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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2023 · IF 4.4

Directly and ultrasensitivity detecting SARS-CoV-2 spike protein in pharyngeal swab solution by using SERS-based biosensor

Yansheng Liu,Zhenle Qin,Xiaobo Jia,Jin Zhou,Hongli Li,Xiaohong Wang,Yating Chen,Junpeng Deng,Zhicheng Jin,Guofu Wang

The global pandemic of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has caused a great disaster to the economy and human society. Nowadays, SARS-CoV-2 is fading away from people’s memory but it still exists around us. PCR plays an important role in detecting SARS-CoV-2 but it requires a long detecting time, equipped laboratory, and professional operators. In comparison with polymerase chain reaction (PCR), surface-enhanced Raman scattering (SERS) is a promising method for detecting SARS-CoV-2 due to its fast, easily operated, and high-sensitivity properties. In this study, the monolayer Ag nanoparticles (MAgNPs) covered with single-layer graphene (SLG) are applied as a SERS substrate. The angiotensin converting enzyme 2 (ACE2) is selected as a bio-probes that can specifically bind to the SARS-CoV-2 S protein. The SERS-based biosensor is formed by ACE2 functionalized SLG/MAgNPs and the LODs of detecting SARS-CoV-2 S protein in phosphate-buffered saline (PBS) and in pharyngeal swabs solution (PSS) are 0.1 fg mL −1 and 10 fg mL −1 , respectively. This biosensor provides a way of directly detecting SARS-CoV-2 S protein with high sensitivity and specificity. It illustrates a practical potential in the rapid detection of the SARS-CoV-2 virus.

研究领域: 生物传感器 · 医学检测 · 纳米技术
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Small · 2025 · IF 12.1

DNA Locked-in Double-Faced-Nanotube for Ultrafast Biosensing of Hepatitis Virus

Xinxin Liu,Tao Liu,Xueli Yuan,Jing Zhang,Mengjiao Zhu,Wei Zhang,Zhenyu Chu,Wanqin Jin

Viral hepatitis is a highly infectious disease caused by various hepatitis viruses that, thus far, have no cure. In early viral invasion, a low viral load in the blood makes early detection difficult unless the symptoms are severe. Herein, a new ultrasensitive and ultrafast hepatitis virus detection strategy is proposed by constructing a dual-surface-activated nanotube that enables recognition probes to not only bind to the outer surface of the nanotube but also penetrate and lock onto its inner surface. This approach significantly enhances both the specific surface area and number of active sites, thereby improving the capture efficiency for traces of hepatitis viral DNA, such as the B type (HBV-DNA). Compared with current DNA detection methods, this approach eliminates the additional amplification steps to achieve an ultralow detection limit of 10 −18 m , advancing the available detection time as early as possible. Using human serum as a sample, this technique enables the precise and quantitative reporting of HBV-DNA within only 15 min and overcomes the interference of usual proteins and other viral DNA. This technique provides new inspiration for quick and early hepatitis diagnosis for in-hospital and non-hospital patients without bulky instruments and complex operations.

研究领域: 生物技术 · 医学诊断 · 分子生物学
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TALANTA · 2024 · IF 5.6

Electrochemiluminescence aptasensing method for ultrasensitive determination of lipopolysaccharide based on CRISPR-Cas12a accessory cleavage activity

Jiayue Shi,Sijia Li,Rongguang Shao,Yang Jiang,Yanxia Qiao,Jin Liu,Yaqian Zhou,Yan Li

