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Reversible Humidity-Driven Transformation of a Bimetallic {EuCo} Molecular Material: Structural, Sorption, and Photoluminescence Studies.

ABSTRACT: Functional molecule-based solids built of metal complexes can reveal a great impact of external stimuli upon their optical, magnetic, electric, and mechanical properties. We report a novel molecular material, {[Eu^III(H₂O)₃(pyrone)₄][Co^III(CN)₆]}·nH₂O (1, n = 2; 2, n = 1), which was obtained by the self-assembly of Eu³⁺ and [Co(CN)₆]^3- ions in the presence of a small 2-pyrrolidinone (pyrone) ligand in an aqueous medium. The as-synthesized material, 1, consists of dinuclear cyanido-bridged {EuCo} molecules accompanied by two H-bonded water molecules. By lowering the relative humidity (RH) below 30% at room temperature, 1 undergoes a single-crystal-to-single-crystal transformation related to the partial removal of crystallization water molecules which results in the new crystalline phase, 2. Both 1 and 2 solvates exhibit pronounced Eu^III-centered visible photoluminescence. However, they differ in the energy splitting of the main emission band of a ⁵D₀ ? ⁷F₂ origin, and the emission lifetime, which is longer in the partially dehydrated 2. As the 1 ? 2 structural transformation can be repeatedly reversed by changing the RH value, the reported material shows a room-temperature switching of detailed luminescent features including the ratio between emission components and the emission lifetime values.

SUBMITTER: Zakrzewski JJ

PROVIDER: S-EPMC7923019 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Reversible Humidity-Driven Transformation of a Bimetallic {EuCo} Molecular Material: Structural, Sorption, and Photoluminescence Studies.

Zakrzewski Jakub J JJ Heczko Michal M Jankowski Robert R Chorazy Szymon S

Molecules (Basel, Switzerland) 20210219 4

Functional molecule-based solids built of metal complexes can reveal a great impact of external stimuli upon their optical, magnetic, electric, and mechanical properties. We report a novel molecular material, {[EuIII(H2O)3(pyrone)4][CoIII(CN)6]}·nH2O (1, n = 2; 2, n = 1), which was obtained by the self-assembly of Eu3+ and [Co(CN)6]3- ions in the presen ...[more]

PMID: 33669754

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Project description:Nuclear power facilities are being expanded to satisfy expanding worldwide energy demand. Thus, uranium recovery from secondary resources has become a hot topic in terms of environmental protection and nuclear fuel conservation. Herein, a mesoporous biosorbent of a hybrid magnetic-chitosan nanocomposite functionalized with cysteine (Cys) was synthesized via subsequent heterogeneous nucleation for selectively enhanced uranyl ion (UO22+) sorption. Various analytical tools were used to confirm the mesoporous nanocomposite structural characteristics and confirm the synthetic route. The characteristics of the synthesized nanocomposite were as follows: superparamagnetic with saturation magnetization (MS: 25.81 emu/g), a specific surface area (SBET: 42.56 m2/g) with a unipore mesoporous structure, an amine content of ~2.43 mmol N/g, and a density of ~17.19/nm2. The experimental results showed that the sorption was highly efficient: for the isotherm fitted by the Langmuir equation, the maximum capacity was about 0.575 mmol U/g at pH range 3.5-5.0, and Temperature (25 ± 1 °C); further, there was excellent selectivity for UO22+, likely due to the chemical valent difference. The sorption process was fast (~50 min), simulated with the pseudo-second-order equation, and the sorption half-time (t1/2) was 3.86 min. The sophisticated spectroscopic studies (FTIR and XPS) revealed that the sorption mechanism was linked to complexation and ion exchange by interaction with S/N/O multiple functional groups. The sorption was exothermic, spontaneous, and governed by entropy change. Desorption and regeneration were carried out using an acidified urea solution (0.25 M) that was recycled for a minimum of six cycles, resulting in a sorption and desorption efficiency of over 91%. The as-synthesized nanocomposite's high stability, durability, and chemical resistivity were confirmed over multiple cycles using FTIR and leachability. Finally, the sorbent was efficiently tested for selective uranium sorption from multicomponent acidic simulated nuclear solution. Owing to such excellent performance, the Cys nanocomposite is greatly promising in the uranium recovery field.

Dataset Information

Reversible Humidity-Driven Transformation of a Bimetallic {EuCo} Molecular Material: Structural, Sorption, and Photoluminescence Studies.

Publications

Reversible Humidity-Driven Transformation of a Bimetallic {EuCo} Molecular Material: Structural, Sorption, and Photoluminescence Studies.

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