“Hot-node” controlled facile synthesis of 3D rare earth micro-networks with symmetry deviation induced high luminescence

Chen, Bin-Bin; Lv, Jian; Chang, Shuai; Wang, Xiao-Yuan; Qian, Ruo‐Can; Li, Dawei

doi:10.1039/d0tc02919j

Cited by 18 publications

(9 citation statements)

References 42 publications

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“…Luminescent rare earth complexes have become the research hotspot of new rare earth functional materials, because of their unique luminescence properties, such as extremely sharp emission bands [1,2], long excited-state lifetimes [3][4][5], and potential high internal quantum efficiency [6][7][8]. When rare earth metals are complexed with appropriate organic ligands, their improved solubility and dispersion would make their luminescence properties more prominent than they are in states of inorganic salts [9,10].…”

Section: Introductionmentioning

confidence: 99%

Eu3+- and Tb3+-Based Coordination Complexes of Poly(N-Isopropyl,N-methylacrylamide-stat-N,N-dimethylacrylamide) Copolymer: Synthesis, Characterization and Property

Cui

et al. 2022

Polymers

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This contribution reports the syntheses, structural analyses and properties of europium (Eu3+)- and terbium (Tb3+)-based coordination complexes of poly(N-isopropyl,N-methylacrylamide-stat-N,N-dimethylacrylamide) (poly(iPMAm-stat-DMAm)) copolymer, named as poly-Eu(III) and poly-Tb(III), respectively. In greater detail, poly(iPMAm85-stat-DMAm15) is first prepared by random copolymerization of N-isopropyl,N-methylacrylamide (iPMAm) and N,N-dimethylacrylamide (DMAm) via group transfer polymerization (GTP). Next, poly(iPMAm85-stat-DMAm15) is used as the polymer matrix for chelating with Eu3+ and Tb3+ cations at its side amide groups, to produce poly-Eu(III) and poly-Tb(III). Their structural characterizations by FT-IR spectroscopy and XPS confirm the formation of polymeric complexes. The study on their fluorescence emission characteristics and luminescence lifetime demonstrates that Poly-Eu(III) shows four strong emission peaks at 578, 593, 622, and 651 nm, which are responsible for the electron transitions from the excited 5D0 state to the multiplet 7FJ (J = 0, 1, 2, 3) states, respectively, and poly-Tb(III) also displays four emission peaks at 489, 545, 588, and 654 nm, mainly due to the electron transitions of 5D4 → 7Fi (i = 6, 5, 4, 3). The luminescence lifetimes of poly-Eu(III) (τpoly-Eu(III)) and poly-Tb(III) (τpoly-Tb(III)) are determined to be 4.57 and 7.50 ms, respectively. In addition, in aqueous solutions, poly-Eu(III) and poly-Tb(III) are found to exhibit thermoresponsivity, with their cloud temperatures (Tcs) locating around 36.4 and 36.8 °C, respectively. Finally, the cytotoxicity study on the human colon carcinoma cells LoVo and DLD1 suggests that the luminescent Eu3+ and Tb3+ in the chelated state with poly(iPMAm-stat-DMAm) show much better biocompatibility and lower toxicity than their inorganic salts.

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Section: Introductionmentioning

confidence: 99%

Eu3+- and Tb3+-Based Coordination Complexes of Poly(N-Isopropyl,N-methylacrylamide-stat-N,N-dimethylacrylamide) Copolymer: Synthesis, Characterization and Property

Cui

et al. 2022

Polymers

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“…Advanced functional materials play an important role in promoting the progress and development of science and technology. − Among various functional materials, two-dimensional (2D) nanomaterials such as graphene and graphitic carbon nitride show high mechanical flexibility, optical transparency, and electronic properties because of the structural characteristics of ultrathin thickness, large lateral size, and surface area. − To improve the structural and functional properties of 2D nanomaterials, various strategies such as hybridization, , heteroatom doping, surface defect, and pore engineering have been developed. Of which, pore engineering endows 2D nanomaterials with nanopore structure to improve the density of active sites and the charge/mass transport, expanding their application ranges.…”

Section: Introductionmentioning

confidence: 99%

Large-Scale Manual Grinding Preparation of Ultrathin Porous Sulfur (S₈)-Anchored ScOOH Nanosheets for Photothermal Conversion and Dye Adsorption

Chen

Wang

Chang

et al. 2022

ACS Appl. Nano Mater.

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Porous two-dimensional (2D) nanomaterials have attracted much attention in recent years and shown unique electronic and physicochemical properties by utilizing the advantages of both porous structure and 2D architecture. However, the low-cost, large-scale, and high-quality synthesis of porous 2D nanomaterials is still very challenging. Herein, for the first time, we develop a facile manual grinding strategy for the preparation of ultrathin porous sulfur (S 8 )-anchored ScOOH nanosheets (S 8 /ScOOH-NSs) by the mechanical stripping of S 8 -anchored ScOOH nanorods (S 8 /ScOOH-NRs). The formation of S 8 /ScOOH-NSs should be due to the intrinsic lamellar structure of S 8 /ScOOH-NRs. The obtained S 8 /ScOOH-NSs with rich mesopores have a high-quality crystal structure. Because of hydrophobic sulfur and carbon components on the surface, S 8 /ScOOH-NSs show good hydrophobicity. In addition, S 8 /ScOOH-NSs exhibit more excellent photothermal conversion efficiency and adsorption capacity compared with S 8 /ScOOH-NRs, which is directly attributed to the synergistic effect of sulfur-doping, porous structure, and 2D architecture. Therefore, the facile and large-scale synthesis strategy endows S 8 / ScOOH-NSs with multifunctional properties that have great application prospects in water cleaning and photothermal evaporators.

