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A novel
Lanthanide-based single-molecule magnets (Ln-SMMs) showing stimuli-responsive changes in photoluminescence (PL) and magnetic properties are attractive for their potential applications in information storage and molecular devices. In this work, we report two mononuclear complexes, namely, Dy(SCN)2(NO3)(Cl-depma)2(4-hpy)2(Dy-Cl) and Dy(SCN)2(NO3)(Br-depma)2(4-hpy)2(Dy-Br), where X-depma represents 10-X-9-diethylphosphinomethylanthracene (X = Cl, Br) and 4-hpy is 4-hydroxypyridine. Both contain face-to-face π-π-interacted anthracene rings and exhibit yellow-green excimer emission. Unlike the other related Dy–anthracene complexes without a halogen substituent,Dy-ClandDy-Brcannot undergo photocycloaddition reaction under UV-light irradiation. However, they exhibited remarkable grinding-induced changes in luminescence. Magnetic studies revealed thatDy-ClandDy-Brshow SMM behavior under zero dc field with the effective energy barriers (Ueff/kB) of 259 K and 264 K, respectively. We also investigated the effect of pressure on the magnetic properties ofDy-Brand observed a reduction in the magnetization value, narrowing of the butterfly-shaped hysteresis loop, and acceleration of the magnetic relaxation under 1.09 GPa. The results demonstrate that introducing a halogen substituent into an anthracene group may pose significant influences on the photophysical and photochemical properties of the complexes. In addition, pressure may be a promising external stimulus to modulate the PL and SMM behaviors of Dy–anthracene complexes.
It has been challenging to integrate various medical imaging modalities into an ultra-small nanoparticle with good biocompatibility to build highly efficient multimodal imaging nanoprobes. A new manganese and dysprosium codoped carbon quantum dots (Mn,Dy-CQDs) with a mean diameter of 1.77 nm was synthesized for fluorescence imaging, T1/T2-weighted magnetic resonance imaging (T1/T2-weighted MRI), and x-ray computed tomography (CT) imaging using a simple one-step hydrothermal approach. The obtained Mn,Dy-CQDs showed good water solubility, long-term stability, strong stable fluorescence property (fluorescence quantum yield of 31.62%), and excellent biocompatibility. The cell imaging verified that the Mn,Dy-CQDs have high efficiency of fluorescence imaging. The Mn,Dy-CQDs, on the other hand, had a superior x-ray absorption performance (47.344 HU l g−1), a higher longitudinal relaxivity (r1 = 7.47 mM−1 s−1), a higher transverse relaxivity (r2 = 42.686 mM−1 s−1). In vitro T1/T2-weighted MRI and CT imaging showed that Mn,Dy-CQDs can produce a strong contrast enhancement impact. To summarise, the Mn,Dy-CQDs may be used as a T1/T2-weighted MRI/CT/fluorescent quadri-modal imaging nanoprobe, indicating that they have a lot of uses in biomedical multimode imaging and clinics.
The adsorption of dysprosium ions from rare earth waste by hydrometallurgy is of great significance for both sustainable resource development and environmental protection. However, poor adsorption kinetics, low selectivity and difficult desorption regeneration cycle of adsorption limit the separation and recovery of rare earth ions. Herein, a photo-responsive imprinted cellulose nanocrystal composite aerogel (P-IAM) was prepared by introducing azobenzene-silane for selective adsorption of dysprosium ions. Highly ordered pore structure templated by cellulose nanocrystal effectively improve the adsorption rate; coupled with ion imprinting technology for highly selective adsorption separation of Dy 3+ ; more importantly, inspired by nature's light response, light response modulation mechanism of aerogel can achieve green desorption. It was shown that the adsorption–desorption of P-IAM was possible under the variation of Vis-UV light. When Dy 3+ solution concentration was 250 mg/L, the maximum adsorption capacity of P-IAM achieved 68.65 mg g −1 . In the presence of competing ions, P-IAM still has good recognition and memory ability for Dy(III). In addition, P-IAM was still able to reach 87.19% of its initial adsorption capacity after five cycles, maintaining a good adsorption capacity and green regeneration capability. These studies provide a green technology basis for the recovery of Dy(III).