In this study, an ultrasensitive electrochemiluminescence (ECL) aptasensing method was developed for lipopolysaccharide (LPS) determination based on CRISPR-Cas12a accessory cleavage activity. Tris (2,2'-bipyridine) dichlororuthenium (II) (Ru(bpy) 3 2+ ) was adsorbed on the surface of a glassy carbon electrode (GCE) coated with a mixture of gold nanoparticles (AuNPs) and Nafion film via electrostatic interaction. The obtained ECL platform (Ru(bpy) 3 2+ /AuNP/Nafion/GCE) exhibited strong ECL emission. Thiol-functionalized single-stranded DNA (ssDNA) was modified with a ferrocenyl (Fc) group and autonomously assembled on the ECL platform of Ru(bpy) 3 2+ /AuNP/Nafion/GCE via thiol-gold bonding, resulting in the quenching of ECL emission. After hybridization of the LPS aptamer strand (AS) with its partial complementary strand (CS), the formed double-stranded DNA (dsDNA) could activate CRISPR-Cas12a to indiscriminately cleave ssDNA-Fc on the surface of Ru(bpy) 3 2+ /AuNP/Nafion/GCE, resulting in recovery of the ECL intensity of Ru(bpy) 3 2+ due to the increasing distance between Fc and the electrode surface. The combination of LPS and AS suppressed the formation of dsDNA, inhibited the activation of CRISPR-Cas12a, and prevented further cleavage of ssDNA-Fc. This mechanism aided in upholding the integrity of ssDNA-Fc on the surface of the electrode and was combined with ECL quenching induced by the target. The ECL intensity decreased linearly as the concentration of LPS increased from 1 to 50,000 pg/mL and followed a logarithmic relationship. This method exhibited a remarkably low detection limit of 0.24 pg/mL, which meets the requirement for low-concentration detection of LPS in the human body. The proposed method demonstrates the capacity of CRISPR-Cas12a to perform non-specific cutting of single-stranded DNA and transform the resultant cutting substances into changes in the ECL signal. By amalgamating this approach with the distinct identification abilities of LPS and its aptamers, a simple, responsive, and discriminatory LPS assay was established that holds immense significance for clinical diagnosis.

CAS / MDL: 10294-29-8
研究领域: 生物传感 · 分子诊断 · 临床医学
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 16 ·9817-9829 · IF 10.7

SERS sensing chip based on Ti3C2/nano-Au@MA for ultrasensitive amine gas detection

Liwei Hou,Xinyue Xu,Xiaoli Wang,Li Wang,Fengchun Tian,Yi Xu

In this paper, we propose a composite nano-microstructure comprising Ti3C2 and nanogold as a surface-enhanced Raman spectroscopy (SERS)-active substrate for the highly sensitive sensing of amine gases. The adsorption performance of Ti3C2 was tested by a quartz crystal microbalance (QCM) sensor. Excellent adsorption ability of Ti3C2 was observed for aniline, phenylenediamine, and diethylamine, with adsorption amounts exceeding 2210, 1740, and 970 ng cm−2, respectively. The synergistic effect of the electromagnetic properties of Ti3C2 and nano-Au in the Ti3C2/nano-Au composite nanostructures was verified by finite-difference time-domain simulation. Partial chemical enhancement between Ti3C2 and aniline was verified by photocurrent tests. To achieve assay specificity, mercaptoacetaldehyde (MA) was adopted as a recognition probe. The Schiff base reaction between aldehyde groups and amino groups produces the –CN– bond, with the Raman characteristic peak at 1635 cm−1, enabling precise amine identification with the SERS chip. To obtain the Ti3C2/nano-Au@MA SERS sensing chip, nano Au was deposited on an indium tin oxide substrate using the chronoamperometric method, followed by nano-Au aldolization modification through Au-SH interactions and the spin-coating of a Ti3C2 film layer. Due to the high affinity of Ti3C2 for amine molecules and the low SERS background signal of MA and Ti3C2, the SERS spectra could be used for ultra-sensitive detection of amines. Three amine gases, i.e. aniline, p-phenylenediamine, and diethylamine, were detected quantitatively using the intensity ratiometric method on the functionalized Ti3C2/nano-Au@MA SERS sensor chip. The detection limits were 1, 1, and 20 parts per billion, respectively. By identifying the characteristic fingerprint peaks and comparing the relative intensity of the –CN– characteristic peak, quantitative analysis of the components of aniline and p-phenylenediamine mixed gas was accomplished. These findings demonstrate that the Ti3C2/nano-Au@MA SERS sensor chip offers a promising approach for the detection of amine gas molecules and holds potential for applications in environmental monitoring, disease diagnosis, and chemical analysis.

