Publications by authors named "Mingyuan Gao"

125 Publications

Cu-Doped Alloy Layer Guiding Uniform Li Deposition on a Li-LLZO Interface under High Current Density.

ACS Appl Mater Interfaces 2021 Sep 24;13(35):42212-42219. Epub 2021 Aug 24.

Key Laboratory of Advanced Civil Engineering Materials of Ministry of Education, Functional Materials Research Laboratory, School of Materials Science & Engineering, Tongji University, 4800 Caoan Road, Shanghai 201804, P. R. China.

LiLaZrO(LLZO)-based ceramics as promising solid-state electrolytes (SSEs) have received much attention for use in high-energy lithium (Li) metal batteries. However, the Li growth through the solid garnet electrolyte under a low current density hinders its practical application. In this work, the Cu doped LiZn was designed to guide uniform Li deposition by magnetron cosputtering and an in situ alloying reaction on LiLaZrTaO (LLZTO) pellets. After introducing the composite layer, a small interfacial area specific resistance (∼30 Ω·cm) can be obtained. Improved lithium plating/stripping performance, including a long-life span of 450 h (under a current density of 0.8 mA cm without short circuit) and a high critical current density (CCD) of 2.8 mA cm is performed by the composite interlayer with a Zn:Cu ratio of 10:1. And the Li/Cu-LiZn SSEs/LFP full cell exhibits good electrochemical performance. Accordingly, the Li deposited behavior in the Li plating/stripping process at the intermediate layer is discussed in detail. This work provides a new sight for the alloy interface designed on the solid-state garnet SSEs for high performance lithium metal batteries under high current density.
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http://dx.doi.org/10.1021/acsami.1c11607DOI Listing
September 2021

Quantitatively visualizing the activity of MMP-2 enzyme in vivo using a ratiometric photoacoustic probe.

Methods Enzymol 2021 12;657:59-87. Epub 2021 Jul 12.

State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou, PR China. Electronic address:

In this chapter, we describe the recent progress in development of small-molecule probes for quantitatively imaging of matrix metalloproteinase-2 (MMP-2) activity in living mice. We provide the detailed protocols for synthesis, characterization, and validation of a new multimodal probe QC with the near-infrared (NIR), single-photon emission computed tomography (SPECT), and photoacoustic (PA) imaging capabilities for accurate and quantitative detection of MMP-2 in vivo. We believe that this probe developed in our research group would offer a useful tool for precise evaluation of tumor metastasis as well as therapeutic efficacy.
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http://dx.doi.org/10.1016/bs.mie.2021.06.035DOI Listing
August 2021

Ultrasmall superparamagnetic iron oxide nanoparticles: A next generation contrast agent for magnetic resonance imaging.

Wiley Interdiscip Rev Nanomed Nanobiotechnol 2021 Jul 23:e1740. Epub 2021 Jul 23.

Center for Molecular Imaging and Nuclear Medicine, State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University, Collaborative Innovation Center of Radiological Medicine of Jiangsu Higher Education Institutions, Suzhou, China.

As a research hotspot, the development of magnetic resonance imaging (MRI) contrast agents has attracted great attention over the past decades for improving the accuracy of diagnosis. Ultrasmall superparamagnetic iron oxide (USPIO) nanoparticles with core diameter smaller than 5.0 nm are expected to become a next generation of contrast agents owing to their excellent MRI performance, long blood circulation time upon proper surface modification, renal clearance capacity, and remarkable biosafety profile. On top of these merits, USPIO nanoparticles are used for developing not only T contrast agents, but also T /T switchable contrast agents via assembly/disassembly approaches. In recent years, as a new type of contrast agents, USPIO nanoparticles have shown considerable applications in the diagnosis of various diseases such as vascular pathological changes and inflammations apart from malignant tumors. In this review, we are focusing on the state-of-the-art developments and the latest applications of USPIO nanoparticles as MRI contrast agents to discuss their advantages and future prospects. This article is categorized under: Diagnostic Tools > In Vivo Nanodiagnostics and Imaging.
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http://dx.doi.org/10.1002/wnan.1740DOI Listing
July 2021

Furin Enzyme and pH Synergistically Triggered Aggregation of Gold Nanoparticles for Activated Photoacoustic Imaging and Photothermal Therapy of Tumors.

Anal Chem 2021 07 23;93(26):9277-9285. Epub 2021 Jun 23.

State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Centre of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, 199 Renai Road, Suzhou 215123, China.

Specific and effective accumulation of nanoparticles within tumors is highly crucial for precise cancer diagnosis and treatment. Therefore, spatiotemporally manipulating the aggregation of small gold nanoparticles (AuNPs) in a tumor microenvironment is of great significance for enhancing the diagnostic and therapeutic efficacy of tumors. Herein, we reported a novel furin enzyme/acidic pH synergistically triggered small AuNP aggregation strategy for activating the photoacoustic (PA) imaging and photothermal (PTT) functions of AuNPs in vivo. Smart gold nanoparticles decorated with furin-cleavable RVRR (Arg-Val-Arg-Arg) peptides (Au-RRVR) were rationally designed and fabricated. Both in vitro and in vivo experiments demonstrated that such Au-RRVR nanoparticles could be simultaneously induced by furin and acidic pH to form large aggregates within tumorous tissue resulting in improved tumor accumulation and retention, which can further activate the PA and PTT effect of AuNPs for sensitive imaging and efficient therapy of tumors. Thus, we believe that this dual-stimuli-responsive aggregation system may offer a universal platform for effective cancer diagnosis and treatment.
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http://dx.doi.org/10.1021/acs.analchem.1c01713DOI Listing
July 2021

Turning-on persistent luminescence out of chromium-doped zinc aluminate nanoparticles by instilling antisite defects under mild conditions.

