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Вид документа : Статья из журнала
Шифр издания :
Автор(ы) : Ehrling S., Senkovska I., Bon V., Evans J. D., Petkov P., Krupskaya Y., Kataev V., Wulf T., Krylov A. S., Vtyurin A. N., Krylova S. N., Adichtchev S., Slyusareva E., Weiss M. S., Buchner B., Heine T., Kaskel S.
Заглавие : Crystal size: Versus paddle wheel deformability: Selective gated adsorption transitions of the switchable metal-organic frameworks DUT-8(Co) and DUT-8(Ni)
Место публикации : J. Mater. Chem. A. - 2019. - Vol. 7, Is. 37. - P.21459-21475. - ISSN 20507488 (ISSN), DOI 10.1039/c9ta06781g
Примечания : Cited References: 106. - The authors thank DFG (FOR 2433) for financial support. We thank HZB for the allocation of synchrotron radiation beam-time and financial support. PP, TW and TH used high performance facilities of ZIH Dresden. TW thanks the European Social Funds for Germany for a PhD fellowship.
Аннотация: Switchable pillared layer metal–organic frameworks M2(2,6-ndc)2(dabco) (DUT-8(M), M = Ni, Co, 2,6-ndc = 2,6-naphthalenedicarboxylate, dabco = 1,4-diazabicyclo-[2.2.2]octane, DUT – Dresden University of Technology) were synthesised in two different crystallite size regimes to produce particles up to 300 μm and smaller particles around 0.1 μm, respectively. The textural properties and adsorption-induced switchability of the materials, obtained from both syntheses, were studied by physisorption of N2 at 77 K, CO2 at 195 K and n-butane at 273 K, revealing pronounced differences in adsorption behavior for Ni and Co analogues. While the smaller nano-sized particles (50–200 nm) are rigid and show no gating transitions confirming the importance of crystallite size, the large particles show pronounced switchability with characteristic differences for the two metals resulting in distinct recognition effects for various gases and vapours. Adsorption of various vapours demonstrates consistently a higher energetic barrier for the “gate opening” of DUT-8(Co) in contrast to DUT-8(Ni), as the “gate opening” pressure for Co based material is shifted to a higher value for adsorption of dichloromethane at 298 K. Evaluation of crystallographic data, obtained from single crystal and powder X-ray diffraction analysis, showed distinct geometric differences in the paddle wheel units of the respective MOFs. These differences are further disclosed by solid-state UV-vis, FT-IR and Raman spectroscopy. Magnetic properties of DUT-8(Co) and DUT-8(Ni) were investigated, indicating a high-spin state for both materials at room temperature. Density functional theory (DFT) simulations confirmed distinct energetic differences for Ni and Co analogues with a higher energetic penalty for the structural “gate opening” transformation for DUT-8(Co) compared to DUT-8(Ni) explaining the different flexibility behaviour of these isomorphous MOFs.
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Вид документа : Статья из журнала
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Автор(ы) : Huang J., Su B., Song E., Molokeev M. S., Xia Z.
Заглавие : Ultra-broad-band-excitable Cu(I)-based organometallic halide with near-unity emission for light-emitting diode applications
Место публикации : Chem. Mater. - 2021. - Vol. 33, Is. 12. - P.4382-4389. - ISSN 08974756 (ISSN), DOI 10.1021/acs.chemmater.1c00085
Примечания : Cited References: 43. - This research was supported by the National Natural Science Foundation of China (Grant Nos. 51961145101 and 51972118), the Fundamental Research Funds for the Central Universities (D2190980), the Guangzhou Science and Technology Project (202007020005), International Cooperation Project of National Key Research and Development Program of China (2021YFE0105700), and the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01X137). The reported study was also funded by RFBR according to research project no. 19-52-80003
Аннотация: Low-dimensional hybrid metal halides demonstrate broad-band emission and high photoluminescence quantum yield (PLQY) acting as excellent candidates for a new generation of luminescent materials in lighting fields. However, most luminescent metal halides can only be excited by ultraviolet radiation, and the discovery of high-efficient emitters with broad-band excitation characteristics, especially upon efficient blue light irradiation, is a challenge. Herein, a zero-dimensional (0D) Cu(I)-based organometallic halide (18-crown-6)2Na2(H2O)3Cu4I6 (CNCI) was prepared with a green emission band centered at 536 nm and a near-unity PLQY (91.8%) upon excitation of 450 nm. Importantly, the ultrabroad excitation band covering a 300-500 nm range was observed in CNCI, and the luminescence mechanism has been discussed in detail. A white light-emitting diode (WLED) was fabricated with high luminous efficiency of 156 lm/W and a high color rendering index of 89.6. This work provides guidance for designing high-performance luminescent metal halides with suitable excitation characteristics and also promotes the application prospects of such materials in WLED fields.
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Вид документа : Статья из журнала
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Автор(ы) : Hoffman A. E.J., Senkovska I., Wieme J., Krylov A. S., Kaskel S., Van Speybroeck V.
Заглавие : Unfolding the terahertz spectrum of soft porous crystals: rigid unit modes and their impact on phase transitions
Место публикации : J. Mater. Chem. A. - 2022. - Vol. 10, Is. 33. - P.17254-17266. - ISSN 20507488 (ISSN), DOI 10.1039/d2ta01678h
Примечания : Cited References: 80. - This work was financially supported by the Fund for Scientific Research Flanders (FWO), the Research Board of the Ghent University (BOF), the Deutsche Forschungsgemeinschaft (DFG, project number 448809307), and the Russian Foundation for Basic Research (RFBR, project number 21-52-12018). The authors thank Kerstin Zechel for sample synthesis. The computational resources and services used in this work were provided by the Flemish Supercomputer Center (VSC), funded by FWO and the Flemish Government
Аннотация: Phase transitions in flexible metal-organic frameworks or soft porous crystals are mediated by low-frequency phonons or rigid-unit modes. The alteration of specific building blocks may change the lattice dynamics of these frameworks, which can influence the phase transition mechanism. In this work, the impact of building block substitution on the rigid-unit modes in flexible MIL-53 analogs with a winerack topology will be investigated via ab initio lattice dynamics calculations. First, the accuracy of the theoretical simulations is verified via experimental Raman measurements, which provide unique fingerprint vibrations in the terahertz range to characterize the phase transition. Following analysis of the low-frequency vibrations shows that there exists a set of universal rigid-unit modes inducing translations and/or rotations of the building blocks. The theoretical results demonstrate that linker substitutions have a large effect on the rigid-unit mode frequencies, whereas this is less so for inorganic chain substitutions. These findings may help to rationally tune the phonon frequencies in soft porous crystals.
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