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RSC Advances · 2018 ·Vol. 8 ·期 18 ·9611-9617 · IF 2.936

Revealing the in situ NaF generation balance for user-friendly controlled synthesis of sub-10 nm monodisperse low-level Gd3+-doped β-NaYbF4:Er

Ji-Wei Shen,Zhiqing Wang,Xiaoxuan Wei,Jiawei Liu,Yinmao Wei

Herein, user-friendly control of the synthesis of sub-10 nm hexagonal (β-) NaYbF4:Er nanocrystals (NCs) with extremely low-level Gd3+ doping (0%, 10 mol%) was achieved. We reveal for the first time that the effective sodium/fluoride levels during the formation of cubic (α-) nuclei are not only controlled by the sodium/fluoride to rare-earth precursor ratios used, but also sensitively restricted by the in situ NaF generation reaction in a sodium oleate-based solvothermal system. Excessive in situ NaF generation will lead to a respective sodium- and fluoride-deficient environment, delayed α-to-β transition and larger β-NCs. Based on these effects, sub-10 nm monodisperse low-level Gd3+-doped β-NaYbF4:Er was obtained with a user-friendly low fluoride dosage by finely balancing this NaF generation reaction and achieving an intrinsic optimized sodium-fluoride level for NC nucleation. Notably, our work represents the first example where the focus is on the competing in situ NaF generation reaction and its use for nucleation regulation, as well as for the user-friendly control of the solvothermal synthesis of sub-10 nm β-NaYbF4:Er.

研究领域: 材料科学 · 纳米技术
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JOURNAL OF LUMINESCENCE · 2026 · IF 3.8

Boosting near-infrared quantum cutting of Ce3+/Yb3+ via Gd3+ -induced site-selective occupation in Y2SiO5 phosphors: Enhanced downconversion for silicon solar cells and NIR-LEDs

Viswadevarayalu Annavaram,Weicheng Xiang,Zihang Chai,Kangwei Zhu,Zaifa Pan

Enhanced quantum-cutting (QC) materials are highly desirable for promising applications such as solar cells. In this work, a series of Ce 3+ , Gd 3+ , and Yb 3+ tri-doped phosphors using Y 2 SiO 5 as the host were synthesized via a solid-state reaction. X-ray diffraction confirms that the dopants do not alter the monoclinic phase of Y 2 SiO 5 . Photoluminescence spectroscopy reveals that, the optimized tri-doped phosphor exhibits intense near-infrared (NIR) emission centered at 976 nm under UV excitation. Mechanism investigation reveals that Gd 3+ preferentially occupies the 7-coordinate Y2 site (associated with the Ce 3+ 392-nm emission), displacing Ce 3+ ions toward the 6-coordinate Y1 site (associated with the 425-nm emission). The Y1-site Ce 3+ emission at ∼425 nm (≈23,500 cm −1 ) is energetically closer to twice the Yb 3+ absorption energy (≈20,000 cm −1 ) than the Y2-site emission at ∼392 nm (≈25,500 cm −1 ), making the Y1 site more favorable for cooperative energy transfer to Yb 3+ pairs. This site-selective occupation effect significantly enhances the quantum-cutting efficiency. Furthermore, the synthesized tri-doped phosphor demonstrates superior performance in NIR phosphor-converted LEDs (pc-LEDs), achieving an electrical-to-optical conversion efficiency 1.55 times that of the co-doped counterpart. The output power of the tri-doped NIR LED is enhanced to 206.4% of that of the co-doped device. For solar cell applications, the short-circuit current density (J SC ) of the tri-doped device reaches 2.47 mA/cm 2 , with a power conversion efficiency (η) of 10.58%. The tri-doped phosphor solar cell exhibits an extra 0.1% enhancement in conversion efficiency compared to the co-doped counterpart. These results highlight the potential of Y 2 SiO 5 :Ce 3+ ,Gd 3+ ,Yb 3+ as an efficient spectral converter for boosting the energy yield of silicon photovoltaics.