Nanoscale 2021 May 27;13(18):8514-8523. Epub 2021 Apr 27.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China.

Spinel oxide nanocrystals are appealing hosts for Cr for forming persistent luminescent nanomaterials due to their suitable fundamental bandgaps. Benefiting from their antisite defect-tolerant nature, zinc gallate doped with Cr ions has become the most studied near-infrared (NIR) persistent luminescent material. However, it remains challenging to achieve persistent luminescence from its inexpensive analogs, e.g., zinc aluminate (ZnAlO). Because the radius difference of the cations in the latter system is bigger, it is intrinsically unfavorable for ZnAlO to form Zn-Al antisite defects under mild conditions. Herein, we report a wet-chemical synthetic route for preparing Cr-doped ZnAlO nanoparticles with long NIR persistent luminescence. It was demonstrated that methanol (MeOH) as an important component of the mixed solvent played a critical role in tailoring the morphology of the resulting ZnAlO:Cr nanocrystals. It could particularly drive the formation of antisite defects in the resulting coral-like nanoparticles bearing zinc-rich cores and zinc gradient peripheries. To disclose the effects of MeOH on the formation of antisite defects as well as particle morphologies, small molecules released during the pyrolysis of metal acetylacetonate precursors were analyzed by using gas chromatography-mass spectrometry. In combination with density functional theory (DFT) calculations, it was found that MeOH can effectively catalyze the thermolysis of metal acetylacetonate precursors, in particular Zn(acac). Therefore, MeOH exhibits remarkable effects on the formation of antisite defects by balancing the decomposition rates of Zn(acac) and Al(acac) through its volume fraction in the reaction system. This work thus constitutes a hitherto less common strategy for achieving NIR persistent luminescence from Cr-doped ZnAlO nanoparticles by engineering the cation defects under mild conditions.
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http://dx.doi.org/10.1039/d0nr08267hDOI Listing
May 2021

A Cyclodextrin-Hosted Ir(III) Complex for Ratiometric Mapping of Tumor Hypoxia In Vivo.

Adv Sci (Weinh) 2021 04 5;8(8):2004044. Epub 2021 Feb 5.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China.

Hypoxia is considered as a key microenvironmental feature of solid tumors. Luminescent transition metal complexes particularly those based on iridium and ruthenium have shown remarkable potentials for constructing sensitive oxygen-sensing probes due to their unique oxygen quenching pathway. However, the low aqueous solubility of these complexes largely retards their sensing applications in biological media. Moreover, it remains difficult so far to use the existing complexes typically possessing only one luminescent domain to quantitatively detect the intratumoral hypoxia degree. Herein, an Ir(III) complex showing red emissions is designed and synthesized, and innovatively encapsulated within a hydrophobic pocket of Cyanine7-modified cyclodextrin. The Ir(III) complex enables the oxygen detection, while the cyclodextrin is used not only for improving the water solubility and suppressing the luminescence quenching effect of the surrounding aqueous media, but also for carrying Cyanine7 to establish a ratiometric oxygen fluorescence probe. 2D nuclear magnetic resonance is carried out to confirm the host-guest structure. The oxygen-responsive ability of the resulting ratiometric probe is evaluated through in vitro cell and multicellular experiments. Further animal studies about tumor oxygen level mapping demonstrate that the probe can be successfully used for quantitatively visualizing tumor hypoxia in vivo.
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http://dx.doi.org/10.1002/advs.202004044DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8061356PMC
April 2021

Sequential SPECT and NIR-II imaging of tumor and sentinel lymph node metastasis for diagnosis and image-guided surgery.

Biomater Sci 2021 Apr 5;9(8):3069-3075. Epub 2021 Mar 5.

State Key Laboratory of Radiation Medicine and Protection, School of Radiation Medicine and Protection & School for Radiological and Interdisciplinary Sciences (RAD-X), Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, PR China.

Efficacious cancer treatment largely relies on accurate imaging diagnosis and imaging-guided surgery, which can be achieved by combining different mode imaging probes on one single nanoplatform. Herein, a novel radiolabeled NIR-II nanoprobe (I-MT NP) was developed to enable versatile single-photon emission computed tomography (SPECT) and second near-infrared (NIR-II) fluorescence dual-modal imaging against breast cancer. I-MT was precipitated with an amphiphilic triblock copolymer (PEO-PPO-PEO) to form I-MT NPs. The I-MT NPs exhibited high labeling efficiency (98 ± 2%) with a hydrodynamic diameter of 91.3 ± 5.5 nm. In vitro and in vivo studies demonstrated that I-MT NPs emitted intensive NIR-II fluorescence and SPECT signals, and possessed good biocompatibility. By using a breast tumor xenograft mouse model after intravenous injection of I-MT NPs, the SPECT imaging and NIR-II imaging showed clear images of tumor tissues at 8 h and 48 h postinjection, respectively, suggesting the feasibility of using I-MT NPs to detect tumors before surgery and visualize the dissection area during surgery. In addition, the SPECT scan of a lymph node mapping was performed at 1 h postinjection and NIR-II fluorescence imaging was carried out at 4 h postinjection. This further guarantees the accurate imaging of lymph nodes before and during surgery for lymphadenectomy. Overall I-MT NP is a promising, practical imaging probe for sequential imaging and precision cancer therapy.
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http://dx.doi.org/10.1039/d1bm00088hDOI Listing
April 2021

X-ray-Based Techniques to Study the Nano-Bio Interface.

ACS Nano 2021 03 2;15(3):3754-3807. Epub 2021 Mar 2.

Mathematics, Informatics, and Natural Sciences (MIN) Faculty, University of Hamburg, 20354 Hamburg, Germany.

