Highly hydrated paramagnetic amorphous calcium carbonate nanoclusters as an MRI contrast agent

Dong, Liang; Xu, Yongfen; Sui, Cong; Zhao, Yang; Mao, Li‐Bo; Gebauer, Denis; Rosenberg, Rose; Avaro, Jonathan; Wu, Yadong; Gao, Huai‐Ling; Pan, Zhao; Wen, Hui-Qin; Yan, Xu; Li, Fēi; Lu, Yang; Cölfen, Helmut; Yu, Shu‐Hong

doi:10.1038/s41467-022-32615-3

Cited by 31 publications

(37 citation statements)

References 58 publications

(77 reference statements)

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“…Gd-doped amorphous CC NPs have been successfully applied for in vivo studies of NP biodistribution and contrast-enhanced MR angiography. 22,23 In this study, we demonstrate these contrast agents' application in targeted atherosclerosis imaging. First, we synthesized amorphous calcium carbonate NPs with enhanced MRI contrast using a fast and cost-efficient method.…”

Section: Introductionmentioning

confidence: 69%

“…First, we prepared Gd-doped CC NPs by mixing CaCl 2 , GdCl 3 •6H 2 O, PAA and Na 2 CO 3 at room temperature for 1 min and then stopping the particle growth with the addition of ethanol to the reaction solution, as reported previously. 23 We separated the unreacted species from the nanoparticles by precipitation and filtration (3 kDa molecular weight cutoff) and freeze-dried the CC NPs for further use, obtaining 2.2 g of nanoparticles with a 3 wt % of Gd. The size of these NPs was 2−3 nm, as shown in atomic force microscopy (AFM), transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM) images in Figure 1a S8), which is the main component of the calcifications found in the atherosclerotic plaque.…”

Section: Resultsmentioning

confidence: 99%

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A Comparative Study of Ultrasmall Calcium Carbonate Nanoparticles for Targeting and Imaging Atherosclerotic Plaque

et al. 2023

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Atherosclerosis is a complex disease that can lead to life-threatening events, such as myocardial infarction and ischemic stroke. Despite the severity of this disease, diagnosing plaque vulnerability remains challenging due to the lack of effective diagnostic tools. Conventional diagnostic protocols lack specificity and fail to predict the type of atherosclerotic lesion and the risk of plaque rupture. To address this issue, technologies are emerging, such as noninvasive medical imaging of atherosclerotic plaque with customized nanotechnological solutions. Modulating the biological interactions and contrast of nanoparticles in various imaging techniques, including magnetic resonance imaging, is possible through the careful design of their physicochemical properties. However, few examples of comparative studies between nanoparticles targeting different hallmarks of atherosclerosis exist to provide information about the plaque development stage. Our work demonstrates that Gd (III)-doped amorphous calcium carbonate nanoparticles are an effective tool for these comparative studies due to their high magnetic resonance contrast and physicochemical properties. In an animal model of atherosclerosis, we compare the imaging performance of three types of nanoparticles: bare amorphous calcium carbonate and those functionalized with the ligands alendronate (for microcalcification targeting) and trimannose (for inflammation targeting). Our study provides useful insights into ligand-mediated targeted imaging of atherosclerosis through a combination of in vivo imaging, ex vivo tissue analysis, and in vitro targeting experiments.

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Section: Introductionmentioning

confidence: 69%

Section: Resultsmentioning

confidence: 99%

A Comparative Study of Ultrasmall Calcium Carbonate Nanoparticles for Targeting and Imaging Atherosclerotic Plaque

et al. 2023

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“…As a typical example, amorphous calcium carbonate conjugated with gadolinium ions was recently reported to exhibit superior imaging performance as a magnetic resonance imaging contrast agent. [ 38 ] However, the exploration of amorphous nanomaterials for biomedical applications is still very limited so far. For example, how the crystallinity (crystalline or amorphous phase) will affect the performance of nanomaterials for cancer therapy, such as SDT, still remain unexplored.…”

Section: Introductionmentioning

confidence: 99%

Boosting the Sonodynamic Cancer Therapy Performance of 2D Layered Double Hydroxide Nanosheet‐Based Sonosensitizers Via Crystalline‐to‐Amorphous Phase Transformation

