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ACS Applied Nano Materials · 2020 · IF 0

Surface-Enhanced Raman Scattering Trace-Detection Platform Based on Continuous-Rolling-Assisted Evaporation on Superhydrophobic Surfaces

Yingnan Sun,Xiaodong Chen,Yongxin Zheng,Yuhan Song,Huairong Zhang,Shusheng Zhang

Surface-enhanced Raman scattering (SERS) has proved to be an efficient approach for ultrasensitive detection of highly diluted analytes, and the metal colloid-based SERS platform is one of the most successful techniques to perform evaporation-assisted collection and enrichment of highly diluted molecules in hot spot regions on various substrates. However, there are still no effective and facile ways to achieve high SERS sensitivity at femtomolar levels on superhydrophobic (SH) surfaces. Here, for the first time, an efficient and versatile strategy, termed continuous-rolling-assisted evaporation on an SH surface (CRESH), is developed for the ultrasensitive colloid-based SERS platform, which overcomes the inherent limitations of the pinning effect during evaporative enrichment on unpatterned SH substrates. This strategy combines an SH surface with a rolling property and droplet continuous-rolling motion in a synergistic way to achieve trace analyte detection at the femtomolar level. A 50 μL droplet based on CRESH can be considerably condensed from approximately 0.6 cm to 0.2 mm in diameter, and final sizes are independent of the initial droplet volumes, showing remarkable condensing efficiency and potential applications for a lower detection limit. Our results of numerical analysis of nanoparticle motions inside the droplet show, in contrast to common belief, that the CRESH strategy endows the SH surface with nearly pinning-free peculiarity by means of significantly reducing the critical contact line values when the Cassie–Wenzel transition occurs. As a proof of concept, CRESH is further evaluated by detecting trace quantities of Raman probes with quantitative SERS detection down to the femtomolar level (1 × 10–15 mol/L). Our platform may open the possibility of universal applications of unpatterned SH surfaces that have long been suspected to play a role in effective, facile, cost-effective, and ultrasensitive SERS detection.

研究领域: 分析化学 · 材料科学 · 纳米技术
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ANALYTICAL CHEMISTRY · 2018 · IF 6.042

Ultradeep Palmitoylomics Enabled by Dithiodipyridine-Functionalized Magnetic Nanoparticles

Xiaoqin Zhang,Yuting Zhang,Caiyun Fang,Lei Zhang,Pengyuan Yang,Changchun Wang,Haojie Lu

Palmitoylation, a type of fatty acylation, has vital roles in many biological processes. For ultradeep identification of protein palmitoylation, an enrichment approach based on a novel magnetic microsphere modified with 2,2′-dithiodipyridine (Fe3O4/SiO2-SSPy microsphere) is presented in this study. The Fe3O4/SiO2-SSPy microspheres were synthesized by directly coating thiol-containing silane coupling agent onto the magnetic supraparticles in aqueous solution at room temperature. Due to the intrinsic magnetic properties, high surface-to-volume ratios, and abundant reactive functional groups on the surface, these microspheres enabled direct capture of palmitoylated targets and convenient isolation, contributing to remarkable enrichment selectivity (purifying palmitoylated peptides from mixtures with nonpalmitoylated peptides even at a 1:500 molar ratio) and sensitivity (the detection limit was at femtomole level), thus enabling a global annotation of protein palmitoylation for complex biological samples. We successfully identified 1304 putative palmitoylated proteins from mouse brain tissues by using this method, which is the largest mouse palmitoylome data set to date. Except for those known members, many new proteins and pathways were also found to be regulated by palmitoylation.