X-ray-based analytics are routinely applied in many fields, including physics, chemistry, materials science, and engineering. The full potential of such techniques in the life sciences and medicine, however, has not yet been fully exploited. We highlight current and upcoming advances in this direction. We describe different X-ray-based methodologies (including those performed at synchrotron light sources and X-ray free-electron lasers) and their potentials for application to investigate the nano-bio interface. The discussion is predominantly guided by asking how such methods could better help to understand and to improve nanoparticle-based drug delivery, though the concepts also apply to nano-bio interactions in general. We discuss current limitations and how they might be overcome, particularly for future use .
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http://dx.doi.org/10.1021/acsnano.0c09563DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7992135PMC
March 2021

Two-Dimensional and Subnanometer-Thin Quasi-Copper-Sulfide Semiconductor Formed upon Copper-Copper Bonding.

ACS Nano 2021 Jan 6;15(1):873-883. Epub 2021 Jan 6.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China.

Ultrathin two-dimensional (2D) semiconductors exhibit outstanding properties, but it remains challenging to obtain monolayer-structured inorganic semiconductors naturally occurring as nonlayered crystals. Copper sulfides are a class of widely studied nonlayered metal chalcogenide semiconductors. Although 2D copper sulfides can provide extraordinary physical and chemical applications, investigations of 2D copper sulfides in the extreme quantum limit are constrained by the difficulty in preparing monolayered copper sulfides. Here, we report a subnanometer-thin quasi-copper-sulfide (q-CS) semiconductor formed upon self-assembly of copper(I)-dodecanethiol complexes. Extended X-ray absorption fine structure analysis revealed that the existence of Cu-Cu bonding endowed the layer-structured q-CS with semiconductor properties, such as appreciable interband photoluminescence. Theoretical studies on the band structure demonstrated that the optical properties of copper-dodecanethiol assemblies were dominated by the q-CS layer and the photoluminescence originated from exciton radiative recombination across an indirect band gap, borne out by experimental observation at higher temperatures, but with the onset of a direct emission process at cryogenic temperatures. The following studies revealed that the metal-metal bonding occurred not only in copper-alkanethiolate complex assemblies with variable alkyl chain length but also in silver-alkanethiolate and cadmium-alkanethiolate assemblies. Therefore, the current studies may herald a class of 2D semiconductors with extremely thin thickness out of nonlayered metal sulfides to bridge the gap between conventional inorganic semiconductors and organic semiconductors.
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http://dx.doi.org/10.1021/acsnano.0c07388DOI Listing
January 2021

Enhanced-Performance PEDOT:PSS/CuSe-Based Composite Films for Wearable Thermoelectric Power Generators.

ACS Appl Mater Interfaces 2021 Jan 4;13(1):631-638. Epub 2021 Jan 4.

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China.

Herein, we report the preparation and thermoelectric (TE) properties of flexible PEDOT:PSS/CuSe-based nanocomposite films on a nylon membrane using facile vacuum filtration and then hot pressing. The main composition of the composite film changed during hot pressing, causing the change of the carrier transport and TE performance intensively. Consequently, the optimized film shows a high power factor of 820 μW/mK at 400 K, which is 3 times as high as that of the nonhot-pressed one. The film shows excellent flexibility with 85% retention of the power factor after 1000 bending cycles around a 5 mm diameter rod. The outstanding flexibility results from a good combination between the nylon membrane and the CuSe-based nanoporous structured film. By pairing with n-type PEDOT/AgSe/CuAgSe films, a ten-legged flexible TE generator outputs maximum voltage and power of 50 mV and 1.55 μW, respectively, at a temperature difference of 44 K. Our research opens up a promising avenue to design high property flexible TE films for energy conversion.
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http://dx.doi.org/10.1021/acsami.0c18577DOI Listing
January 2021

Quantitative Mapping of Glutathione within Intracranial Tumors through Interlocked MRI Signals of a Responsive Nanoprobe.

Angew Chem Int Ed Engl 2021 04 1;60(15):8130-8138. Epub 2021 Mar 1.

Department Key Laboratory of Colloid Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing, 100190, China.

Studies reveal that malignant tumors feature uneven distributions of some key biomarkers across the entire tumorous region. Nevertheless, only very limited progress has been made towards non-invasive and quantitative detection of tumor-specific biomarkers in vivo, especially with clinically compatible imaging modalities. Reported here is an Fe O nanoparticle-based glutathione (GSH) responsive magnetic resonance imaging (MRI) probe that can form particle aggregates within tumors in vivo to give rise to strong GSH concentration dependent interlocked relaxivities. A quantitative correlation between the interlocked MRI signals and local GSH concentration was established, and further applied for mapping the heterogeneous distribution of GSH within an intracranial tumor (2.4 mm × 1.6 mm) in vivo. This methodology will offer a practical route for quantitatively mapping tumor-specific biomarkers in vivo with unlimited detection depth, which largely challenges optical-imaging-based approaches.
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http://dx.doi.org/10.1002/anie.202014348DOI Listing
April 2021

Doping Lanthanide Nanocrystals With Non-lanthanide Ions to Simultaneously Enhance Up- and Down-Conversion Luminescence.

Front Chem 2020 23;8:832. Epub 2020 Sep 23.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China.