Shen

Meng

et al. 2023

Advanced Materials

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“…In another aspect, due to the fluctuation of endogenous paramagnetic species as well as the concentration gradient of CAs, false‐positive signals were frequently encountered. [ 14 ] As we know, T 1 / T 2 dual‐mode MRI CAs have attracted great research interest, with T 1 ‐weighted MRI being used to assess adipose tissues or anatomical structures, while T 2 ‐weighted MRI for assessing water‐rich structures or local inflammation. [ 15 ] Thus, self‐confirmative CAs especially with T 1 / T 2 dual‐modal MRI were able to provide an accurate diagnosis.…”

Section: Introductionmentioning

confidence: 99%

Single‐Atom Gd Nanoprobes for Self‐Confirmative MRI with Robust Stability

Luo

Liu

et al. 2023

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which could exacerbate nephrogenic systemic fibrosis, and deposit in the heart, kidney, skin and even in the brain, threatening the patient's health. [5] To overcome these shortcomings, Gdbased inorganic nanoparticles (NPs), such as Gd 2 O 3 , [6] NaGdF 4 , [7] Gd-doped oxide, [8] were reported on account of the higher stability of Gd 3+ ions in Gd NPs-based CAs. The unsaturated coordination properties of Gd 3+ exposed at the NPs surface can be used to increase the hydration sites, which contribute to the high T 1 relaxivity for MRI. [9] While metal ions inside NPs were not available for direct chemical exchange with protons and thus attenuated the MRI signal. Therefore, increasing the number of accessible paramagnetic metal centers would directly increase the relaxivity. Recently, single-atom materials (SAMs) have been reported and extensively utilized in catalysis, pollution treatment, biosensing, and tumor therapy. [10] However, few studies have focused on the construction of SAMs as MRI contrast agents. [11] We anticipated that SAMs such as single-atom Gd nanomaterial could provide as a good substitute for traditional Gd complex by simulating the coordination environment of paramagnetic metal with ligands at the atomic level, maximizing the exposure of Gd atom as well as possessing better structural stability, which was conducive to enhance imaging contrast. In addition, according to Solomon-Bloembergen-Morgan theory, [12] the enhanced relaxivity was mainly related to increasing the number of coordination water in the inner layer (q), shortening water exchange lifetime (τ M ), prolonging molecular rotation time (τ R ) and facilitating diffusion related time of water molecules (τ D ). [13] Therefore, the fabrication of Gd SAMs with open coordination sites, large surface area, and hydrophilic properties are highly desirable. In another aspect, due to the fluctuation of endogenous paramagnetic species as well as the concentration gradient of CAs, false-positive signals were frequently encountered. [14] As we know, T 1 /T 2 dual-mode MRI CAs have attracted great research interest, with T 1 -weighted MRI being used to assess adipose tissues or anatomical structures, while T 2 -weighted MRI for assessing waterrich structures or local inflammation. [15] Thus, self-confirmative CAs especially with T 1 /T 2 dual-modal MRI were able to provide an accurate diagnosis. [16] Herein, we constructed a highly stable single atom Gd-based MRI CA through spatial confinement and controllable etching strategy for effective T 1 /T 2 dual-mode MRI with excellent Gadolinium (Gd)-based complexes are extensively utilized as contrast agents (CAs) in magnetic resonance imaging (MRI), yet, suffer from potential safety concerns and poor tumor targeting. Herein, as a mimic of Gd complex, single-atom Gd nanoprobes with r 1 and r 2 values of 34.2 and 80.1 mM −1 s −1 (far higher than that of commercial Gd CAs) at 3 T are constructed, which possessed T 1 /T 2 dual-mode MRI with excellent stability and good tumor targeting ability. Specificall...

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Highly hydrated paramagnetic amorphous calcium carbonate nanoclusters as an MRI contrast agent

Cited by 31 publications

References 58 publications

A Comparative Study of Ultrasmall Calcium Carbonate Nanoparticles for Targeting and Imaging Atherosclerotic Plaque

A Comparative Study of Ultrasmall Calcium Carbonate Nanoparticles for Targeting and Imaging Atherosclerotic Plaque

Boosting the Sonodynamic Cancer Therapy Performance of 2D Layered Double Hydroxide Nanosheet‐Based Sonosensitizers Via Crystalline‐to‐Amorphous Phase Transformation

Single‐Atom Gd Nanoprobes for Self‐Confirmative MRI with Robust Stability

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