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Nature Communications · 2021 ·Vol. 12 ·期 1 ·1-8 · IF 14.919

Visualization of gaseous iodine adsorption on single zeolitic imidazolate framework-90 particles

Lei Yuting,Zhang Guihua,Zhang Qinglan,Yu Ling,Li Hua,Yu Haili,He Yi

Zeolitic imidazolate frameworks (ZIFs) are very useful as high-capacity iodine (I 2 ) adsorbents. The adsorption performance is usually probed by measuring a statistical average property over an entire sample consisting of a large number of ZIF particles, leaving the interparticle heterogeneity information among individuals. Here we report a dark-field microscopy (DFM) method to visualize gaseous I 2 adsorption on single ZIF-90 particles in situ and in real time. The adsorption of I 2 is found to alter the scattering spectrum of ZIF-90 particles, inducing a distinct color change from bluewhite to yellow. According to correlating the adsorption amount of gaseous I 2 with the change of B value from DFM images, we quantitatively image the adsorption process and estimate the related kinetic parameters at the single particle level. Single particle measurements clarify the large particle-to-particle heterogeneity in adsorption reactivity and significant adsorption activity improvement of ZIF-90 after introduction of linker defects, which provides a microscopic understanding of the structure-activity relationship. We further demonstrate the capacity of this strategy for studying gaseous I 2 adsorption on single ZIF-91 particle as a derivative of ZIF-90 to illustrate the generality.

研究领域: 材料科学 · 化学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Thermal Stability and Kinetics of Single I2@ZIF-8 Particles

Qianxi Wang,Yuting Lei,Yunyi Cui,Jingruolan Lin,Wei Huang,Yi He

Thermogravimetric analysis (TGA) is a key material characterization method for studying the thermal stability and thermochemical process. However, the common TGA for bulk samples lacks sufficient spatial information, which blurs the intrinsic thermal decomposition characteristic and limits the understanding of the structure–performance relationship. Here, we report a dark-field microscope (DFM) method for studying thermal desorption process of I2 from I2-loaded zeolitic imidazolate framework-8 (I2@ZIF-8). Because of the high spatial resolution, DFM enables the imaging and tracking of the local mass loss of I2 in single I2@ZIF-8 particles at different reaction temperatures. We obtain from the DFM images the single-particle thermogravimetric and differential thermogravimetric curves to evaluate the inherent thermal stability of single I2@ZIF-8 particles. We also find the heterogeneous thermal decomposition property among different I2@ZIF-8 particles. Furthermore, we demonstrate the capacity of DFM to quantitatively determine thermal kinetics parameters such as the diffusion coefficient and activation energy of I2 in individual and multiple ZIF-8 particles. These useful results are essential for developing high-efficient porous adsorbents for the capture of I2.

CAS / MDL: 64-17-5 693-98-1
研究领域: 材料科学 · 化学工程
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ANALYST · 2019 ·Vol. 144 ·期 6 ·2011-2016 · IF 4.019

A single gold nanoprobe for colorimetric detection of silver(I) ions with dark-field microscopy

Yi Fen Xie,Yun Ying Cheng,Meng Li Liu,Hong Yan Zou,Cheng Zhi Huang

Highly sensitive colorimetric detection of silver(I) ions (Ag+) at the single-particle level was developed based on the color of a gold nanoparticle (AuNP) assembly captured by dark-field microscopy (DFM) imaging. Formation of C–Ag+–C bonding between cytosines was utilized to induce interparticle coupling of AuNPs modified with single-strand DNA, resulting in a color change as the signal transduction to quantify Ag+ under DFM imaging. This method allowed visual quantitation of Ag+ in the range of 0.05 nM–250.00 nM and a detection limit of 28.8 pM was achieved. Furthermore, we demonstrated its applicability for the colorimetric detection of Ag+ in a small quantity of real samples, showing the good potential of this developed method for environmental monitoring and drug quality control.