The rare-earth nanocrystals containing Er emitters offer very promising tools for imaging applications, as they can not only exhibit up-conversion luminescence but also down-conversion luminescence in the second near-infrared window (NIR II). Doping non-lanthanide cations into host matrix was demonstrated to be an effective measure for improving the luminescence efficiency of Er ions, while still awaiting in-depth investigations on the effects of dopants especially those with high valence states on the optical properties of lanthanide nanocrystals. To address this issue, tetravalent Zr doped hexagonal NaGdF:Yb,Er nanocrystals were prepared, and the enhancement effects of the Zr doping level on both up-conversion luminescence in the visible window and down-conversion luminescence in NIR II window were investigated, with steady-state and transient luminescence spectroscopies. The key role of the local crystal field distortions around Er emitters was elucidated in combination with the results based on both of Zr and its lower valence counterparts, e.g., Sc, Mg, Mn. Univalent ions such as Li was utilized to substitute Na ion rather than Gd, and the synergistic effects of Zr and Li ions by co-doping them into NaGdF:Yb,Er nanocrystals were investigated toward optimal enhancement. Upon optimization, the up-conversion emission of co-doped NaGdF:Yb,Er nanocrystals was enhanced by more than one order of magnitude compared with undoped nanocrystals. The current studies thus demonstrate that the local crystal field surrounding emitters is an effective parameter for manipulating the luminescence of lanthanide emitters.
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http://dx.doi.org/10.3389/fchem.2020.00832DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7538674PMC
September 2020

Longer and Stronger: Improving Persistent Luminescence in Size-Tuned Zinc Gallate Nanoparticles by Alcohol-Mediated Chromium Doping.

ACS Nano 2020 09 19;14(9):12113-12124. Epub 2020 Aug 19.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China.

Benefiting from near-infrared persistent luminescence, chromium-doped zinc gallate nanoparticles have become appealing for background-free biomedical imaging applications, where autofluorescence from adjacent tissues no longer poses a problem. Nevertheless, the synthesis of persistent luminescent nanoparticles with controllable and biologically appropriate size, high luminescence intensity, and long persistent duration remains very challenging. Herein, we report a solvothermal synthetic route for preparing differently sized ZnGaO:Cr nanoparticles with a particle size tunable from 4 to 31 nm and afterglow duration longer than 20 h. The route involves lower reaction temperatures and involves no reworking of the particles postsynthesis, providing materials that have far fewer unwanted defects and much higher luminescence yields (up to 51%). It was found that methanol played a paramount role in obtaining the Cr-doped ZnGaO nanoparticles. The effects of methanol were discussed in combination with NMR spectroscopy studies and theoretical calculations, and the underlying alcohol-mediated growth and doping mechanisms were elucidated, which will be beneficial for developing highly persistent luminescent nanoparticles.
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http://dx.doi.org/10.1021/acsnano.0c05655DOI Listing
September 2020

An MRI contrast agent based on a zwitterionic metal-chelating polymer for hepatorenal angiography and tumor imaging.

J Mater Chem B 2020 08;8(31):6956-6963

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China.

MRI contrast agents such as paramagnetic Gd(iii)-chelates, can improve the ability of MRI in differentiating diseased and healthy tissues, and have been widely used in clinical diagnosis. However, the enhancement effect of small molecular MRI contrast agents is unsatisfied due to their relative high rotation rates. Furthermore, the small molecular contrast agents also suffer from the short blood half-life and nonspecific extracellular diffusion in tissues, which also restricts their applications. To address these issues, we developed a macromolecular MRI contrast agent based on a zwitterionic metal-chelating polymer. Poly(acrylic acid) (PAA) was chosen as the main chain, and diethylenetriamine pentaacetic acid (DTPA) as the metal-chelating group was coupled through the carboxyl groups of PAA using diethylenetriamine (DET) as a linker. The macromolecular MRI contrast agent constructed by chelating with Gd3+ (Gd-PAA) exhibited a much higher longitudinal relaxation rate (r1) than the clinical contrast agent Gd-DTPA. Importantly, due to the stealth ability of the zwitterionic structure, Gd-PAA can reside in the blood long enough without any microvascular leakage in the extracellular space of normal tissues, which allows it to be used for precise blood MR imaging, such as hepatorenal angiography, but also for tumor imaging because of the enhanced permeability and retention (EPR) effecta. Besides, the result of long-term toxicity tests highlights the safety feature of the current contrast agent. Hence, the current contrast agent overcomes the defect of traditional small molecular Gd(iii)-based T1-weighted contrast agents and shows great prospects for future clinical applications.
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http://dx.doi.org/10.1039/d0tb00893aDOI Listing
August 2020

Recent advances in molecular imaging of atherosclerotic plaques and thrombosis.

Nanoscale 2020 Apr 2;12(15):8040-8064. Epub 2020 Apr 2.

State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X), Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, China.

As the complications of atherosclerosis such as myocardial infarction and stroke are still one of the leading causes of mortality worldwide, the development of new diagnostic tools for the early detection of plaque instability and thrombosis is urgently needed. Advanced molecular imaging probes based on functional nanomaterials in combination with cutting edge imaging techniques are now paving the way for novel and unique approaches to monitor the inflammatory progress in atherosclerosis. This review focuses on the development of various molecular probes for the diagnosis of plaques and thrombosis in atherosclerosis, along with perspectives of their diagnostic applications in cardiovascular diseases. Specifically, we summarize the biological targets that can be used for atherosclerosis and thrombosis imaging. Then we describe the emerging molecular imaging techniques based on the utilization of engineered nanoprobes together with their challenges in clinical translation.
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http://dx.doi.org/10.1039/d0nr00599aDOI Listing
April 2020

Red blood cell membrane-coated upconversion nanoparticles for pretargeted multimodality imaging of triple-negative breast cancer.

Biomater Sci 2020 Mar;8(7):1802-1814

Department of Nuclear Medicine, Union Hospital, Tongji Medical College, Huazhong University of Science and Technology, Wuhan 430022, China. and Hubei Province Key Laboratory of Molecular Imaging, Wuhan 430022, China.

