CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Weiquan Zhan,Yuan Yuan,Qizheng Weng,Yanan Pan,Shaoxian Song,José Luis Arauz-Lara,Feifei Jia,Wencai Zhang
Separation and recovery of trace gadolinium(III) from rare earth elements (REEs) with similar properties is increasingly crucial for renewable energy resources and sustainable development. This study proposed a method to regulate the chemisorption activity of gadolinium(III) using defects-rich molybdenum disulfide (DR-MoS 2 ) electrodes, enabling the separation and recovery of gadolinium(III) from aqueous solutions. Lanthanum(III), gadolinium(III), and yttrium(III), representing light, medium, and heavy REEs respectively, were selected to investigate their adsorption behaviors of on MoS 2 and DR-MoS 2 electrodes at low concentrations. Experiments and simulation results verified distinct adsorption behaviors of REEs on MoS 2 , influenced by their out-shell electron binding capabilities. Interestingly, gadolinium(III) exhibited a unique interaction where its f orbitals strongly interacted with p orbitals of unsaturated sulfur atoms, unlike the other REEs, facilitating effective separation and recovery of gadolinium(III). Furthermore, increased binding affinity enhanced the electric double layer capacity (EDLC) and reduced electrons immigration resistance. Consequently, DR-MoS 2 electrodes achieved 100% recovery of trace gadolinium(III) recovery with high separation efficiency. Hopefully, strongest lanthanum(III) interaction with unsaturated Mo atoms was expected to realize lanthanum(III) separation and recovery. This study presented a promising approach to selectively recover target REEs from similar elements through modulating the chemisorption.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Shengxiang Fu,Zhongyuan Cai,Li Liu,Xiaomin Fu,Changqiang Wu,Liang Du,Chunchao Xia,Su Lui,Qiyong Gong,Bin Song,Hua Ai
Compared to traditional branched polymers with Gd(III) chelates conjugated on their surface, branched polymers with Gd(III) chelates as the internal skeleton are considered to be a reasonable strategy for preparing efficient magnetic resonance imaging contrast agents. Herein, the Gd(III) ligand DOTA was chosen as the internal skeleton; four different molecular weights (3.5, 5.3, 8.6, and 13.1 kDa) and degrees of branching poly-DOTA branched polymers (P1, P2, P3, and P4) were synthesized by a simple “A2 + B4”-type one-pot polymerization. The Gd(III) chelates of these poly-DOTA branched polymers (P1-Gd, P2-Gd, P3-Gd, and P4-Gd) display excellent kinetic stability, which is significantly higher than those of linear Gd-DTPA and cyclic Gd-DOTA-butrol and slightly lower than that of cyclic Gd-DOTA. The T1 relaxivities of P1-Gd, P2-Gd, P3-Gd, and P4-Gd are 29.4, 38.7, 44.0, and 47.9 Gd mM–1 s–1, respectively, at 0.5 T, which are about 6–11 times higher than that of Gd-DOTA (4.4 Gd mM–1 s–1). P4-Gd was selected for in vivo magnetic resonance angiography (MRA) because of its high kinetic stability, T1 relaxivity, and good biosafety. The results showed excellent MRA effect, sensitive detection of vascular stenosis, and prolonged observation window as compared to Gd-DOTA. Overall, Gd(III) chelates of poly-DOTA branched polymers are good candidates of MRI probes, providing a unique design strategy in which Gd chelation can occur at both the interior and surface of the poly-DOTA branched polymers, resulting in excellent relaxivity enhancement. In vivo animal MRA studies of the probe provide possibilities in discovering small vascular pathologies.
研究领域:
医学影像学
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材料科学
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
POLYHEDRON
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2018
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IF 2.067
Fuxian Wan,Lipeng Wang,Wenxin Xu,Changcheng Li,Ying Li,Chunbao Zhang,Lin Jiang
A novel dimeric gadolinium(III) complex, bis(4-Gd-DTPA-aminophenyl)adamantane ( 5 ), was successfully synthesized using bis(4-aminophenyl)adamantane to link two Gd-DTPA units. All the intermediates and bis(4-Gd-DTPA-aminophenyl)adamantane ( 5 ) have been characterized by 1 H NMR, 13 C NMR, ES-API-MS, HR-ESI-MS, FT-IR and elemental analysis (EA). The longitudinal relaxivity of bis(4-Gd-DTPA-aminophenyl)adamantane is 8.43 mM −1 Gd −1 s −1 at 0.43 T (32 °C, pH 7.0), and 4.89 mM −1 Gd −1 s −1 at 3.0 T (32 °C, pH 7.4). The T 1 -weighted imaging in vitro showed that bis(4-Gd-DTPA-acetylaminophenyl)adamantane can enhance the contrast of images distinctly. But most of all, the kinetic inertness of bis(4-Gd-DTPA-aminophenyl)adamantane ( 5 ) was comparable to that of [Gd(DTPA)(H 2 O)] 2− (Magnetvist®). Moreover, cytotoxicity tests indicated that the bis(4-Gd-DTPA-acetylaminophenyl)adamantane exhibited low toxicity to healthy liver cells (L-02 cells). These results demonstrate that the Gd(III) complex 5 may be a promising MRI contrast agent candidate.