In the field of white-light LED lighting technology, the development of single-phase white light emitting phosphors with excellent luminescent thermal stability has been the core research focus. This study introduced a color-tunable Na 3 YSi 2 O 7 : x Tm 3+ , y Dy 3+ (abbreviated as NYSO: x Tm 3+ , y Dy 3+ ) phosphor. Under an excitation wavelength of 351 nm, through the energy transfer (ET) process from Tm 3+ to Dy 3+ dominated by dipole-dipole interactions and by finely adjusting the doping ratios of Tm 3+ and Dy 3+ ions, white light emission was successfully achieved in the NYSO:5%Tm 3+ ,1%Dy 3+ phosphor. The phosphor exhibited color coordinates at (0.340, 0.344), which were extremely close to the ideal white light region. Notably, the NYSO:5%Tm 3+ ,1%Dy 3+ phosphor exhibited remarkable thermal stability luminescent performance. At high temperatures of 424 K and 474 K, its emission intensity only decreased by 3.64% and 6.10%, respectively. Moreover, at a high temperature of 474 K, the chromaticity shift ( Δε ) of the phosphor was merely 6.16×10 -3 , demonstrating far superior anti-thermal quenching and luminescent color stability performance compared with similar phosphor materials. This work provided a new strategy for addressing the thermal stability issue of white LED phosphors and was expected to facilitate the advancement of white LED lighting technology.
New and sustainable approaches for the removal of cationic organic pollutants, such as methyl violet (MV) and methylene blue (MB) dyes, from aqueous solutions are needed. In this study, hickory wood was pyrolyzed with montmorillonite and then ball milled with dysprosium oxide at 350 rpm for 3 h, without any use of toxic compounds. The resulting composite was rich in oxygen-containing functional groups (e.g., carboxyl and hydroxyl), had uniform lamellar-porous micromorphology and a surface area (88.9 m 2 g −1 ) 2.5 times that of the original biochar. The composite exhibited excellent removal of aqueous methylene blue (113.6 mg g −1 ) and methyl violet (107.6 mg g −1 ), which was approximately 6.6 and 2.6 times that of the biochar. Modeling and characterization results suggest that the adsorption of cationic organic pollutants on the composite was controlled by multiple mechanisms including electrostatic attraction, hydrogen bonding, ion exchange, and surface complexation. After five regenerations, the composite maintained methylene blue (87.4 %) and methyl violet (84.8 %) removal ability, thus demonstrating good stability and reusability potential. These findings highlight the advantages and potential of ball-milled dysprosium oxide-loaded-biochar-montmorillonite composite for water treatment and environment remediation.
The development of smart responsive materials is crucial for not only achieving high-performance adsorption of rare earth elements but also enabling green regeneration. Herein, we report the fabrication of ultraviolet (UV)-light responsive imprinted chitosan-based aerogel (UV-IA) and near-infrared (NIR)-light responsive imprinted chitosan-based aerogel (NIR-IA) for the selective adsorption and eco-friendly desorption of Dy(III). Both light-responsive imprinted chitosan-based aerogels were prepared by low-temperature thermally induced phase separation (LT-TIPs), and NIR-IA was prepared by adding the photo-thermal conversion material croconaine. The chitosan aerogels with nanofiber network pore structure were prepared by LT-TIPs. The adsorption capacities of 10 mg of UV-IA and NIR-IA were 76.32 mg g -1 and 76.11 mg g -1 under the condition of pH 5.0 and room temperature, respectively. The selective adsorption effect of UV-IA and NIR-IA on dysprosium ions was obviously better than other competitive ions, and their adsorption separation constants can reach 2408.45 mL g -1 and 2623.29 mL g -1 , respectively. The results showed that cinnamic acid in UV-IA changed to cis structure under UV irradiation, while croconaine in NIR-IA decomposed the chitosan/cinnamic acid conjugate by applying heat to it under NIR irradiation. These changes caused the imprint sizes of UV-IA and NIR-IA to be changed, realizing the green desorption of Dy(III). The best desorption rate of 88.64% was achieved by UV-IA. These materials provide a promising approach for the green and economical separation and recovery of Dy(III) from secondary resources.