研究领域: 材料科学 · 分析化学 · 环境科学
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Ultrabright fluorescence probe mediated biosensor for rapid and ultrasensitive quantification of chloramphenicol in milk

Jiacheng Tao,Niu Feng,Yu Zhang,Yiping Chen,Zhen Zeng,Hong Jiang,Jimei Ma

The improper and excessive use of chloramphenicol has placed a heavy burden and adverse impact on the environment and human health. Herein, a fluorescent molecule with aggregation-induced emission characteristic is designed, synthesized, and encapsulated into polystyrene nanospheres, serving as an optical signaling probe in biosensors for ultrasensitive, rapid and accurate detection of chloramphenicol in milk. In this method, magnetic nanoparticles coupled with chloramphenicol antibody are used as immunomagnetic separation carriers. The polystyrene microspheres embedding aggregation-induced emission molecules are modified with complete antigen of chloramphenicol and used as stable and efficient signal probes. Chloramphenicol in sample and complete antigen modified-polystyrene microspheres are competitively bound to the immuno-magnetic carrier. The concentration is determined by the fluorescence intensity of the binding magnetic complex. This optical immunosensor presents an ultra-wide linear range (100 pg/mL–500 ng/mL), extraordinary sensitivity (limit of qualification was 100 pg/mL, 10-fold sensitive than enzyme-linked immunosorbent assay), and rapid detection speed (∼40 min). Accuracy is strong concordant with that of HPLC and ELISA in the test of milk samples. This strategy exhibits notable sensitivity, stability, specificity and reproducibility. The detection time is considerably shortened and the procedure is streamlined. It is a potential method for monitoring antibiotic contamination in a variety of settings, including the environment, food, and clinical circumstances.

研究领域: 分析化学 · 食品科学 · 环境科学
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ANALYST · 2023 ·Vol. 148 ·期 5 ·1016-1023 · IF 4.2

Rare earth upconversion luminescent composite based on energy transfer for specific and sensitive detection of cysteine

Yulian Zhu,Xiaomei Guo,Xiao Ma,Kai Liu,Yuting Han,Yongquan Wu,Xun Li

Abnormal levels of thiols in cysteine (Cys) have been shown to be associated with growth retardation, skin lesions, and neurotoxicity in humans. Herein, we designed and synthesized a rare earth upconversion luminescent (UCL) nanocomposite probe UCNP–PEG–NOF1 for the UCL detection of Cys using NOF1 developed by our group as a Cys probe. The core structure of rare earth nanoparticles can absorb light at 980 nm and convert it into visible light. The detection principle of Cys was based on the change in absorption peak before and after the reaction between NOF1 and Cys, as well as the change in UCL intensity. The rare earth nanocomposite in the probe could be excited by near-infrared light and had low background fluorescence and strong penetration ability; thus, the probe was successfully employed to specifically and sensitively detect Cys with a low background signal. Overall, the developed UCNP–PEG–NOF1 probe had good selectivity and high sensitivity for Cys; its detection limit was as low as 83 nM.

研究领域: 分析化学 · 生物化学 · 纳米技术
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TALANTA · 2018 · IF 4.244

Ultrasensitive detection of thiophenol based on a water-soluble pyrenyl probe

Zhiyi Yao,Wenqi Ge,Mingwei Guo,Keren Xiao,Yadong Qiao,Zhong Cao,Hai-Chen Wu

We report a simple pyrene-based fluorescent probe , sodium 8-(2,4-dinitrophenoxy)pyrene-1,3,6-trisulfonate (HPTS-DNP), for the ultrasensitive and visual detection of thiophenol in 100% aqueous media. The sensing mechanism of this method is based on nucleophilic aromatic substitution on HPTS-DNP caused by thiophenol to afford a highly fluorescent product, 8-hydroxypyrene-1,3,6-trisulfonic acid trisodium salt (HPTS). The extremely low fluorescence background of HPTS-DNP and high quantum yield of HPTS ensure the superior sensing performance toward thiophenol, including rapid responses, off-on detection mode and excellent sensitivity. The detection limit is as low as 0.49 nmol L −1 according to the measurements with a spectrofluorimeter. This probe also features good selectivity (response ratio of thiophenol to interferents >30), precision (2.93%) and accuracy (102%). This approach could be applied for monitoring the thiophenol concentrations in environmental water samples. HPTS-DNP also showed good cell permeation capacity and low cellular cytotoxicity, indicating further application in bioimaging studies.