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ANALYTICA CHIMICA ACTA · 2020 · IF 5.977

Mono-dispersed nano-hydroxyapatite based MRI probe with tetrahedral DNA nanostructures modification for in vitro tumor cell imaging

Yaqin He,Caizhi Lv,Xiandeng Hou,Lan Wu

Taking advantage of the superior biocompatibility, good stability in a wide pH and temperature range, as well as its strong affinity with DNA of hydroxyapatite (HAp), tetrahedral DNA nanostructures (TDNs) conjugated with AS1411 aptamer ( anti -nucleolin overexpressed on tumor cell membranes) were employed as affinity ligands to construct a novel mono-dispersed HAp based probe with Gd 3+ doping (Apt-TDNs-GdHAp) for MR imaging. The adsorption of TDNs on the nano-HAp surface facilely accomplished the construction of the Apt-TDNs-GdHAp probes. Meanwhile, the use of hydrophilic TDNs not only favored the phase-transfer from the oil phase to the aqueous phase, but also enhanced the mono-dispersion of this probe due to the well-ordered distribution of TDNs on the surface of nano-HAp. Moreover, Apt-TDNs-GdHAp probe with a better mono-dispersion and crystalinity achieved twice higher longitudinal relaxivity (r 1 value) than that of GdHAp synthesized by microwave-assisted method (Microwave-GdHAp), exhibiting much more excellent T 1 -weighted imaging performance. With the introduction of TDNs, the stability and the tumor-targeting accessibility were also greatly improved, showing its great potential for further bio-applications.

研究领域: 纳米技术 · 生物医学工程 · 分子生物学 · 材料科学 · 医学成像
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CHEMISTRY OF MATERIALS · 2021 · IF 9.811

Degradable Carrier-Free Metal–Phenolic Network Theranostic Agent with Targeted Mitochondrial Damage for Efficient Cancer Theranostics

Yu Wen,Junjiao Hu,Jun Liu,Ming Li

Mitochondria-targeted cancer therapy holds great promise for anticancer treatments. It is thus of great significance to explore effective strategies for targeted mitochondrial damage in cancer cells. Herein, a degradable carrier-free curcumin-based metal–phenolic network (MPN) theranostic agent, namely, the indocyanine green-loaded curcumin–Gd nanoparticle (ICG@cur-Gd NP), is reported for magnetic resonance (MR)/fluorescence dual-modal imaging-guided chemo-/photodynamic combination cancer therapy. The ICG@cur-Gd NPs are fabricated by coordination-driven self-assembly of curcumin and Gd3+, followed by ICG loading. This theranostic agent intrinsically enables the MR and fluorescence imaging for real-time tumor visualization and precise guidance during anticancer treatments. Tumor-acidity-responsive degradation of ICG@cur-Gd NPs induces tumor-specific release of curcumin, ICG, and Gd3+ with no long-term systemic toxicity. The results reveal that the curcumin component of ICG@cur-Gd NPs can induce efficient mitochondrial damage. The excellent anticancer efficacy of ICG@cur-Gd NPs with laser exposure is confirmed in vivo, highlighting its potential for clinical use. This study constitutes the first report of a curcumin-based MPN theranostic agent combined with the clinically approved and used MR imaging contrast agent Gd3+. This work provides a novel and efficient strategy to construct carrier-free theranostic agents for imaging-guided cancer theranostics.

CAS / MDL: 67-68-5
研究领域: 癌症研究 · 材料科学 · 纳米医学 · 诊疗学 · 生物医学工程
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JOURNAL OF MATERIALS CHEMISTRY · 2011 ·Vol. 22 ·期 6 ·2632-2640 · IF 5.101

Lanthanide dopant-induced formation of uniform sub-10 nm active-core/active-shell nanocrystals with near-infrared to near-infrared dual-modal luminescence

Daqin Chen,Yunlong Yu,Feng Huang,Hang Lin,Ping Huang,Anping Yang,Zhaoxing Wang,Yuansheng Wang

We present a novel strategy involving the lanthanide dopant-induced formation of ultrasmall (sub-10 nm) uniform Ln3+:BaF2/Ln3+:SrF2 active-core/active-shell architectures. The lanthanide ions doped in the shell are demonstrated to play a key role to retard the growth of the core/shell nanocrystals. Particularly, adopting ∼3 nm Tm3+,Yb3+:BaF2 nanocrystals as cores prepared by a solvothermal reaction, growth of Gd3+,Nd3+:SrF2 shells is successfully induced on the surfaces of these cores through a thermal decomposition process, forming ∼7 nm highly uniform and monodisperse Tm3+,Yb3+:BaF2/Gd3+,Nd3+:SrF2 active-core/active-shell nanocubes. In this architecture, the Gd3+,Nd3+:SrF2 shell not only benefits the enhancement of the near-infrared to near-infrared upconversion luminescence of the Tm3+,Yb3+:BaF2 core, but also acts as the host to realize the near-infrared to near-infrared downconversion luminescence of Nd3+ dopants and the paramagnetism of Gd3+ ones. Importantly, the doping of Tm3+/Yb3+ and Nd3+ into the core and shell respectively effectively suppresses the adverse energy transfer from Tm3+ to Nd3+ as well as from Nd3+ to Yb3+, resulting in lessening of the quenching for both Tm3+ upconversion and Nd3+,Yb3+ downconversion emissions. These hydrophobic core/shell nanocrystals are further converted into hydrophilic ones using thioglycolic acid as the surface ligand. The sub-10 nm water-soluble active-core/active-shell architectures with near-infrared to near-infrared dual-modal luminescence and proper paramagnetism may find potential applications in biomedical imaging and detection.