CAS / MDL: 2127-03-9 4420-74-0
研究领域: 生物化学 · 蛋白质组学 · 纳米技术 · 分子生物学
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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

Structure-switching locked hairpin triggered rolling circle amplification for ochratoxin A (OTA) detection by ICP-MS

Jie Zhang,Yuheng Lu,Wei Gao,Peng Yang,Nansheng Cheng,Yanwen Jin,Junbo Chen

Ochratoxin A (OTA) is usually found in the contaminated cereal food that its trace concentration would cause severe carcinogenicity and neurotoxicity. Herein, a recognition-triggered structure switching-based element spectrometric assay was proposed for ultrasensitive and highly specific detection of OTA. OTA aptamer was first adapted into a primer for the formation of a locked hairpin (LHP), and followed by attachment on the surface of magnetic beads (MBs). In the presence of OTA, the binding event between OTA molecule and its aptamer induced the liberation of the primer for that is otherwise unable to spontaneously structure-switching. For the rolling circle amplification (RCA), thereby a dumbbell structure was designed as the template (DT). The hybridization of the dumbbell template with free primer initiates the rolling circle amplification along with the production of repeated sequences. To obtain the signal output, the DNA-AuNP tag was prepared which contained the complementary sequences with RCA products. Thus, each tag can hybridize with the repeated sequences derived from the RCA, enabling the formation of detectable signal by the following ICP-MS measurement. Such design can translate a single recognition event into numerous AuNPs, enabling amplified detection of OTA. Taking advantage of this principle, the OTA in real sample (AFP, PSA) can be quantified at femtomolar concentration and it can be expanded into application in food safety inspection.

研究领域: 食品安全 · 分析化学 · 毒理学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-13 · IF 15.7

Multivariate metal-organic frameworks enable chemical shift-encoded MRI with femtomolar sensitivity for biological systems

Zeng Qingbin,Yue Quer,Zhang Ming,Zhou Rui,Wang Zhen,Xiao Zhongyu,Yuan Yaping,Zhao Xiuchao,Jiang Weiping,Zhang Lei,Yang Yuqi,Yang Minghui,Li Haidong,Bouchard Louis-S.,Guo Qianni,Zhou Xin

Fluorescent molecules with specific target moieties are essential for histopathological analysis, but their limited tissue penetration depth makes in vivo, in situ color encoding analysis challenging. Magnetic resonance imaging (MRI) offers deep tissue penetration. When combined with chemical shift-encoded MRI reporters, it enables in vivo chemical shift encoding for biotarget imaging and analysis. These reporters require both strong signal intensity and large chemical shift window. However, conventional proton MRI reporters, with low sensitivity and a small chemical shift window, limit their in vivo applications. Here, we describe a chemical shift-encoded hyperpolarized 129 Xe MRI reporter based on the multivariate metal-organic framework, NiZn-ZIF-8, to overcome these challenges. The proposed NiZn-ZIF-8 gives distinct chemical shifts for dissolved and entrapped 129 Xe without signal interference, enhancing the 129 Xe NMR signal by 210 times compared to dissolved 129 Xe in water and biological media. This enables detection threshold at ≈ 4 fM concentrations, setting a record for the lowest concentration of xenon hosts detected in nanomaterials. Additionally, NiZn-ZIF-8 exhibits good in vivo MRI performance, allowing xenon encoding and distinction in rat lungs. NiZn-ZIF-8 represents a versatile and powerful platform for advanced molecular imaging and in vivo biomedical diagnostics.

CAS / MDL: 693-98-1
研究领域: 医学成像 · 纳米材料 · 分子成像 · 生物医学诊断 · 磁共振成像
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Real-time Cd2+ detection at sub-femtomolar level in various liquid media by an aptasensor integrated with microfluidic enrichment

Jian Zhang,Yuyu Zhang,Jayne Wu,Haochen Qi,Meiqi Zhao,Maoxiang Yi,Zhenmin Li,Lei Zheng

