Two series of lanthanide metal–organic frameworks (Ln-MOFs) from two structurally related flexible carboxylate-based ligands were solvothermally synthesized. H3L2 with additional −CH2− group provides more flexibility and different coordination modes and conformations compared with H3L1. As a result, 2-Ln MOFs are modulated from two-dimensional kgd of 1-Ln to three-dimensional rtl topological frameworks and further achieve enhanced chemical stability. The Eu- and Tb-MOFs exhibit strong fluorescent emission at the solid state because of the antenna effect of the ligands. Interestingly, the emissions can be tuned by simply doping Eu3+ and Tb3+ of different concentrations within the Eu x Tb 1–x MOFs. Notably, 2-Ln MOFs realize nearly white light emission by means of a trichromatic approach (red of Eu(III), green of Tb(III), and blue of the H3L2 ligand). Furthermore, 2-Ln MOFs also exhibit water stability and demonstrate high selective and sensitive sensing activities toward Fe(III) and Cr(VI) in aqueous solutions. The results further highlight the importance of the ligand flexibility on tuning MOF structures with improved structural stability and ion-sensing properties.
Lowering platinum (Pt) loadings without sacrificing power density and durability in fuel cells is highly desired yet challenging because of the high mass transport resistance near the catalyst surfaces. We tailored the three-phase microenvironment by optimizing the ionomer by incorporating ionic covalent organic framework (COF) nanosheets into Nafion. The mesoporous apertures of 2.8 to 4.1 nanometers and appendant sulfonate groups enabled the proton transfer and promoted oxygen permeation. The mass activity of Pt and the peak power density of the fuel cell with Pt/Vulcan (0.07 mg of Pt per square centimeter in the cathode) both reached 1.6 times those values without the COF. This strategy was applied to catalyst layers with various Pt loadings and different commercial catalysts.
Luminescent metal–organic frameworks (LMOFs) as sensors showing highly efficient detection toward toxic heavy-metal ions are in high demand for human health and environmental protection. A novel nanocage-based N-rich LMOF (LCU-103) has been constructed and characterized. It is a 2-fold interpenetrating structure built from N-rich {Zn6(dttz)4} nanocages extended by N-donor ligand Hdpa [H3dttz = 4,5-di(1H-tetrazol-5-yl)-2H-1,2,3-triazole; Hdpa = 4,4′-dipyridylamine]. Notably, LCU-103 contains abundant N functional sites anchoring on both the windows of nanocages and the inner channels of the framework that can interact with metal ions and then recognize them. As a result, it can serve as a luminescent sensing material for detecting trace amounts of Fe3+ and Cu2+ ions with low limits of detection (LODs) of 1.45 and 1.66 μM, respectively, through a luminescent quenching mechanism. Meanwhile, LCU-103 as a LMOF sensor exhibits several advantages such as high sensitivity, appropriate selectivity (for Fe3+ in H2O), recycling stability, and fast response times in N,N-dimethylformamide. Moreover, LCU-103 also displays good luminescent quenching activity toward Fe3+ in H2O and a simulated 4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid biological system with low LODs of 1.51 and 1.52 μM, respectively. LCU-103 test papers were further prepared to offer easy and real-time detection of Fe3+ and Cu2+ ions. Importantly, when density functional theory calculations and multiple experimental evidence, including X-ray photoelectron spectroscopy, UV–vis absorption, luminescence decay lifetimes, and quantum efficiencies, are combined, a preferred N-donor site and possible weak interaction sensing mechanism is also proposed to elucidate the quenching effect.
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