研究领域:
医学影像学
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化学
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DOI
高影响因子
DALTON TRANSACTIONS
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2016
·Vol. 45
·期 44
·17616-17623
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IF 4.177
Yue Wang,Renfeng Song,Ke Guo,Qingtao Meng,Run Zhang,Xiangfeng Kong,Zhiqiang Zhang
A novel Gd(III) complex, Gd(TTA)3-DPPZ, was designed and assembled as a dual-modal probe for the simultaneous fluorescence and magnetic resonance imaging (MRI) detection of fluoride ions in aqueous media and in vivo. In this system, the Gd(III) center is not only serving as a MRI signal output unit, but also as a binding site for fluoride ions. When appropriate equivalents of fluoride ions were added into the solution of Gd(TTA)3-DPPZ, the replacement of the coordination water led to a decrease of the longitudinal relaxivity (r1) as well as distinct spectroscopic changes, by which MRI/fluorescence dual-modal fluoride ion sensing was achieved. In the presence of fluoride ions, a 2-fold fluorescence emission enhancement of Gd(TTA)3-DPPZ, and a notable decrease of the UV–vis absorption spectrum were observed. The fluorescence detection limit for fluoride ions was established at 70 nM. Gd(TTA)3-DPPZ also exhibits about 75% decrease of the longitudinal relaxivity (r1) upon addition of fluoride ions in aqueous medium. The appropriate blood circulation time of Gd(TTA)3-DPPZ allows its potential application in MRI in vivo. The results demonstrated that Gd(TTA)3-DPPZ could serve as a potential MRI/fluorescence bimodal imaging agent for the specific and high-sensitive sensing of fluoride ions in vivo.
研究领域:
生物化学
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医学影像学
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分析化学
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DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2018
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IF 3.849
Keyu Cui,Baihui Gao,Meng Tai,Bin Su
Rapid development of rare earth industry has led to an increasing demand for highly purified rare earth elements (REEs). The combination of ion-imprinted technique (IIT) and membrane separation technique (MST) is recently regarded as a promising strategy for selectively separating specific ions from multiple REEs. In this work, a facile bionic strategy for preparation of Gd (III)-imprinted membranes (GIMs) were developed via interlaced stacking of one-dimensional Gd (III)-imprinted carbon nanotubes (GICNTs) and two-dimensional polydopamine-modified graphene oxide (pDA@GO). Polydopamine was synthesized on graphene oxide to large enhance the interfacial adhesion, and ion-imprinting polymerization is implemented on carbon nanotubes (CNTs) by direct cross-link of linear polymers. The obtained materials are characterized in detail by FTIR, SEM, TEM and AFM to explorer the evolution of chemical composition and morphology. Selectivity towards Gd (III) is obtained by isothermal adsorption, kinetic adsorption and time-depended permeation. Isothermal and kinetic models are fitted with adsorption data to obtain the mechanism of selective separation on GIMs. The as-synthesized GIMs with high permeation selectivity (2.91 and 2.49) towards Gd (III) and stable permeation regeneration would potentially be applied to separation and purification of specific ions form multiple REEs.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
JOURNAL OF RARE EARTHS
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2022
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IF 4.632
Wenhao Li,Lijinhong Huang,Bin Xiao,Xiaoguang Duan,Haike Li,Lang Li,Wanfu Huang
With the development of the economy and the increasing demand for environmental protection, the efficient and selective recovery of Gd(III) from actual wastewater is of critical importance. In this work, lanthanum-based metal–organic framework (LaBDC) materials were prepared by a hydrothermal method, and then polyethyleneimine (PEI) and LaBDC were combined by an impregnation method to form a novel LaBDC@ x PEI composite. The prepared materials were characterized using Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), Brunauer–Emmett–Teller (BET), thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS). Experiments show that LaBDC@50%PEI has the highest adsorption capacity (181.77 mg/g) among lanthanum-based MOFs with different PEI loadings at pH = 5.5, which is about 5.1 times that of bare LaBDC. The adsorption isotherm analysis shows that LaBDC@50%PEI follows the Langmuir model. In addition, the adsorption kinetics of LaBDC@50%PEI follows a pseudo-second-order kinetic model, indicating that the adsorption process is chemical adsorption. It is worth noting that LaBDC@50%PEI maintains good adsorption performance and stability after three recycling tests, and exhibits excellent selectivity in cation interference experiments. Overall, the LaBDC@50%PEI composites possess good stability and hold great promises in rapid recovery of Gd(III) from practical aqueous environments.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CARBOHYDRATE POLYMERS