Cadmium ion (Cd 2+ ) is a highly toxic heavy metal pollutant with long biological half-life and strong bioaccumulation, which may cause irreversible damage to human health even at low-dose intake. Sensitive and specific detection of ultra-trace Cd 2+ is of great significance in food safety and environmental monitoring. In this work, a simple-to-use aptasensor to rapidly detect Cd 2+ in various liquid media is developed based on a DNA aptamer modified gold interdigitated electrode (IDE). Capacitance at the solid-liquid interface is utilized to reflect the change caused by adsorbed Cd 2+ . With the microfluidic enrichment by AC electrothermal (ACET) effect, Cd 2+ ions are sped up toward the IDE surface and captured by the probes instantaneously. Owing to the integration of target enrichment and capacitance detection, the sample-to-result time of this sensor is as short as 30 s. This aptasensor as a quantitative detector has a linear response range from 0.45 fM to 4.5 pM, with a limit of detection of 253.16 aM. The selectivity ratio reaches 2320: 1 against non-target metal ions. By detection of Cd 2+ spiked in tap water and olive oil as well as natural residual Cd 2+ in rice leaching solution, the sensor’s applicability and reliability in different practical liquid media are demonstrated.

研究领域: 环境科学 · 分析化学 · 食品安全 · 生物技术
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ELECTROCHIMICA ACTA · 2014 · IF 4.086

A Fetomolar Level 17β-estradiol Electrochemical Aptasensor Constructed On Hierachical Dendritic Gold Modified Boron-Doped Diamond Electrode

Hongyang Ke,Meichuan Liu,Lu Zhuang,Zhengxin Li,Lifang Fan,Guohua Zhao

It is of great significance to develop efficient monitoring strategies with high sensitivity and selectivity for 17β-estradiol (E2), a typical steroidal hormones endocrine disrupting chemicals , in water samples. Here reports a novel practical electrochemical impedance aptasensor for the detection of E2 effectively and fast. A unique hierachical dendritic gold microstructure is constructed on boron doped diamond (BDD) electrode surface through a double template method. The obtained dendritic Au/BDD electrode has lower background current, better electrochemical performance and higher capacity to immobilize biomolecules. E2 aptamers which can specifically binding to E2 were immobilized on the surface of the dendritic Au/BDD electrode through Au-S interaction, obtaining a newly-typed E2 aptasensor. The aptasensor performed supersensitive and specific recognition capacity towards E2. Once E2 enters into the detecting system, it reacts with aptamers and enlarges the interfacial electron transfer resistance significantly, which leads to the increment of impedance signal and realizes the quantification of E2. Results show that the constructed E2 aptasensor exihbits a wide linear range with the logarithm of concentration of E2 from 1.0   ×   10 −14 to 1.0   ×   10 −9   mol/L with a femtomolar level detection limit of 5.0   ×   10 −15   mol/L. High specificity is also evidenced by control experiments performed with the E2 aptasensor in a co-existing system including estriol , bisphenol A , nonyl phenol , diethyl phthalate , resorcinol and atrazine . Real water sample analysis showed the reliability and potential in practical environmental monitoring of the aptasensor. Besides, the aptasensor is easy to prepare, and the dendritic Au/BDD electrode can be a promising platform for design of other sensors.

研究领域: 分析化学 · 环境科学 · 生物化学
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Nanomedicine-Nanotechnology Biology and Medicine · 2015 · IF 6.155

Designer SiO2@Au nanoshells towards sensitive and selective detection of small molecules in laser desorption ionization mass spectrometry

Jinrui Gan,Xiang Wei,Yixin Li,Jiao Wu,Kun Qian,Baohong Liu

We report a novel platform using optimized SiO 2 @Au core–shell structures as matrices for highly efficient laser desorption/ionization mass spectrometry analysis of small biomolecules (MW   <   700   Da). Owing to the designer structure, SiO 2 @Au nanoshells can achieve low detection-of-limits (~   pmol–fmol) in mass spectrometry and selective laser desorption/ionization in bio-mixtures towards diverse small molecules. By further surface modification with aptamers , Apt-SiO 2 @Au nanoshells allowed simultaneously targeted enrichment and detection of kanamycin with a detection limit at 200   pM. Our work not only starts new applications of SiO 2 @Au nanoshells in mass spectrometry, but also contributes to advanced analysis of either a group of small molecules or one target small molecule from complex bio-samples in a pre-designed manner for bio-diagnostics. From the Clinical Editor Existing methods for the detection of small molecules are often not sensitive enough. Here, the authors developed aptamer functionalized [email protected] nanoshells for use in mass spectrometry, with very low detection limits. The new platform appeared to be simple and efficient and should be applicable in detection of clinical samples.