Upconversion nanoparticles (UCNPs) have been widely employed for tumor imaging using magnetic resonance imaging (MRI) and upconversion luminescence (UCL) imaging. The short blood clearance time and immunogenicity of UCNPs have limited their further application in vivo. We have designed UCNPs camouflaged with an exterior red blood cell (RBC) membrane coating (RBC-UCNPs) to solve these problems. Moreover, because of some intrinsic disadvantages of MRI and UCL imaging, we investigated the use of pretargeted RBC-UCNPs for positron-emission tomography (PET) imaging to obtain more comprehensive information. Our data showed that RBC-UCNPs retained the immunity feature from the source cells and the superior optical and chemical features from the pristine UCNP cores. The tumor-targeting ability of RBC-UCNPs was enhanced by binding 1,2-distearoyl-sn-glycero-3-phosphoethanolamine-N-[folate(polyethylene glycol)-2000] (DSPE-PEG-FA) molecules onto the cell membranes. PET imaging with short half-life radionuclides to visualize the RBC-UCNPs was successfully realized by a combination of pre-targeting and in vivo click chemistry. Blood chemistry, hematology, and histologic analysis suggested good in vivo biocompatibility of the RBC-UCNPs. Our method provides a new potential biomedical application of biomimetic nanoparticles.
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http://dx.doi.org/10.1039/d0bm00029aDOI Listing
March 2020

Ultra-sensitive Nanoprobe Modified with Tumor Cell Membrane for UCL/MRI/PET Multimodality Precise Imaging of Triple-Negative Breast Cancer.

Nanomicro Lett 2020 Feb 22;12(1):62. Epub 2020 Feb 22.

Department of Nuclear Medicine, Union Hospital, Tongji Medical College, Huazhong University of Science and Technology, Wuhan, 430022, People's Republic of China.

Triple-negative breast cancer (TNBC) is a subtype of breast cancer in which the estrogen receptor and progesterone receptor are not expressed, and human epidermal growth factor receptor 2 is not amplified or overexpressed either, which make the clinical diagnosis and treatment very challenging. Molecular imaging can provide an effective way to diagnose TNBC. Upconversion nanoparticles (UCNPs), are a promising new generation of molecular imaging probes. However, UCNPs still need to be improved for tumor-targeting ability and biocompatibility. This study describes a novel probe based on cancer cell membrane-coated upconversion nanoparticles (CCm-UCNPs), owing to the low immunogenicity and homologous-targeting ability of cancer cell membranes, and modified multifunctional UCNPs. This probe exhibits excellent performance in breast cancer molecular classification and TNBC diagnosis through UCL/MRI/PET tri-modality imaging in vivo. By using this probe, MDA-MB-231 was successfully differentiated between MCF-7 tumor models in vivo. Based on the tumor imaging and molecular classification results, the probe is also expected to be modified for drug delivery in the future, contributing to the treatment of TNBC. The combination of nanoparticles with biomimetic cell membranes has the potential for multiple clinical applications.
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http://dx.doi.org/10.1007/s40820-020-0396-4DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7770711PMC
February 2020

Metformin-Induced Stromal Depletion to Enhance the Penetration of Gemcitabine-Loaded Magnetic Nanoparticles for Pancreatic Cancer Targeted Therapy.

J Am Chem Soc 2020 03 28;142(10):4944-4954. Epub 2020 Feb 28.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, P. R. China.

Pancreatic ductal adenocarcinoma, as one of the most aggressive cancers, is characterized by rich desmoplastic stroma that forms a physical barrier for anticancer drugs. To address this issue, we herein report a two-step sequential delivery strategy for targeted therapy of pancreatic cancer with gemcitabine (GEM). In this sequential strategy, metformin (MET) was first administrated to disrupt the dense stroma, based on the fact that MET downregulated the expression of fibrogenic cytokine TGF-β to suppress the activity of pancreatic stellate cells (PSCs), through the 5'-adenosine monophosphate-activated protein kinase pathway of PANC-1 pancreatic cancer cells. In consequence, the PSC-mediated desmoplastic reactions generating α-smooth muscle actin and collagen were inhibited, which promoted the delivery of GEM and pH (low) insertion peptide (pHLIP) comodified magnetic nanoparticles (denoted as GEM-MNP-pHLIP). In addition, pHLIP largely increased the binding affinity of the nanodrug to PANC-1 cells. The targeted delivery and effective accumulation of MET/GEM-MNP-pHLIP in vivo were confirmed by magnetic resonance imaging enhanced by the underlying magnetic nanoparticles. The tumor growth inhibition of the sequential MET and GEM-MNP-pHLIP treatment were investigated on both subcutaneous and orthotopic tumor mice models. A remarkably improved therapeutic efficacy, for example, up to 91.2% growth inhibition ratio over 30 d of treatment, well-exemplified the novel cascade treatment for pancreatic cancer and the innovative use of MET.
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http://dx.doi.org/10.1021/jacs.0c00650DOI Listing
March 2020

Manganese-Mediated Growth of ZnS Shell on KMnF:Yb,Er Cores toward Enhanced Up/Downconversion Luminescence.

ACS Appl Mater Interfaces 2020 Mar 28;12(10):11934-11944. Epub 2020 Feb 28.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing 100190, China.