CAS / MDL: 7761-88-8
研究领域: 分析化学 · 环境科学 · 药物分析
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TALANTA · 2024 · IF 5.6

Highly sensitive and specific detection of human papillomavirus type 16 using CRISPR/Cas12a assay coupled with an enhanced single nanoparticle dark-field microscopy imaging technique

Jiajia Hu,Yang Yu,Xiaoyan Pan,Yue han,Xinyi She,Xiaojun Liu,Qingquan Zhang,Hongwei Gai,Chenghua Zong

Human papillomavirus (HPV) is a prevalent sexually transmitted pathogen associated with cervical cancer . Detecting high-risk HPV (hr-HPV) infections is crucial for cervical cancer prevention, particularly in resource-limited settings. Here, we present a highly sensitive and specific sensor for HPV-16 detection based on CRISPR/Cas12a coupled with enhanced single nanoparticle dark-field microscopy (DFM) imaging techniques . Ag–Au satellites were assembled through the hybridization of AgNPs-based spherical nucleic acid (Ag-SNA) and AuNPs-based spherical nucleic acid (Au-SNA), and their disassembly upon target-mediated cleavage by the Cas12a protein was monitored using DFM for HPV-16 quantification. To enhance the cleavage efficiency and detection sensitivity, the composition of the ssDNA sequences on Ag-SNA and Au-SNA was optimized. Additionally, we explored using the SynSed technique (synergistic sedimentation of Brownian motion suppression and dehydration transfer) as an alternative particle transfer method in DFM imaging to traditional electrostatic deposition. This addresses the issue of inconsistent deposition efficiency of Ag–Au satellites and their disassembly due to their size and charge differences. The sensor achieved a remarkable limit of detection (LOD) of 10 fM, lowered by 9-fold compared to traditional electrostatic deposition methods . Clinical testing in DNA extractions from 10 human cervical swabs demonstrated significant response differences between the positive and negative samples. Our sensor offers a promising solution for sensitive and specific HPV-16 detection, with implications for cancer screening and management.

研究领域: 分子生物学 · 医学诊断 · 纳米技术
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Nanoscale · 2017 ·Vol. 9 ·期 10 ·3568-3575 · IF 7.367

Real-time dark-field light scattering imaging to monitor the coupling reaction with gold nanorods as an optical probe

Hong Zhi Zhang,Rong Sheng Li,Peng Fei Gao,Ni Wang,Gang Lei,Cheng Zhi Huang,Jian Wang

Gold nanorods (GNRs) have opened up promising applications based on their reshaping, due to the fact that a tiny change in shape or size could directly lead to optical changes. Herein, we report chemical reshaping of GNRs induced by the coupling reaction between Au, ferric chloride and thiourea. In the coupling reaction, Fe3+ oxidizes the GNRs to yield Au(I), which complexes with the thiourea ligand, lowering the Gibbs free energy of the gold species and promoting the reaction equilibrium to enable the chemical reshaping of the GNRs. This coupling reaction process was monitored using a light-scattering dark-field microscopy (DFM) imaging technique and scanning electron microscopy (SEM). The light scattering underwent a colour change from bright red to yellow and finally to green, and the GNRs underwent a morphological change from rod-shaped to fusiform and finally to spherical, which is somewhat different from the results of other chemical etching processes of GNRs. It is believed that the coupling reaction induced chemical reshaping of GNRs not only provides an alternative way to monitor the coupling reaction, but also offers a facile way to obtain a desirable GNR morphology, which is important for the preparation of fusiform nanostructures.

研究领域: 纳米材料科学 · 光学成像 · 化学动力学
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Highly Sensitive Determination of Copper Ions as MnO2 Etching Inhibitor in Single-Particle Nanoplasmonic Imaging

Jing Shang,Siyu Jiang,Pei Zhang,Jinsong Fan,Kun Li

Dark-field microscopy (DFM) imaging based on plasmonic metal nanoparticles has garnered significant attention. Here, we exploit the susceptibility of MnO2 to reduction to modulate the local dielectric environment of an Au nanoparticle core through the etching/antietching effects of specific targets on the encapsulated MnO2 shell. The presence of d-penicillamine promotes MnO2 etching, while the chelation of d-penicillamine with Cu2+ effectively inhibits this etching. By recording the Cu2+-induced color shift of scattered light from orange to bright green at the single-particle level and performing the statistical analysis of the green-to-red (G/R) values in DFM images, we achieved quantitative determination of Cu2+ with a wide linear range (0.1–10 μM) and a low limit of detection (4.55 nM). With the facile and reliable Cu2+ assay in real-world samples exemplifying the practicality of the single-particle nanoplasmonic imaging method, this work may inspire future DFM-based investigations of nanoshell etching inhibition processes.