研究领域: 分析化学 · 质谱技术 · 生物传感器 · 纳米技术 · 临床诊断
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BIOSENSORS & BIOELECTRONICS · 2017 · IF 7.78

Proximity hybridization triggered hemin/G-quadruplex formation for construction a label-free and signal-on electrochemical DNA sensor

Fenglei Gao,Taotao Fan,Jing Wu,Sha Liu,Yan Du,Yao Yao,Fuyi Zhou,Yu Zhang,Xianjiu Liao,Deqin Geng

We describe a novel label-free and signal-on electrochemical DNA sensing platform via proximity hybridization triggered hemin/G-quadruplex formation based on the direct electron transfer of hemin . The thiolated modified G-DNA1 was first immobilized onto the Au electrode surface . In the presence of target DNA, Y-junction-structure ternary complex can be formed to trigger the proximity assembly of G-DNA1, hemin, and G-DNA2, which leads to the formation of hemin/G-quadruplex for generation an amplified electrochemical signal by differential pulse voltammetry . The observed signal gain was sufficient to achieve a demonstrated detection limit of 54 fM, with a wide linear dynamic range from 10 −13 to 10 −9 M and discriminated mismatched DNA from perfect matched target DNA with a high selectivity. Benefiting from the one step proximity dependent hemin/G-quadruplex formation, the assay method is extremely simple and can be carried out within 40   min. The advantages of free of any label conjugation step, and versatility make it a promising candidate for point-of-care testing and commercial application.

研究领域: 分析化学 · 生物化学 · 电化学 · 纳米技术 · 分子诊断
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Arabian Journal of Chemistry · 2022 · IF 6.212

Dual recognition strategy for ultra-sensitive fluorescent detection of Hg2+ at femto-molar level based on aptamer functionalized sulfur quantum dots

Xiaobin Wang,Wei Guo,Xiaoling Wang,Qing Hua,Feiyan Tang,Xin Li,Feng Luan,Zhiyang Zhang,Chunyuan Tian,Xuming Zhuang,Lijun Zhao

In the present study, a dual recognition strategy for ultrasensitive detection of Hg 2+ was successfully developed for the first time based on aptamer functionalized sulfur quantum dots (Apt-SQDs). The developed Apt-SQDs not only retained the good fluorescence properties of quantum dots but also overcame the problem of poor selectivity of SQDs for heavy metal ions. This system used the dual recognition strategy, including the combination of S x 2− and Hg 2+ and T-Hg 2+ -T structures to excellently identify and capture Hg 2+ , and an ultrahigh sensitivity fluorescent aptasensor was fabricated. The fluorescent aptasensor had a good response to Hg 2+ at concentrations ranging of 10 −15 to 10 −7 M with an ultralow limit of detection of 0.3 fM, and the response to other metal ions was far less than that to Hg 2+ . It was successfully applied to detect Hg 2+ in nearby environmental water samples (tap water, lake water and river water) with a good recovery rate. Moreover, portable test papers that would be useful for Hg 2+ monitoring in environmental water were designed. The dual recognition strategy not only achieves ultrasensitive fluorescent detection of Hg 2+ but also provides a new insight into the further expansion of the application of SQDs.

研究领域: 分析化学 · 环境科学 · 纳米技术 · 材料科学
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Amplification-Free Analysis of Bladder Cancer MicroRNAs on Wrinkled Silica Nanoparticles with DNA-Functionalized Quantum Dots

Pei Wang,Xiaowei Wei,Luming Shen,Kexin Xu,Zhongting Wen,Nengjiao Gao,Ting Fan,Shenmei Xun,Qingyi Zhu,Xiaojun Qu,Yefei Zhu