Epitaxially growing a semiconductor shell on the surface of upconversion nanocrystals to form a core/shell structure is believed to be a promising strategy to improve the luminescent efficiency of lanthanide ions doped in particle cores and, meanwhile, enriches the optical properties of the resulting nanocrystals. However, liquid-phase synthesis of such core/shell-structured nanocrystals comprised of a lanthanide ion-doped core and semiconductor shell remains challenging because of the chemical incompatibilities between lanthanides and the most intermediate gap semiconductors. In this context, the successful growth of ZnS shell on a KMnF core codoped with Yb/Er ions is reported to enhance the upconversion luminescence of Er ions. The underlying core/shell formation mechanism is elucidated in detail combining the hard-soft acid-base theory with structural analysis of the resulting nanocrystals. Quite unexpectedly, Mn diffusion across the core/shell interface occurs during ZnS shell growth, giving rise to Mn emission from the ZnS shell. Thus, the resulting core/shell particles exhibited unique up/downconversion luminescence from doped lanthanide metal ions and transition-metal ions, respectively. By manipulating the ion diffusion and shell growth kinetics, the upconversion and downconversion luminescent performance of KMnF:Yb,[email protected] nanocrystals are further optimized and the related mechanisms are discussed. Further, temperature-dependent upconversion and downconversion photoluminescence properties of KMnF:Yb,[email protected] nanocrystals show potential for ratiometric luminescence temperature sensing.
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http://dx.doi.org/10.1021/acsami.9b21832DOI Listing
March 2020

Electrosprayed Soft Capsules of Millimeter Size for Specifically Delivering Fish Oil/Nutrients to the Stomach and Intestines.

ACS Appl Mater Interfaces 2020 Feb 24;12(5):6536-6545. Epub 2020 Jan 24.

National R&D Branch Center for Freshwater Aquatic Products Processing Technology (Shanghai), Integrated Scientific Research Base on Comprehensive Utilization Technology for By-Products of Aquatic Product Processing, Ministry of Agriculture and Rural Affairs of the People's Republic of China, Shanghai Engineering Research Center of Aquatic-Product Processing and Preservation, College of Food Science & Technology , Shanghai Ocean University , Shanghai 201306 , China.

Contrasting to the traditional centimeter-sized soft capsules that are difficult to swallow or micro/nanometer-sized soft capsules that suffer from limited loading capacity for fish oil/nutrients and lowered stability, the millimeter-sized soft capsules with good enough stability could be a potential solution in solving these problems. Herein, we report millimeter-sized soft core-shell capsules of 0.42-1.85 mm with an inner diameter of 0.36-1.75 mm, for fish oil/nutrients, obtained through an electrospray approach upon optimization of different fabrication parameters such as applied voltage, sodium alginate concentration, shell/core feeding rate ratio, times of feeding rate, and types of coaxial needles. Further in vitro and in vivo studies reveal that the resulting soft capsules were apparently weakened and became mechanically destructive in the simulated small intestine solution and were totally destroyed in the simulated small intestine solution if they were first treated in the simulated stomach solution but not in the simulated stomach solution, which makes the millimeter-sized capsules useful as containers for specific delivery of fish oils and lipophilic nutrients to the stomach and intestines with excellent in vivo bioavailability (>90%). The whole fabrication approach is very facile with no complicated polymer modification and formulations involved, which endows the resulting soft capsules with broad application prospect in food and drug industries.
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http://dx.doi.org/10.1021/acsami.9b23623DOI Listing
February 2020

Biocompatible near-infrared quantum dots delivered to the skin by microneedle patches record vaccination.

Sci Transl Med 2019 12;11(523)

Koch Institute for Integrative Cancer Research, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, USA.

Accurate medical recordkeeping is a major challenge in many low-resource settings where well-maintained centralized databases do not exist, contributing to 1.5 million vaccine-preventable deaths annually. Here, we present an approach to encode medical history on a patient using the spatial distribution of biocompatible, near-infrared quantum dots (NIR QDs) in the dermis. QDs are invisible to the naked eye yet detectable when exposed to NIR light. QDs with a copper indium selenide core and aluminum-doped zinc sulfide shell were tuned to emit in the NIR spectrum by controlling stoichiometry and shelling time. The formulation showing the greatest resistance to photobleaching after simulated sunlight exposure (5-year equivalence) through pigmented human skin was encapsulated in microparticles for use in vivo. In parallel, microneedle geometry was optimized in silico and validated ex vivo using porcine and synthetic human skin. QD-containing microparticles were then embedded in dissolvable microneedles and administered to rats with or without a vaccine. Longitudinal in vivo imaging using a smartphone adapted to detect NIR light demonstrated that microneedle-delivered QD patterns remained bright and could be accurately identified using a machine learning algorithm 9 months after application. In addition, codelivery with inactivated poliovirus vaccine produced neutralizing antibody titers above the threshold considered protective. These findings suggest that intradermal QDs can be used to reliably encode information and can be delivered with a vaccine, which may be particularly valuable in the developing world and open up new avenues for decentralized data storage and biosensing.
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http://dx.doi.org/10.1126/scitranslmed.aay7162DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7532118PMC
December 2019

Self-Illuminating Agents for Deep-Tissue Optical Imaging.

Front Bioeng Biotechnol 2019 12;7:326. Epub 2019 Nov 12.

State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X), Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou, China.

Optical imaging plays an indispensable role in biology and medicine attributing to its noninvasiveness, high spatiotemporal resolution, and high sensitivity. However, as a conventional optical imaging modality, fluorescence imaging confronts issues of shallow imaging depth due to the need for real-time light excitation which produces tissue autofluorescence. By contrast, self-luminescence imaging eliminates the concurrent light excitation, permitting deeper imaging depth and higher signal-to-background ratio (SBR), which has attracted growing attention. Herein, this review summarizes the progress on the development of near-infrared (NIR) emitting self-luminescence agents in deep-tissue optical imaging with highlighting the design principles including molecular- and nano-engineering approaches. Finally, it discusses current challenges and guidelines to develop more effective self-illuminating agents for biomedical diagnosis and treatment.
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http://dx.doi.org/10.3389/fbioe.2019.00326DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6861855PMC
November 2019

Biocompatible off-stoichiometric copper indium sulfide quantum dots with tunable near-infrared emission via aqueous based synthesis.

Chem Commun (Camb) 2019 Dec;55(100):15053-15056

Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Zhengzhou Road 53, Qingdao 266042, China.