Background Radiotherapy is a widely used clinical tool for tumor treatment but can cause systemic toxicity if excessive radiation is administered. Although numerous nanoparticles have been developed as radiosensitizers to reduce the required dose of X-ray irradiation, they often have limitations, such as passive reliance on radiation-induced apoptosis in tumors, and little consider the unique tumor microenvironment that contributes radiotherapy resistance.Methods In this study, we developed and characterized a novel self-assembled nanoparticle containing dysprosium ion and manganese ion (Dy/Mn-P). We systematically investigated the potential of Dy/Mn-P nanoparticles (NPs) as a reactive oxygen species (ROS) amplifier and radiosensitizer to enhance radiation therapy and modulate the tumor microenvironment at the cellular level. Additionally, we evaluated the effect of Dy/Mn-P on the stimulator of interferon genes (STING), an innate immune signaling pathway.Results Physicochemical analysis demonstrated the prepared Dy/Mn-P NPs exhibited excellent dispersibility and stability, and degraded rapidly at lower pH values. Furthermore, Dy/Mn-P was internalized by cells and exhibited selective toxicity towards tumor cells compared to normal cells. Our findings also revealed that Dy/Mn-P NPs improved the tumor microenvironment and significantly increased ROS generation under ionizing radiation, resulting in a ~70% increase in ROS levels compared to radiation therapy alone. This enhanced ROS generation inhibited ~92% of cell clone formation and greatly contributed to cytoplasmic DNA exposure. Subsequently, the activation of the STING pathway was observed, leading to the secretion of pro-inflammatory immune factors and maturation of dendritic cells (DCs).Conclusion Our study demonstrates that Dy/Mn-P NPs can potentiate tumor radiotherapy by improving the tumor microenvironment and increasing endogenous ROS levels within the tumor. Furthermore, Dy/Mn-P can amplify the activation of the STING pathway during radiotherapy, thereby triggering an anti-tumor immune response. This novel approach has the potential to expand the application of radiotherapy in tumor treatment.
Molecular design is crucial for improving the performance of single-molecule magnets (SMMs). For dysprosium(III) SMMs, enhancing ligand-field axiality is a well-suited strategy to achieve high-performance SMMs. We synthesized a series of dysprosium(III) complexes, (NNTIPS)DyBr(THF)2 (1, NNTIPS = fc(NSiiPr3)2; fc = 1,1′-ferrocenediyl, THF = tetrahydrofuran), [(NNTIPS)Dy(THF)3][BPh4] (2), (NNTIPS)DyI(THF)2 (3), and [(NNTBS)Dy(THF)3][BPh4] (4, NNTBS = fc(NSitBuMe2)2), supported by ferrocene diamide ligands. X-ray crystallography shows that the rigid ferrocene backbone enforces a nearly axial ligand field with weakly coordinating equatorial ligands. Dysprosium(III) complexes 1–4 all exhibit slow magnetic relaxation under zero fields and possess high effective barriers (Ueff) around 1000 K, comparable to previously reported (NNTBS)DyI(THF)2 (5). We probed the influences of structural variations on SMM behaviors by theoretical calculations and found that the distribution of negative charges defined by rq, i.e., the ratio of the charges on the axial ligands to the charges on the equatorial ligands, plays a decisive role. Moreover, theoretical calculations on a series of model complexes 1′–5′ without equatorial ligands unveil that the axial crystal-field parameters B20 are directly proportional to the N–Dy–N angles and support the hypothesis that enhancing the ligand-field axiality could improve SMM performance.
