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ACS Sensors · 2022 · IF 9.618

High-Throughput Surface-Enhanced Raman Scattering for Screening Chemical Sensor Candidates Enabled by Bipolar Electrochemistry

Sanjun Fan,Xinyu Wang,Yingling Li,Xiaofeng Chen,Haotian Chen,Zachary D. Schultz,Zheng Li

A variety of hydrothermal or electrochemical methods have been explored to prepare noble metal nanostructures as surface-enhanced Raman scattering (SERS) substrates. However, most of those metallic nanoarrays are structurally homogeneous, which makes it laborious to select the high-performance substrates for particular Raman sensing purposes. Here, a high-throughput SERS imaging strategy is demonstrated for the first time for screening chemical sensors with sub-nanomolar sensitivities. Bipolar electrochemistry was applied to generate Au or Au–Ag gradient nanoarrays with diverse chemical compositions, morphologies, and particle dimensions ranging from several nanometers to micrometers. The selected “hot-spots” on the Au–Ag alloy nanoarray exhibited a 660-fold enhancement in SERS intensity compared to those on the pure Au gradient nanoarray. The SERS screening of 4-aminothiophenol, 4-nitrothiophenol, and 4-mercaptobenzoic acid was carried out that provided a limit of detection (LOD) between 1 and 5 pM. The distinctive LODs among three thiophenolic Raman probes are ascribed to the differences in the affinity of the probe to the alloy, orientation of the metal–ligand monolayer, or plasmonic environment of the nanoarray surface. As a continuous, rapid, and cost-effective manner to fabricate transitional nanostructures and screen out SERS responsive sites, this method not only facilitates controllable synthesis of noble metal nanoarrays but has the potential to provide an alternative tool for ultrasensitive chemical sensing on a wide range of bimetallic substrates.

CAS / MDL: 64-17-5 7761-88-8
研究领域: 分析化学 · 材料科学 · 电化学 · 纳米技术 · 光谱学
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MICROCHIMICA ACTA · 2019 ·Vol. 186 ·期 7 ·1-8 · IF 5.479

Surface-enhanced Raman spectroscopic single step detection of Vibrio parahaemolyticus using gold coated polydimethylsiloxane as the active substrate and aptamer modified gold nanoparticles

Wu Shijia,Duan Nuo,Shen Mofei,Wang Jing,Wang Zhouping

A method is described for single-step detection of V. parahaemolyticus in seafood via aptamer-based SERS. A gold-coated polydimethylsiloxane (PDMS) film was used for the enhancement of Raman scattering. The Raman reporter 4-mercaptobenzoic acid was linked to aptamer modified gold nanoparticles (AuNPs) served as a signalling probe. The negatively charged signalling probe was assembled onto the cysteamine-modified Au-PDMS film through electrostatic adsorption. On addition of V. parahaemolyticus , it will be bound by the aptamer as a biorecognition element, and this leads to the dissociation of the signalling probe from the Au-PDMS film. Hence, the Raman signal (at 1592 cm −1 ) decreases. The assay has a wide linear response that covers the 1.2 × 10 2 to 1.2 × 10 6  cfu·mL −1   V. parahaemolyticus concentration range. The detection limit is 12 cfu·mL −1 . The method was successfully applied to the determination of V. parahaemolyticus in oyster and salmon samples. Schematic presentation of a surface-enhanced Raman spectroscopic method for single step detection of Vibrio parahaemolyticus using gold coated polydimethylsiloxane as the active substrate and aptamer modified gold nanoparticles. This solid substrate simplified the analysis procedures and enhanced the sensitivity.