研究领域: 材料科学 · 纳米技术 · 生物医学工程 · 光学
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Advanced Healthcare Materials · 2024 · IF 10

A Closed-Loop Cascade Strategy for On-Demand Regulation of Uric Acid

Chenyao Nie,Ji Xu,Yuhui Zhao,Ke Nan,Manqi Tan,Zhaobo Liu,Ming Huang,Wenzhi Ren,Bing Wang

Despite that the current anti-hyperuricemia drugs can effectively reduce uric acid (UA) levels, imprecise medication dosage or uncontrolled lowering of UA levels may result in undesired effects. To address this issue, a closed-loop cascade strategy based on a biocompatible network composite, NW-FPNP/uricase (UOX), is proposed for on-demand regulation of UA levels. NW-FPNP/UOX is constructed by encapsulation of UOX) as UA-responsive element and FPNP, a nanoparticle of phenylboronic acid modified xanthine oxidase (XOD) inhibitor febuxostat, as H 2 O 2 -sensitive element with AMP/Gd 3+ network. It interrelates the UA metabolization and generation processes into a closed loop of cascade reactions involving UOX-catalyzed UA metabolization and H 2 O 2 generation, H 2 O 2 -triggered febuxostat regeneration and XOD inhibition, and XOD-catalyzed UA generation. Through UA level-dependent auto-adjustment of XOD activity, specially 6% at 600 × 10 −6 m UA compared to 82% at 100 × 10 −6 m , UA levels can be regulated to an appropriate range through dynamically balancing UA metabolization and generation. This biocompatible on-demand UA regulation system prevents the overdose of UA-lowering medications and avoids hypouricemia in hyperuricemia treatment, demonstrating great potential in intelligent UA level management. This work also introduces a new concept of a closed-loop cascade strategy for on-demand regulation of biochemical indicators within specific thresholds.

研究领域: 生物医学工程 · 药学 · 纳米技术 · 生物化学
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2023 · IF 5.8

Cu-In-S/ZnS:Gd3+ quantum dots with isolated fluorescent and paramagnetic modules for dual-modality imaging in vivo

Yong-Qiang Xu,Liu-Yuan Zang,Hai-Yu Gao,Jin Peng,Dong-Yun Zheng,Chao Liu,Xiao-Jun Liu,Dong-Bing Cheng,Chun-Nan Zhu

Gd 3+ -doped quantum dots (QDs) have been widely used as small-sized bifunctional contrast agents for fluorescence/magnetic resonance (FL/MR) dual-modality imaging. However, Gd 3+ doping will always compromise the FL of host QDs. Therefore, balancing the Gd 3+ doping and the optical properties of QDs is crucial for constructing high-performance bifunctional nanoprobes . Additionally, most paramagnetic QDs are synthesized in the organic phase and need to be transferred to the aqueous phase for bioimaging. Herein, ingeniously designed shell-doped Cu-In-S/ZnS:Gd 3+ QDs have been prepared in the aqueous phase. It has been demonstrated that isolating paramagnetic Gd 3+ from fluorescent Cu-In-S core via doping Gd 3+ into ZnS shell not only avoided the decrease of FL quantum yield (QY), but also ensured the water accessibility of paramagnetic Gd 3+ ions, by which the FL QY and r 1 relaxivity of Cu-In-S/ZnS:Gd 3+ QDs achieved as much as 15.6% and 15.33 mM -1 ·s -1 , respectively. These high-performance QDs with excellent stability, low biotoxicity, and good tumor permeability were successfully applied for in vivo tumor FL/MR dual-modality imaging, and have shown significant potential in the precision detection and diagnosis of diseases.

研究领域: 纳米技术 · 生物医学工程 · 材料科学 · 医学成像
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