Incorporating rare-earth (RE 3+ ) ions into lead-free halide double perovskites represents a promising strategy for modulating their optical properties through energy transfer mechanisms. In this study, Dy 3+ ions were successfully incorporated into Cs 2 NaLuCl 6 :Sb 3+ double perovskites via a facile hydrothermal method. The synthesized crystals not only exhibit intense blue emission originating from self-trapped excitons (STEs) but also display effective Dy 3+ characteristic emissions, thereby broadening the emission spectrum from the visible to the near-infrared region. The energy transfer from STEs to Dy 3+ is confirmed and extends across various RE 3+ ions. Temperature-dependent photoluminescence spectra reveal insights into the excitation and emission processes, as well as thermal quenching mechanism. Additionally, the characteristic emissions of Dy 3+ demonstrate varied anti-thermal quenching behaviors, indicating the remarkable thermal stability of the synthesized crystals. The thermally coupled sub-levels of Dy 3+ ions are employed to develop optical thermometers with notable sensitivity. Finally, the light-emitting diodes fabricated by encapsulating the optimized samples onto commercial chips highlight the great potential of Dy 3+ -doped Cs 2 NaLuCl 6 :Sb 3+ materials for photoelectric applications.
The exploitation of phosphors with tunable color emissions is of great significance in the field of display and lighting. Herein, a series of Eu 3+ /Dy 3+ /Eu 2+ ions single-/multiple-doped NaMgPO 4 phosphors have been successfully synthesized via a high-temperature solid-state reaction method. The luminescence properties of the synthesized NaMgPO 4 phosphors were systematically investigated. The incorporation of Dy 3+ enables the tuning of emission peaks in NaMgPO 4 :Eu 3+ phosphors through an efficient energy transfer (ET) process from Eu 3+ to Dy 3+ , thereby facilitating white light emission in a single-composition phosphor. Eu 3+ and Eu 2+ co-activated NaMgPO 4 phosphors were achieved by controlling the reduction of Eu 3+ to Eu 2+ under a reducing atmosphere generated by activated carbon. Photoluminescence (PL) spectra revealed simultaneous blue emission from Eu 2+ and red emission from Eu 3+ . By varying the amount of activated carbon, tunable emission colors can be realized in the Eu 3+ /Eu 2+ codoped NaMgPO 4 phosphors. Consequently, through the strategic design of rare-earth ion codoping, the Eu 3+ /Dy 3+ /Eu 2+ ions single-/multiple-doped NaMgPO 4 phosphors exhibit promising practical applications in phosphor-converted white light-emitting diodes (LEDs).
Summary Rare-earth doping is an efficient strategy to elevate the oxygen evolution reaction activity of transition-metal-based electrocatalysts, yet it often leads to deleterious electrochemical corrosion. Here, we introduce non-layered dysprosium oxysulfide (Dy 2 O 2 S) to a cobalt catalyst to address this issue. Benefiting from an electron-withdrawing Dy 2 O 2 S shell, the optimum chainmail-structured catalyst displays low overpotentials of 225 ± 1 and 299 ± 5 mV at 0.1 and 1.0 A·cm −2 , respectively, for the oxygen evolution reaction under industrially relevant conditions. Moreover, Dy 2 O 2 S blocks the dissolution of dysprosium and cobalt, endowing the catalyst with almost 100% activity retention for at least 120 h at 1 A·cm −2 . A variety of in situ / ex situ characterization techniques and theoretical calculations unveil the active sites and the interfacial electron redistribution, which facilitate the oxygen intermediate adsorption and oxygen desorption. This work provides a route to utilize rare-earth elements to optimize the performance of electrocatalysts.
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