CAS / MDL: 1074-36-8
研究领域: 分析化学 · 微生物学 · 食品科学
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OPTICS EXPRESS · 2019 ·Vol. 27 ·期 17 ·23981-23995 · IF 3.561

Core-shell Au@Ag nanodendrites supported on TiO2 nanowires for blue laser beam-excited SERS-based pH sensing

Anxin Jiao,Hua Zhang,Linlin Xu,Yue Tian,Xiangdong Liu,Ming Chen,Feng Chen

The blue laser beam-excited surface-enhanced Raman scattering (SERS)-based pH sensing holds great promise for avoiding undesired thermal heating effect on some special temperature-vulnerable molecules, as compared to the vast majority studies by exciting in the red or near-infrared (NIR). Herein, we report an ingenious approach to support core-shell Au@Ag nanodendrites (NDs) on TiO2 nanowires, which can possess enhanced SERS activity under 473 nm laser excitation, owing to the improved charge-transfer effect on modified TiO2 support by inserting plasmonic Au@Ag. By using pH-indicating 4-mercaptobenzoic acid (4-MBA), the obtained TiO2/Au@Ag NDs can not only exhibit high sensitive linear-responses of pH changes ranging from pH 4.0 to 9.0 in different solutions (deionized water, NaCl, CaCl2, and MgCl2) but also provide excellent temperature stability under 4°C, 25°C and 37°C temperatures as well as good time stability after storage for 10 days. The established SERS-pH sensing by using shorter wavelength laser excitation is highly desirable for understanding physiological process in temperature-vulnerable microenvironment.

研究领域: 材料科学 · 分析化学 · 纳米技术 · 光学
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Journal of Physical Chemistry C · 2023 · IF 3.7

Detection of Oxytetracycline on NH2–UiO-66(Zr)@Au NPs with High Sensitivity and Selectivity by SERS

Huan-Yu Chen,Xing-Biao Liu,Qi-Xin Guan,Can-Jun Zou,Ping-Ping Fang

The detection of antibiotics has attracted great attention among scientists and health researchers in the past decades. However, it is still difficult to realize the sensitive and selective detection of antibiotics with similar structures. Herein, the antibiotic molecules of oxytetracycline (OTC) can be sensitively and selectively detected by surface-enhanced Raman spectroscopy (SERS) on NH2–UiO-66(Zr)@Au nanoparticles (NPs). The SERS substrate of NH2–UiO-66(Zr)@Au NPs realizes a detection sensitivity of 1 × 10–12 g·L–1 for 4-mercaptobenzoic acid, indicating its high SERS activity. A high detection sensitivity of 10–11 g·L–1 is obtained for OTC on such a SERS substrate. Besides the high sensitivity, NH2–UiO-66(Zr)@Au NPs can also selectively detect OTC from streptomycin sulfate, salicylic acid, and ofloxacin by SERS on NH2–UiO-66(Zr)@Au NPs, with a selective detection limit of 10–10 g·L–1. Furthermore, OTC can be selectively detected in a real sample of river water with a detection limit of 1.0 × 10–10 g·L–1. Therefore, this study provides an effective way to enrich and detect antibiotics in real samples in the environment.

CAS / MDL: 7699-43-6
研究领域: 分析化学 · 环境科学 · 材料科学 · 纳米技术
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ACS Omega · 2020 · IF 2.87

Highly Sensitive Surface-Enhanced Raman Spectroscopy Substrates of Ag@PAN Electrospinning Nanofibrous Membranes for Direct Detection of Bacteria