研究领域: 分析化学 · 环境科学 · 生物医学
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ANALYST · 2014 ·Vol. 140 ·期 4 ·1046-1053 · IF 3.906

β-Cyclodextrin functionalised gold nanoclusters as luminescence probes for the ultrasensitive detection of dopamine

Rui Ban,E. S. Abdel-Halim,Jianrong Zhang,Jun-Jie Zhu

A novel luminescence probe based on mono-6-amino-β-cyclodextrin (NH2-β-CD) functionalised gold nanoclusters (β-CD-AuNC) was designed for dopamine (DA) detection. The NH2-β-CD molecules were conjugated onto the surface of 11-mercaptoundecanoic acid capped AuNCs (11-MUA-AuNC) via a carbodiimide coupling reaction. The integrity of the β-CD cavities was preserved on the surface of AuNCs and they retained their capability for molecular DA host–guest recognition. DA could be captured by the β-CD cavities to form an inclusion complex in which the oxidised DA could quench the fluorescence of the β-CD-AuNC probe by electron transfer. The probe could be used to quantify DA in the range of 5–1000 nM with a detection limit of 2 nM. This sensitivity was 1–2 orders of magnitude higher than that in previously reported methods. Interference by both ascorbic acid (AA) and uric acid (UA) was not observed. Therefore, the β-CD-AuNC probe could be directly used to determine the DA content in biological samples without further separation. This strategy was successfully applied to a DA assay in spiked human serum samples and it exhibited remarkable accuracy, sensitivity and selectivity.

研究领域: 分析化学 · 生物医学 · 材料科学
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MOLECULES · 2024 ·Vol. 29 ·期 12 ·2906 · IF 4.2

Magnetic Titanium Dioxide Nanocomposites as a Recyclable SERRS Substrate for the Ultrasensitive Detection of Histidine

Hailin Wen,Miao Li,Chao-Yang Zhao,Tao Xu,Shuang Fu,Huimin Sui,Cuiyan Han

A highly sensitive, selective and recyclable histidine detection method based on magnetic Fe3O4@mTiO2(M-TiO2) nanocomposites with SERRS was developed. Mesoporous M-TiO2nanoparticles were functionalized with 4-aminothiophenol and then coupled with histidine through an azo coupling reaction in 5 min, producing the corresponding azo compound. The strong and specific SERRS response of the azo product allowed for ultrasensitive and selective detection for histidine with an M-TiO2device loaded with Ag NPs due to the molecular resonance effect and plasmonic effect of Ag NPs under a 532 nm excitation laser. The sensitivity was further enhanced with the magnetic enrichment of M-TiO2. The limit of detection (LOD) was as low as 8.00 × 10−12mol/L. The M-TiO2demonstrated applicability towards histidine determination in human urine without any sample pretreatment. Additionally, the M-TiO2device can be recycled for 3 cycles with the photodegradation of the azo product under UV irradiation due to TiO2-assisted and plasmon-enhanced photocatalysis. In summary, a multifunctional and recyclable M-TiO2device was synthesized based on azo coupling and SERRS spectroscopy for ultra-sensitive and specific histidine sensing. In addition, the proposed system demonstrated the potential for the multiplex determination of toxic compounds in the fields of food safety, industrial production and environmental protection, which benefit from the fingerprint property and universality of SERRS.