CAS / MDL: 10031-43-3 6132-04-3
研究领域: 分析化学 · 纳米生物学
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY · 2021 · IF 1.134

Color-coded Adrenaline Assay Based on GNP@MnO2 Core-shell Nanoparticles with Dark-field Microscopy

Ya-Wen LIAN,Xiang YUAN,Le-Hui XIAO,Lin WEI

Adrenaline (AD) is an important hormone in central nervous system of mammals, and also works as a medium to transmit signal. The abnormal level of AD in nerve tissues and biological fluids can cause a variety of diseases. In this work, we developed a simple and sensitive dark-field microscopy (DFM)-based single-particle detection (SPD) method for quantitative detection of AD in aqueous solution. MnO 2 layer of GNP@MnO 2 core-shell nanoparticles could be readily etched due to the reducibility of AD. Since the localized surface plasmon resonance (LSPR) of GNPs was sensitive to the dielectric change of local environment, the etching process resulted in an evident color change of the probe and could be easily observed in real time under dark-field microscope. The AD was thus sensitively detected in a wide linear concentration range (0.02–5 μmol/L) with a limit of detection (LOD) of 7.17 nmol/L. Moreover, this method was used for the analysis of AD content in commercial injection and satisfactory recoveries were acquired. As a consequence, the sensing assay demonstrated herein based on GNP@MnO 2 NPs showed great application prospects in molecular recognition and drug quality assay.

研究领域: 生物化学 · 医学诊断 · 纳米技术
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ACS Sensors · 2018 · IF 5.711

Fast and Highly Sensitive Detection of Pathogens Wreathed with Magnetic Nanoparticles Using Dark-Field Microscopy

Fenglei Chen,Fang Tang,Chih-Tsung Yang,Xinyao Zhao,Jun Wang,Benjamin Thierry,Vipul Bansal,Jianjun Dai,Xin Zhou

Cryptosporidium parvum (C. parvum) is a highly potent zoonotic pathogen, which can do significant harm to both human beings and livestock. However, existing technologies or methods are deficient for rapid on-site detection of water contaminated with C. parvum. Better detection approaches are needed to allow water management agencies to stop major breakouts of the pathogen. Herein, we present a novel detection method for cryptosporidium in a tiny drop of sample using a magnetic nanoparticle (MNP) probe combined with dark-field microscopy in 30 min. The designed MNP probes bind with high affinity to C. parvum, resulting in the formation of a golden garland-like structure under dark-field microscopy. This MNP-based dark-field counting strategy yields an amazing PCR-like sensitivity of 8 attomolar (aM) (5 pathogens in 1 μL). Importantly, the assay is very rapid (∼30 min) and is very simple to perform as it involves only one step of mixing and magnetic separation, followed by dropping on a slide for counting under dark-field microscope. By combining the advantages of the specific light-scattering characteristic of MNP probe under dark field and the selective magnetic separation ability of functionalized MNP, the proposed MNP-based dark-field enumeration method offers low cost and significant translational potential.

CAS / MDL: 9005-64-5 67-56-1
研究领域: 寄生虫学 · 环境科学 · 医学诊断
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ANALYTICA CHIMICA ACTA · 2020 · IF 5.977

Gold nanoparticles enumeration with dark-field optical microscope for the sensitive glycoprotein sandwich assay

Yameng Han,Zhongju Ye,Langxing Chen,Lehui Xiao

Protein glycosylation is an important post-translational modification and glycoproteins are associated with many crucial metabolic progresses of life. In order to detect glycoproteins sensitively, we propose a gold nanoparticles (GNPs) enumeration method based on boronate affinity sandwich system, which is constructed between the boronic acid polymer functionalized magnetic nanoparticles (Fe 3 O 4 @MPS@VPBA NPs) and 4-mercaptophenylboronic acid modified GNPs (GNPs-MPBA) by the targeted glycoproteins as the linker. Therefore, the sandwich complex is formed, resulting in the decrease of GNPs-MPBA counts in the solution. Based on the dark-field microscope (DFM) imaging technique , the sensitive GNPs enumeration assay is developed for glycoproteins quantitation. Immunoglobulin (IgG), as one of the important glycoproteins, is introduced to evaluate the proposed method. A low detection limit of 1.22 ng mL −1 for IgG analysis is obtained. The result indicates that the proposed GNPs enumeration method offers a simple, effective, label-free and highly sensitive strategy without signal amplification. It also possesses great potential for various target molecules determination at the single-particle level in the future.