Yan Yang,Zhijie Zhang,Menghui Wan,Zhihua Wang,Yanbao Zhao,Lei Sun

Surface-enhanced Raman spectroscopy (SERS) can be applied for biological detection because of its high sensitivity and noninvasiveness for analytes. Herein, we engineer plasmonic free-standing substrates composed of Ag nanoparticles (NPs) supported on polyacrylonitrile (PAN) electrospinning nanofibrous felts as sensors for bacterial detection. Ag NPs are evenly distributed on PAN nanofibers after preimpregnation and impregnation of PAN nanofibers in Tollens’ reagent. The size and loading density of Ag NPs are tunable by adjusting the reaction time of glucose and Tollens’ reagent, thereby allowing the tuning of the surface plasmon resonance. Using 4-mercaptophenol (4-MPh) and 4-mercaptobenzoic acid (4-MBA) as probe molecules, SERS effects of Ag@PAN composite nanofibers are investigated, and the substrates allow the detection of 4-MPh and 4-MBA at a low concentration of 10–9 mol/L. Importantly, the substrates exhibit a high sensitivity of SERS performance for bacterial identification without a specific bacteria–aptamer conjugation. The SERS substrates also show good uniformity of SERS response for bacterial organelles. Furthermore, the antimicrobial property was evaluated, and the results indicate that the sample of Ag@PAN nanofiber mats possesses excellent antibacterial properties against Escherichia coli and Staphylococcus aureus.

研究领域: 材料科学 · 分析化学 · 生物传感器 · 纳米技术
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2020 · IF 4.389

Receptor-mediated photothermal/photodynamic synergistic anticancer nanodrugs with SERS tracing function

Ping Tang,Meishuang Xing,Xinyue Xing,Qiao Tao,Wendai Cheng,Shengde Liu,Xiaoxu Lu,Liyun Zhong

Phototherapy, especially the photothermal therapy (PTT) and the photodynamic therapy (PDT), have become very promising in cancer treatment due to its low invasiveness and high efficacy. Both PTT and PDT involve the utilization of light energy, and their synergistic treatment should be a good solution for cancer treatment by ingenious design. The therapeutic effect of phototherapy is closely associated with the amount and location of anticancer-nanodrugs accumulated in tumor cells, and the receptor-mediated endocytosis should be an excellent candidate for enhancing anticancer-nanodrugs internalization. Surface enhanced Raman spectroscopy (SERS) imaging is suitable for tracing nanodrugs due to its high selectivity, sensitivity and reliability. In this paper, we hope to construct a receptor-mediated PTT/PDT synergistic anticancer nanodrugs and evaluate the corresponding efficacy through SERS tracing function. Here, the receptor-mediated PTT/PDT synergistic anticancer nanodrugs are prepared by the chemical modification of gold nanorods (GNRs), involving protoporphyrin IX (PpIX), 4-mecaptobenzoic acid (MBA), and folic acid (FA). The achieved results show that the receptor-mediated endocytosis can greatly facilitate the internalized amount and intracellular distribution of the nanodrugs, thus lead to the anti-cancer efficacy improvement. Importantly, this receptor-mediated PTT/PDT synergistic treatment with SERS tracing function will provide a simple and effective strategy for the design and application of anticancer phototherapy nanodrugs.

CAS / MDL: 59-30-3
研究领域: 癌症治疗 · 纳米技术 · 生物医学工程 · 光学成像
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ANALYST · 2019 ·Vol. 144 ·期 16 ·4841-4847 · IF 4.019

Monitoring 2,3′,5,5′-tetrachlorobiphenyl with a rapid and sensitive environmental aptamer sensor

Siyao Liu,Qianqian Chen,Zhiming Wang,Tongcheng Cao,Guohua Zhao,Yongxin Zhou

Polychlorinated biphenyl (PCB) detection in the environment is significant for both environmental protection and human health. Herein, a highly sensitive aptamer sensor has been established by employing a 2,3′,5,5′-tetrachlorobiphenyl (PCB72) targeting aptamer as a highly specific recognition element and a gold/silver (Au@Ag) nanocomposite as the surface-enhanced Raman spectroscopy (SERS) substrate for detecting environmental PCB72. The Au@Ag nanoparticles (NPs) exhibit a strong SERS enhancement and provide an efficient substrate for immobilizing the PCB72 aptamer and Raman signal labelled molecule, 4-mercaptobenzoic acid (4-MBA). The targeted PCB72 could competitively bind with the PCB72 aptamer, resulting in a few aptamers sticking to the Au@Ag NPs and the “hot spot” strengthening effect of the substrate. Under optimal conditions, this aptamer sensor exhibits great performance with high sensitivity, excellent selectivity and stability for the monitoring of PCB72, which shows an excellent linear correlation ranging from 1 to 1000 pg mL−1 with a limit of detection of 0.3 pg mL−1. Furthermore, this aptamer assay exhibits high specificity and selectivity for PCB72 with the detection error of less than 0.27 for other PCBs and 0.21 for other interfering species, even if the coexisting interferents are 100-fold concentration in the system. Additionally, the recognition mechanism of the binding of aptamers to PCB72 is analyzed via UV-vis spectroscopy and molecular docking simulations, which suggest that PCB72 could insert into the aptamers. Furthermore, this method is successfully utilized for PCB72 detection in real water samples with a simple pre-treatment. In general, this work provides a new and effective method using an environmental aptamer sensor for rapid and sensitive PCB72 detection.