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“…Therefore, the explanation is that the formation of the Si–O–Si structure during the sol–gel reaction has made the change of the symmetry of the Eu 3+ ion coordination environment from high to low, away from the center of inversion. This phenomenon of luminescence enhancement is directly attributed to the symmetry deviation-induced transition effect …”

Section: Resultsmentioning

confidence: 93%

“…This phenomenon of luminescence enhancement is directly attributed to the symmetry deviation-induced transition effect. 53 In order to further explore the influence of the formation of the Si−O−Si structure on the coordination environment of Eu 3+ ions, the Judd−Ofelt theory 54,55 was introduced, which allows for the calculation of the manifold transition probabilities that can predict the important radiative properties of lanthanide ions. The Ω λ parameters depend on the local geometry, bonding atoms, and polarizability of the first coordination sphere of lanthanide ions.…”

Section: Resultsmentioning

confidence: 99%

Structure-Dependent Photoluminescence of Europium(III) Coordination Oligomeric Silsesquioxane: Synthesis and Mechanism

Wang

et al. 2020

ACS Omega

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The coordination environment of Eu3+ is a crucial factor in the optical performance of the complex. Herein, a new kind of oligomeric silsesquioxane was employed to improve the coordination environment of central ions, the luminescence intensity of which was greatly enhanced with an efficient emission peak at 619 nm. More importantly, the photoluminescent properties of the product will be altered because of the formation of the Si–O–Si structure. The relevant mechanism has also been investigated and proposed by a series of characterization analyses. Additionally, the fluorescence lifetime, intrinsic quantum yield, and energy transfer efficiency were calculated. In addition, the observed trend of Judd–Ofelt intensity parameters was used to justify the coordination environment of Eu3+ ions. The experimental results reveal that the sol–gel reaction of the ligands can effectively promote intramolecular energy transfer. In addition, we introduced four theory modules of ligands (LSi, LSi-1, LSi-2, and LSi-3) with certain rules of formation of Si–O–Si, and density functional theory (DFT) and time-dependent DFT (TD-DFT) were used to explore their excited electron transfer process and their electronic absorption spectra, combined with Marcus theory. The calculated results show that the sol–gel reaction will induce the separation of the distribution of excited holes and electrons, leading to an efficient charge-transfer (CT) process. The predictable results were in good accordance with the experimental findings. Consequently, the sol–gel reaction occurring among ligands will be attributed to an efficient CT process, leading to a strong luminescence intensity, as observed experimentally.

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“Hot-node” controlled facile synthesis of 3D rare earth micro-networks with symmetry deviation induced high luminescence

Abstract: Controlled self-assembly is a powerful strategy for building mesoscopic superstructures. However, the construction of high luminescent, millimeter-sized and spatially well-defined 3D rare earth (RE) material assembles is a challenging objective....

Cited by 18 publications

References 42 publications

Eu3+- and Tb3+-Based Coordination Complexes of Poly(N-Isopropyl,N-methylacrylamide-stat-N,N-dimethylacrylamide) Copolymer: Synthesis, Characterization and Property

Eu3+- and Tb3+-Based Coordination Complexes of Poly(N-Isopropyl,N-methylacrylamide-stat-N,N-dimethylacrylamide) Copolymer: Synthesis, Characterization and Property

Large-Scale Manual Grinding Preparation of Ultrathin Porous Sulfur (S₈)-Anchored ScOOH Nanosheets for Photothermal Conversion and Dye Adsorption

Structure-Dependent Photoluminescence of Europium(III) Coordination Oligomeric Silsesquioxane: Synthesis and Mechanism

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“Hot-node” controlled facile synthesis of 3D rare earth micro-networks with symmetry deviation induced high luminescence

Abstract: Controlled self-assembly is a powerful strategy for building mesoscopic superstructures. However, the construction of high luminescent, millimeter-sized and spatially well-defined 3D rare earth (RE) material assembles is a challenging objective....

Cited by 18 publications

References 42 publications

Eu3+- and Tb3+-Based Coordination Complexes of Poly(N-Isopropyl,N-methylacrylamide-stat-N,N-dimethylacrylamide) Copolymer: Synthesis, Characterization and Property

Eu3+- and Tb3+-Based Coordination Complexes of Poly(N-Isopropyl,N-methylacrylamide-stat-N,N-dimethylacrylamide) Copolymer: Synthesis, Characterization and Property

Large-Scale Manual Grinding Preparation of Ultrathin Porous Sulfur (S8)-Anchored ScOOH Nanosheets for Photothermal Conversion and Dye Adsorption

Structure-Dependent Photoluminescence of Europium(III) Coordination Oligomeric Silsesquioxane: Synthesis and Mechanism

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Large-Scale Manual Grinding Preparation of Ultrathin Porous Sulfur (S₈)-Anchored ScOOH Nanosheets for Photothermal Conversion and Dye Adsorption