研究领域: 生物化学 · 分析化学 · 材料科学
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BIOSENSORS & BIOELECTRONICS · 2015 · IF 6.409

Label-free, sensitivity detection of fibrillar fibrin using gold nanoparticle-based chemiluminescence system

Yuanfu Zhang,Jifeng Liu,Ting Liu,Haibo Li,Qingwang Xue,Rui Li,Lei Wang,Qiaoli Yue,Shuhao Wang

A novel, label-free, gold nanoparticles (AuNPs)-based chemiluminescence assay has been developed for the detection of fibrillar fibrin. The method relied on the interaction of fibrinogen (Fib) with AuNPs and the aggregated AuNPs induce a strong luminol–H 2 O 2 chemiluminesecence (CL) signal. We prepared the 12-nm-diameter AuNPs which well dispersed in the solution. Fib was absorbed on the surface of AuNPs against the aggregation of AuNPs in 1.0   M NaCl. Otherwise, Fib was catalyzed to form fibrillar fibrin in the presence of thrombin. The fibrin induced AuNPs aggregated in the presence of NaCl solution. The catalytic activity of aggregated AuNPs on the luminol–H 2 O 2 CL reaction is greatly enhanced. This allows us to utilize the luminol–H 2 O 2 CL system for quantitative analysis of thrombin, which was used to denote fibrosis degree of Fib. The assay showed a linear toward fibrillar fibrin concentration in the range of 2.7×10 −15 –2.7×10 −13   M with a correlation of 0.9920. The limit of detection for fibrin was experimentally determined to be 1   fM, based on a signal-to-noise ratio ( S / N ) of 3. Relative to conventional methods, this method offers the advantages of higher sensitivity and selectivity and lower cost, showing great potential for medical diagnosis.

CAS / MDL: 16940-66-2 68-04-2
研究领域: 生物化学 · 医学诊断
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iScience · 2021 · IF 5.458

Ultrasensitive molecular building block for biothiol NMR detection at picomolar concentrations

Qingbin Zeng,Qianni Guo,Yaping Yuan,Baolong Wang,Meiju Sui,Xin Lou,Louis-S. Bouchard,Xin Zhou

Magnetic resonance imaging (MRI) provides structural and functional information, but it did not probe chemistry. Chemical information could help improve specificity of detection. Herein, we introduce a general method based on a modular design to construct a molecular building block Xe probe to help image intracellular biothiols (glutathione (GSH), cysteine (Cys) and homocysteine (Hcy)), the abnormal content of which is related to various diseases. This molecular building block possesses a high signal-to-noise ratio and no background signal effects. Its detection threshold was 100 pM, which enabled detection of intracellular biothiols in live cells. The construction strategy can be easily extended to the detection of any other biomolecule or biomarker. This modular design strategy promotes efficiency of development of low-cost multifunctional probes that can be combined with other readout parameters, such as optical readouts, to complement 129 Xe MRI to usher in new capabilities for molecular imaging.

研究领域: 生物化学 · 医学影像 · 分子生物学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Electrochemical-Enhanced Charge State Modulation of Nitrogen-Vacancy Centers for Ultrasensitive Biodetection of MicroRNA-155

Xiaojian Fan,Youqiang Xing,Ze Wu,Bingjue Li,Peng Huang,Lei Liu

Sensitive and accurate miRNA detection is important in cancer diagnosis but remains challenging owing to the essential features of miRNAs, such as their small size, high homology, and low abundance. This work proposes a novel electrochemical (EC)-enhanced quantum sensor achieving quantitative detection of miRNA-155 with simultaneous EC sensing. Specifically, fluorescent nanodiamonds/MXene nanocomposites were synthesized and modified with dual-mode signal labels, enabling miRNA-155 concentration measurement via T1 relaxation time of nitrogen-vacancy (NV) centers and EC signals. Quantum sensing was enhanced via external voltage during the EC process, which modulated the negatively charged state of the NV centers, thereby improving the sensitivity and accuracy of miRNA-155 detection. EC sensing improved the accuracy and reliability of miRNA-155 detection while enhancing quantum sensing. The limit of detection (LOD) of the EC-enhanced quantum biosensor reached 10.0 aM, nearly 106 and 10 times lower than the reported LODs of a quantum sensor using bulk diamond and fluorescent sensors, respectively. The LOD of EC sensing was 2.6 aM, aligning with previous reports. The findings of the study indicated that quantum sensing combined with EC sensing can achieve ultrasensitive miRNA-155 detection with high accuracy and reliability, providing an advanced approach for early cancer diagnosis.

CAS / MDL: 7758-94-3
研究领域: 生物医学工程 · 分子生物学 · 纳米技术
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