The present study reports an aqueous synthesis approach towards off-stoichiometric copper indium sulfide quantum dots with emissions in the near-infrared spectral range. The photoluminescence properties of the dots, and in particular the appearance of dual emission at high Cu deficiency, were studied with temperature-dependent steady-state and transient photoluminescence spectroscopy.
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http://dx.doi.org/10.1039/c9cc07674cDOI Listing
December 2019

NIR nanoprobe-facilitated cross-referencing manifestation of local disease biology for dynamic therapeutic response assessment.

Chem Sci 2019 Nov 27;11(3):803-811. Epub 2019 Nov 27.

Division of Chemistry and Biological Chemistry, School of Physical & Mathematical Sciences, Nanyang Technological University Singapore 637371 Singapore

Pharmacological interventions for effective treatment require opportune, dynamic and accurate manifestation of pathological status. Traditional clinical techniques relying on biopsy-based histological examinations and blood tests are dramatically restricted due to their invasiveness, unsatisfactory precision, non-real-time reporting and risk of complications. Although current strategies through molecular imaging enable non-invasive and spatiotemporal mapping of pathological changes in intact organisms, environment-activatable, sensitive and quantitative sensing platforms, especially for dynamic feedback of the therapeutic response, are still urgently desired in practice. Herein, we innovatively integrate deep-tissue penetrable multispectral optoacoustic tomography (MSOT) and near-infrared (NIR) optical imaging based technology by tailoring a free radical-responsive chromophore with photon-upconverting nanocrystals. During the therapeutic process, the specific reactions between the drug-stimulated reactive oxygen species (ROS) and radical-sensitive probes result in an absorption shift, which can be captured by MSOT. Meanwhile, the radical-triggered reaction also induces multispectral upconversion luminescence (UCL) responses that exhibit the opposite trend in comparison to MSOT. Such reversed-ratiometric dual-modal imaging outcomes provide an ideal cross-referencing system that guarantees the maximum sensing specificity and sensitivity, thus enabling precise disease biology evaluation and treatment assessments .
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http://dx.doi.org/10.1039/c9sc04909fDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8146619PMC
November 2019

Biodegradable Inorganic Nanoparticles for Cancer Theranostics: Insights into the Degradation Behavior.

Bioconjug Chem 2020 02 12;31(2):315-331. Epub 2019 Dec 12.

Center for Molecular Imaging and Nuclear Medicine, State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) , Soochow University, Collaborative Innovation Center of Radiological Medicine of Jiangsu Higher Education Institutions , Suzhou 215123 , China.

Inorganic nanoparticles as a versatile nanoplatform have been broadly applied in the diagnosis and treatment of cancers due to their inherent superior physicochemical properties (including magnetic, thermal, optical, and catalytic performance) and excellent functions (e.g., imaging, targeted delivery, and controlled release of drugs) through surface functional modification or ingredient dopant. However, in practical biological applications, inorganic nanomaterials are relatively difficult to degrade and excrete, which induces a long residence time in living organisms and thus may cause adverse effects, such as inflammation and tissue cysts. Therefore, the development of biodegradable inorganic nanomaterials is of great significance for their biomedical application. This Review will focus on the recent advances of degradable inorganic nanoparticles for cancer theranostics with highlight on the degradation mechanism, aiming to offer an in-depth understanding of degradation behavior and related biomedical applications. Finally, key challenges and guidelines will be discussed to explore biodegradable inorganic nanomaterials with minimized toxicity issues, facilitating their potential clinical translation in cancer diagnosis and treatment.
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http://dx.doi.org/10.1021/acs.bioconjchem.9b00699DOI Listing
February 2020

Emitting/Sensitizing Ions Spatially Separated Lanthanide Nanocrystals for Visualizing Tumors Simultaneously through Up- and Down-Conversion Near-Infrared II Luminescence In Vivo.

Small 2019 12 25;15(51):e1905344. Epub 2019 Nov 25.

Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, Chinese Academy of Sciences, Bei Yi Jie 2, Zhong Guan Cun, Beijing, 100190, P. R. China.

Near-infrared lights have received increasing attention regarding imaging applications owing to their large tissue penetration depth, high spatial resolution, and outstanding signal-to-noise ratio, particularly those falling in the second near-infrared window (NIR II) of biological tissues. Rare earth nanoparticles containing Er ions are promising candidates to show up-conversion luminescence in the first near-infrared window (NIR I) and down-conversion luminescence in NIR II as well. However, synthesizing particles with small size and high NIR II luminescence quantum yield (QY) remains challenging. Er ions are herein innovatively combined with Yb ions in a NaErF @NaYbF core/shell manner instead of being codoped into NaLnF matrices, to maximize the concentration of Er in the emitting core. After further surface coating, NaErF @NaYbF @NaYF core/shell/shell particles are obtained. Spectroscopy studies are carried out to show the synergistic impacts of the intermediate NaYbF layer and the outer NaYF shell. Finally, NaErF @NaYbF @NaYF nanoparticles of 30 nm with NIR II luminescence QY up to 18.7% at room temperature are obtained. After covalently attaching folic acid on the particle surface, tumor-specific nanoprobes are obtained for simultaneously visualizing both subcutaneous and intraperitoneal tumor xenografts in vivo. The ultrahigh QY of down-conversion emission also allows for visualization of the biodistribution of folate receptors.
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http://dx.doi.org/10.1002/smll.201905344DOI Listing
December 2019

Light-triggered crosslinking of gold nanoparticles for remarkably improved radiation therapy and computed tomography imaging of tumors.

Nanomedicine (Lond) 2019 11 22;14(22):2941-2955. Epub 2019 Nov 22.

State Key Laboratory of Radiation Medicine & Protection, School for Radiological & Interdisciplinary Sciences (RAD-X) & Collaborative Innovation Centre of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, PR China.