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2016
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IF 4.219
Yan Huang,Peter Osei Boamah,Jianbo Gong,Qi Zhang,Mingqing Hua,Yuzhen Ye
The fusion of molecular and anatomical modalities facilitates more reliable and accurate detection in clinic. In this work, we prepared gadolinium (III) complex Gd-DTPA-FITC-CS 11 with magnetic resonance (MR) and fluorescence dual-modal imaging modalities. Gd-DTPA-FITC-CS 11 consisted of fluorescein isothiocyanate and low-molecular-weight chitosan (CS 11 ) units conjugated with gadolinium diethylenetriamine pentaacetic acid (Gd-DTPA). Gd-DTPA-FITC-CS 11 exhibited a higher longitudinal relaxivity (14.09 mM −1 s −1 ) than the clinical Gd-DTPA (3.85 mM −1 s −1 ). T 1 -weighted MR contrast enhancement was also demonstrated the comparability to Gd-DTPA at lower dosage. The binding with bovine serum albumin (BSA) was investigated. The fluorescence of BSA in the presence of Gd-DTPA-FITC-CS 11 was weakened due to static quenching mechanism. The conformation of BSA was slightly changed but α -helix was dominant. The binding was entropy-driven and spontaneous and the main contribution was hydrophobic interaction. Our results suggested the potential of Gd-DTPA-FITC-CS 11 as an MR/fluorescence dual-modal imaging contrast agent in improving the diagnostic sensitivity and accuracy.
研究领域:
医学影像学
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生物化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2018
·
IF 0
Yibiao Zou,Honglin Jin,Fei Sun,Xiaomeng Dai,Zushun Xu,Shengli Yang,Guangfu Liao
Dual-modality-imaging-guided photothermal therapy (PTT) exhibits great potential in the field of diagnosis and treatment. Herein, we report a controllable method (atom-transfer radical polymerization) for the preparation of gadolinium(III)-complex-grafted lead sulfide (GCGLS) nanoparticles. A series of characterizations (such as TEM, HR-TEM, EDX, XRD, FTIR, etc.) prove that GCGLS nanoparticles have been successfully prepared. The GCGLS nanoparticles with ultrasmall sizes (ca. 11 nm) have quite strong photoabsorption intensity in the near-infrared (NIR) region because of a low S vacancy concentration of lead sulfide. As the addition amount of gadolinium(III) complexes increases, the sizes of the GCGLS nanoparticles show no evidence of changing. The temperature of the GCGLS nanoparticle solution can quickly elevate to 57.5 °C in 10 min after NIR laser irradiation (1.5 W cm–2) at 808 nm; this result reveals that it possesses high photothermal conversion efficiency (∼31%). When the GCGLS nanoparticles are injected into the mice, it is clearly observed that there is efficient accumulation in the tumor site. Moreover, the GCGLS nanoparticles also show excellent prominent X-ray computer tomography (CT) and T1-weighted magnetic resonance (T1-MR) imaging in vitro/vivo. By the combination of GCGLS and NIR laser irradiation, an effective tumor treatment experiment is conducted in mice. Therefore, the prepared GCGLS nanoparticles with dual-modality-imaging-guided PTT can be used as potential diagnosis and treatment reagents for clinical applications.
研究领域:
生物医学工程
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材料科学
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肿瘤学
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产品关联
DOI
BIOMATERIALS
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2021
·
IF 12.479
Ruijing Zhang,Qin Zeng,Xipeng Li,Da Xing,Tao Zhang
Current light-mediated photodynamic therapy (PDT) is far underutilized in clinical cancer treatment due to its low pharmacological effect . We herein proposed a new gadolinium(III)-phthalocyanine (GdPc)-enabled phototherapeutics, photoacoustic/dynamic therapy (PADT), towards in vivo solid tumors via parallel-produced photocavitation and photodynamic oxidation with excitation by a single pulsed laser . We demonstrated that pulsed irradiation of GdPc could simultaneously produce an intense acoustic effect and a high-level 1 O 2 quantum yield to afford mitochondrial damage and initiate programmed cell death. Under the guidance of magnetic resonance/photoacoustic dual-modal imaging, the mechanical oxygen-independent destruction of acoustic cavitation and the chemical damage of 1 O 2 were validated to afford combinatorial inhibition of tumors under either normal or hypoxic conditions after the agent delivered into the cancer cells by a pH-sensitive nanomicelle. The single-laser initiated PADT using GdPc as a versatile photoagent maximizes the use of light energy to minimize the dose requirement of oxygen and agent towards high therapeutic efficacy, surpassing dramatically over conventional PDT.
研究领域:
诊疗学
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医学成像
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光动力治疗
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肿瘤学
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纳米医学
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产品关联
DOI
PubMed
高影响因子
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