Bladder cancer (BC) occurrence and progression are accompanied by alterations in microRNAs (miRNAs) expression levels. Simultaneous detection of multiple miRNAs contributes to the accuracy and reliability of the BC diagnosis. In this work, wrinkled silica nanoparticles (WSNs) were applied as the microreactor for multiplex miRNAs analysis without enzymes or nucleic acid amplification. Conjugated on the surface of WSNs, the S9.6 antibody was adopted as the universal module for binding DNA/miRNA duplexes, regardless of their sequence. Furthermore, single-stranded DNA (ssDNA) was labeled with quantum dots (QDs) for identifying a given miRNA to form QDs-ssDNA/miRNA, which enabled the specific capture of the corresponding QDs on the wrinkled surface of WSNs. Based on the detection of fluorescence signals that were ultimately focused on WSNs, target miRNAs could be sensitively identified to a femtomolar level (5 fM) with a wide dynamic range of up to 6 orders of magnitude. The proposed strategy achieved high specificity to obviously distinguish single-base mutation sequences and possessed multiplex assay capability. Moreover, the assay exhibited excellent practicability in the multiplex detection of miRNAs in clinical serum specimens.

研究领域: 癌症生物学 · 纳米技术 · 分子诊断 · 生物医学工程
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ANALYTICAL CHEMISTRY · 2014 · IF 5.825

2-Pyridylfuran: A New Fluorescent Tag for the Analysis of Carbohydrates

Zhi Peng Cai,Andrew Kevin Hagan,Mao Mao Wang,Sabine Lahja Flitsch,Li Liu,Josef Voglmeir

We herein report the use of 1,3-di(2-pyridyl)-1,3-propanedione (DPPD) as a fluorogenic labeling reagent for sugars. Reaction of DPPD with the anomeric carbon affords a fluorescent 2-pyridylfuran (2-PF) moiety that permits the sensitive HPLC-based detection of monosaccharides. 2-PF-labeled monosaccharides can be easily separated and analyzed from mixtures thereof, and the reported protocol compares favorably with established labeling reagents such as 2-aminobenzoic acid (2-AA) and 1-phenyl-3-methyl-5-pyrazolone (PMP), ultimately allowing subfemtomole detection of the galactose-derived product. Furthermore, we demonstrate the application of DPPD in the labeling of monosaccharides in complex biological matrices such as blood and milk samples. We envisage that DPPD will prove to be an excellent choice of labeling reagent in monosaccharide and carbohydrate analysis.

研究领域: 分析化学 · 碳水化合物化学 · 生物化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Coordination-Driven Templated Synthesis of Hierarchically Porous Zeolitic Imidazolate Frameworks for Cascade Enzyme Cycle Amplification Coupled Immunoassay

Fan Xia,Jian Yang,Jingwen Chen,Ximeng Liu,Zhefan Ma,Jinlou Gu

Although hierarchically porous zeolitic imidazolate frameworks (HPZIFs) not only inherit the intrinsic architectural and chemical stabilities of their microporous counterparts but also afford open space for the efficient mass diffusion of the macromolecules involved, their rational design and construction are still challenging. Herein, HPZIFs with tailorable pore sizes ranging from 18 to 54 nm were successfully fabricated by using a newly developed soft-template-directed strategy. Our success rooted in the fact that the screened PS81–PVP44–PEO113 triblock copolymer could effectively coordinate with the metal precursor for the directed crystallization of ZIFs along surfactant assemblies. The advantages of continuous large pores and open structures in such HPZIFs were fully taken into account to serve as a bioreactor for the efficient immunoassay. The expanded large pores provided not only a significantly vast surface area to enhance the density of capture antibodies but also enough space for accommodating multiple conjugated biomolecules in one pore channel. In combination with a cascade enzyme cycle amplification strategy, a model biomarker of prostate-specific antigen (PSA) at the femtomolar level was checked with a limit of detection of 92 fM using the developed immunosensor. Specific screening on patients with prostate cancer or even benign prostatic hyperplasia was exemplified through accurately quantifying small changes of PSA concentration in clinical serum samples, prefiguring the great potential of the developed HPZIF-8 immunosensor platform for the early monitoring and diagnostics of diseases.

研究领域: 材料科学 · 分析化学 · 生物传感器 · 生物医学工程 · 纳米技术
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