We aimed to characterize the tumor-targeting and radiosensitization properties of the photo-responsive gold nanoparticles (AuNPs) decorated photolabile diazirine group and folic acid for improved radiotherapy and computed tomography imaging of tumors. Folic acid and photolabile diazirine group were covalently conjugated on the surface of AuNPs to afford the desired photo-responsive dAuNP-FA (AuNPs capped with poly(ethylene) glycol ligands bearing photolabile diazirine group and folic acid). The probes were intravenously injected into tumor-bearing mice followed by photocrosslinking upon 405 nm laser irradiation for radiotherapy and computed tomography imaging of tumors . Light-triggered crosslinking of AuNPs remarkably enhanced the accumulation and retention of AuNPs within tumors. We have successfully developed a novel photo-responsive Au particle-based tumor theranostic probe showing remarkably improved tumor targeting ability and radiosensitization effect.
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http://dx.doi.org/10.2217/nnm-2019-0015DOI Listing
November 2019

Viscoelastic characterization of injured brain tissue after controlled cortical impact (CCI) using a mouse model.

J Neurosci Methods 2020 01 4;330:108463. Epub 2019 Nov 4.

Institute of Medical Imaging Technology, School of Biomedical Engineering, Shanghai Jiao Tong University, Shanghai 200030, China. Electronic address:

Background: Mechanical properties of the brain tissue are crucial to understand the mechanisms of traumatic brain injury (TBI). Injured brain tissue could induce changes of mechanical properties and anatomical structures. However, limited data is available for the injured tissue.

New Method: We developed a custom-built device to introduce controlled cortical impact (CCI) to brain with controlled impact velocity and direction. A study protocol for measuring the viscoelastic properties of injured brain tissue was also developed. Micro-scale morphological changes of the vasculature were quantified by analyzing confocal images of the brain tissue using CLARITY method.

Results: Results showed significant differences of the instantaneous shear modulus of the impact region from different impact angles. However, no significant differences were found for long-term shear modulus by varying the impact angles and velocities. Analysis of the vasculature showed an increased radius of the vessels in the injured tissue compared with that in the control group.

Comparison With Existing Methods: A combination of three different impact velocities and three different impact angles were adopted for producing injury to the brain. In addition, viscoelastic properties were compared between the injured and non-injured regions. The corresponding morphological changes of the vasculature system were also investigated.

Conclusions: The instantaneous shear modulus at the impact region was significantly different for the three impact angles. Compared to that of the control group, increased radius of the vasculature was also observed in the injured brain tissue. Results indicated that the biomechanical and structural changes of the injured tissue were closely related to the impact angles and velocities. Viscoelastic measurements could also help validation of computational models.
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http://dx.doi.org/10.1016/j.jneumeth.2019.108463DOI Listing
January 2020

Radiolabeling nanomaterials for multimodality imaging: New insights into nuclear medicine and cancer diagnosis.

Biomaterials 2020 01 22;228:119553. Epub 2019 Oct 22.

Center for Molecular Imaging and Nuclear Medicine, State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X), Soochow University, Collaborative Innovation Center of Radiological Medicine of Jiangsu Higher Education Institutions, Suzhou, 215123, China; Institute of Chemistry, Chinese Academy of Sciences/School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100190, China.

Nuclear medicine imaging has been developed as a powerful diagnostic approach for cancers by detecting gamma rays directly or indirectly from radionuclides to construct images with beneficial characteristics of high sensitivity, infinite penetration depth and quantitative capability. Current nuclear medicine imaging modalities mainly include single-photon emission computed tomography (SPECT) and positron emission tomography (PET) that require administration of radioactive tracers. In recent years, a vast number of radioactive tracers have been designed and constructed to improve nuclear medicine imaging performance toward early and accurate diagnosis of cancers. This review will discuss recent progress of nuclear medicine imaging tracers and associated biomedical imaging applications. Radiolabeling nanomaterials for rational development of tracers will be comprehensively reviewed with highlights on radiolabeling approaches (surface coupling, inner incorporation and interface engineering), providing profound understanding on radiolabeling chemistry and the associated imaging functionalities. The applications of radiolabeled nanomaterials in nuclear medicine imaging-related multimodality imaging will also be summarized with typical paradigms described. Finally, key challenges and new directions for future research will be discussed to guide further advancement and practical use of radiolabeled nanomaterials for imaging of cancers.
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http://dx.doi.org/10.1016/j.biomaterials.2019.119553DOI Listing
January 2020

Regional biomechanical imaging of liver cancer cells.

J Cancer 2019 25;10(19):4481-4487. Epub 2019 Jul 25.

State Key Laboratory of Radiation Medicine and Protection, School of Radiation Medicine and Protection, Collaborative Innovation Center of Radiological Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, China.

Liver cancer is one of the leading cancers, especially in developing countries. Understanding the biomechanical properties of the liver cancer cells can not only help to elucidate the mechanisms behind the cancer progression, but also provide important information for diagnosis and treatment. At the cellular level, we used well-established atomic force microscopy (AFM) techniques to characterize the heterogeneity of mechanical properties of two different types of human liver cancer cells and a normal liver cell line. Stiffness maps with a resolution of 128x128 were acquired for each cell. The distributions of the indentation moduli of the cells showed significant differences between cancerous cells and healthy controls. Significantly, the variability was even greater amongst different types of cancerous cells. Fitting of the histogram of the effective moduli using a normal distribution function showed the Bel7402 cells were stiffer than the normal cells while HepG2 cells were softer. Morphological analysis of the cell structures also showed a higher cytoskeleton content among the cancerous cells. Results provided a foundation for applying knowledge of cell stiffness heterogeneity to search for tissue-level, early-stage indicators of liver cancer.
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http://dx.doi.org/10.7150/jca.32985DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6746127PMC
July 2019
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