研究领域: 环境科学 · 分析化学 · 纳米技术 · 毒理学
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ANALYST · 2021 ·Vol. 146 ·期 9 ·3016-3024 · IF 4.616

A multimer-based SERS aptasensor for highly sensitive and homogeneous assay of carcinoembryonic antigens

Tian Lu,Liping Wang,Yuhong Xia,Yang Jin,Liying Zhang,Shuhu Du

Carcinoembryonic antigens (CEAs) are known as one of the most common tumor markers. Their facile and affordable detection is critical for early diagnosis of malignant tumors, especially in resource-constrained settings. Here, we report a novel multimer-based surface-enhanced Raman scattering (SERS) aptasensor for a specific CEA assay. The aptasensor is fabricated through aptamer-assisted self-assembly of silver-coated gold nanoparticles (Au@Ag NPs), and the self-assembled multimeric structure possesses abundant hot-spots to provide high SERS response. When CEA is introduced, the specific recognition of CEA by aptamers will lead to the disassembly of Au@Ag multimers due to the lack of a bridging aptamer between Au@Ag NPs. As a result, the number of hot-spots in the multimeric system is decreased, and the intensity at 1585 cm−1 of the SERS reporter (4-mercaptobenzoic acid, 4-MBA) on the surface of NPs will also be decreased. The Raman intensity is proportional to the logarithm of the concentration of CEA. The detection sensitivity can be down to the pg mL−1 level. The analytical method only needs a droplet of 2 μL of sample, and the detection time is less than 20 min. The multimer-based SERS aptasensor can be applied in sensitive and inexpensive detection of CEA in serum samples.

CAS / MDL: 51805-45-9
研究领域: 分析化学 · 纳米技术 · 生物传感器 · 癌症诊断
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Surfaces and Interfaces · 2023 · IF 6.2

SERS sensor with rapid and quantitative detection low back pain application

Qianwen Yue,Cai Wang,Ke Zhang,Huiyu Wan,Baoliang Sun,Jingguo Wu,Jingyi Sun,Ying Wang

Thoracolumbar fascia (TLF) plays an important role in the biomechanics of the spine. TLF often causes low back pain (LBP), leading to limb movement disorders and numbness. At present, the clinical diagnosis mainly depends on doctors' clinical experience and magnetic resonance imaging. In order to make the diagnosis more convenient and accurate, we designed a "sandwich" biosensor based on surface-enhanced Raman scattering (SERS) to detect C-reactive protein (CRP) and serum amyloid A (SAA) in fascia. In this study, Ag nanocubes (AgNCs) were used as the substrate, so that the antibodies of CRP and SAA were modified on the substrate surface. Then substrate combined with antigen to form the bottom layer of the sandwich. 4-Mercaptobenzoic acid (4-MBA) and Nairn blue chloride (NBA) were used as signalling molecule probes. Hollow gold nanoparticles (HGNPs) modified with (EDC / NHS) enabled the attachment of antibodies to CRP and SAA to the surface of HGNPs. Eventually, the complex formed by the antigen-antibody reaction reacted with the sandwich substrate after the modification reaction to form the final "sandwich" structure. We successfully applied it to the specific detection of inflammatory markers in fascial tissue of TLF. The results showed that it had high stability and repeatability, which can bring some help for clinical work.

