework

Cited by 29 publications

References 63 publications

Precise Design and Deliberate Tuning of Turn-On Fluorescence in Tetraphenylpyrazine-Based Metal−Organic Frameworks

Precise Design and Deliberate Tuning of Turn-On Fluorescence in Tetraphenylpyrazine-Based Metal−Organic Frameworks

Insertion of Hemin into Metal–Organic Frameworks: Mimicking Natural Peroxidase Microenvironment for the Rapid Ultrasensitive Detection of Uranium

Hydrolytically Stable Zr-Based Metal–Organic Framework as a Highly Sensitive and Selective Luminescent Sensor of Radionuclides

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