研究领域: 生物化学 · 分析化学 · 医学检测
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Nanoscale · 2014 ·Vol. 7 ·期 2 ·511-517 · IF 6.739

Real-time monitoring for the morphological variations of single gold nanorods

Tao Xie,Chao Jing,Wei Ma,Zhifeng Ding,Andrew James Gross,Yi-Tao Long

The morphological characteristics of metal nanoparticles, particularly the shape, play an essential role in the optical, physical and chemical properties. In this work, we reported a transverse etching process to investigate the morphological variations of single gold nanorods (GNRs). Dark-field microscopy and Rayleigh scattering spectroscopy were used as complementary technologies to track the transverse etching process. Dark-field imaging with high spatial and temporal resolution could easily monitor the transverse etching process of GNRs in situ and in real time. Interactions between the scattering spectrum and the morphological variations were judiciously calculated within the dipole approximation by the Drude function. The calculated peak shift of GNRs (Δλmax = 17 nm) was obtained via the ratio of the long axis and short axis (aspect ratio) of GNRs from transmission electron microscopy. The average scattering peak shift (Δλmax = 22 nm) from Rayleigh scattering spectroscopy was in good agreement with the calculated peak shift. Monitoring the morphological variations of single GNRs enables us to track the transverse etching of GNRs at arbitrary time. This promises to be a useful method for the study of different nanomaterials and their spectral properties.

CAS / MDL: 52-90-4 70-18-8 57-09-0
研究领域: 纳米材料科学 · 光学 · 化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Gold triangular nanoplates with edge effect for reaction monitoring under dark-field microscopy

Hongyan Zou,Xiaoying Gu,Chang Xia,Ru Cheng,Chengzhi Huang,Yuanfang Li,Pengfei Gao

True morphology imaging of individual nanoprobes with high sensitivity and in situ dynamic response is crucial in the dark-field microscopy imaging analysis. However, the geometry and orientation of the probes are experimentally challenging to visualize as their physical dimensions are usually below the diffraction limit. In this work, two-dimensional triangular gold nanoplates (AuNPLs) with the edge length > 600 nm and the thickness ~25 nm displayed clear triangular-shaped far-field scattering patterns (TFSPs) under a dark-field imaging system owing to the strong electrical field strength around the sharp edges and tips. Thus, their actual shape and orientation specific scattering image are directly visualized only by dark-field microscopy and furtherly applied to real-time monitor the etching and alloying progress of AuNPLs. The results showed that the reactive sites of AuNPLs are located at their vertices and sharp edges owing to the sensitive edge effect. This work provides a new perspective to directly monitor the conformation and dynamics of chemical reaction at the single particle level.

研究领域: 纳米技术 · 光学成像 · 化学动力学
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VIEW · 2023 · IF 8.6

A visualized automatic particle counting strategy for single-cell level telomerase activity quantification

Chen Li,Hui Chen,Tingting Fan,Jingru Zhao,Zheng Ding,Zeyu Lin,Shuqing Sun,Chunyan Tan,Feng Liu,Hongtao Jiang,Ying Tan

The accurate evaluation of telomerase activity, a typical cancer biomarker, is vital for early cancer screening. In this study, we developed a dark-field microscopy (DFM) visual single-particle detection scheme to detect telomerase activity based on automatic counting gold nanoparticles (AuNPs). This method started with attaching the telomerase substrate (TS) primer to the magnetic beads (MBs) through streptavidin-biotin interaction. In the presence of telomerase and dNTPs, the TS primer was expanded with (TTAGGG) n repeat units to form the telomerase extension product (MBs-telomerase extension product), which could be hybridized with the complementary DNA (cDNA) modified with AuNPs through Au-S bonds (AuNPs-SH-cDNA). After magnetic separation and DNA double-strand unwinding, AuNPs were collected from the supernatant, and the telomerase activity was quantitatively measured by visually counting bright spots based on DFM. This strategy achieved a limit of detection as low as 1 HeLa cell and distinguished telomerase activity among different cell lines, thus verifying its excellent sensitivity and specificity. Further, two common telomerase inhibitors (BIBR1532 and curcumin) were screened with the consistent IC 50 values with other methods, respectively. It is worth mentioning that this strategy can clearly identify bladder cancer among various urinary diseases. Consequently, the visualized automatic particle counting strategy is potential as a powerful tool in early and noninvasive diagnosis of bladder cancer.

CAS / MDL: 321674-73-1 458-37-7
研究领域: 生物医学 · 癌症诊断 · 纳米技术
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