研究领域: 生物传感器 · 医学诊断 · 纳米技术 · 炎症标志物
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Surface-Roughened SERS-Active Single Silver Nanowire for Simultaneous Detection of Intracellular and Extracellular pHs

Leyi Fang,Xiao-Tong Pan,Kang Liu,Dechen Jiang,Deju Ye,Li-Na Ji,Kang Wang,Xing-Hua Xia

The simultaneous and accurate detection of intracellular pH (pHi) and extracellular pH (pHe) is essential for studying the complex physiological activities of cancer cells and exploring pH-related therapeutic mechanisms. Here, we developed a super-long silver nanowire-based surface-enhanced Raman scattering (SERS) detection strategy for simultaneous sensing of pHi and pHe. A surface-roughened silver nanowire (AgNW) with a high aspect ratio is prepared at a nanoelectrode tip using a Cu-mediated oxidation process, which is then modified by pH-sensitive 4-mercaptobenzoic acid (4-MBA) to form 4-MBA@AgNW as a pH sensing probe. With the assistance of a 4D microcontroller, 4-MBA@AgNW is efficient in simultaneously detecting pHi and pHe in both 2D and 3D culture cancer cells by SERS, with minimal invasiveness, high sensitivity, and spatial resolution. Further investigation proves that the surface-roughened single AgNW can also be used in monitoring the dynamic variation of pHi and pHe of cancer cells upon stimulation with anticancer drugs or under a hypoxic environment.

研究领域: 纳米技术 · 生物医学工程 · 癌症研究 · 分析化学
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FOOD CONTROL · 2024 · IF 5.6

Au@Ag core-shell nanorods enhance surface-enhanced Raman scattering aptasensor for ultrasensitive detection of Salmonella Typhimurium

Xiangyu Song,Huhu Wang,Xuefei Shao,Xiaobo Yu,Xinglian Xu

Salmonella Typhimurium is the prevalent pathogenic bacterium that causes foodborne-related diseases. Here, we developed a surface-enhanced Raman scattering (SERS) biosensor for S . Typhimurium detection. The biosensor was based on Au@Ag core-shell nanorods (Au@Ag NRs) to enhance Raman signal and aptamer-specific identification. 4-mercaptobenzoic acid (4-MBA) and aptamer-modified Au@Ag NRs were used as Raman signal probes. The aptamer adsorbed on the Au@Ag NRs surface when the reaction system was free of bacteria. Once S . Typhimurium was added, the aptamer then specifically identified and captured the cells. The decrease of free aptamers in solution restoring the SERS “hot spot” between the Au@Ag NRs and enhancing the 4-mercaptobenzoic acid (4-MBA) Raman signal. Quantitative analysis of S . Typhimurium was performed using Raman-enhanced spectroscopy. Under optimised conditions, the 4-MBA SERS intensity at 1072 cm −1 was used to determine S . Typhimurium in the range of 10 2 –10 7  CFU mL −1 (y = 1660.84x+2340.7, R 2  = 0.9912). The limit of detection was 64 CFU mL −1 . This method also has high specificity and is not interfered by the other five control bacteria to complete the detection of S . Typhimurium. The developed method is simple, rapid, sensitive and specificity, which can be used to detect actual samples. It can be potentially used for detecting bacteria.

CAS / MDL: 50-81-7 68-04-2
研究领域: 纳米技术 · 分析化学 · 生物传感器 · 食品安全 · 微生物学
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SENSORS · 2019 ·Vol. 19 ·期 23 ·5152 · IF 3.031

Synthesis of MBA-Encoded Silver/Silica Core-Shell Nanoparticles as Novel SERS Tags for Biosensing Gibberellin A3 Based on Au@Fe3O4 as Substrate

Qingmin Wei,Jianjuan Lin,Fa Liu,Changchun Wen,Na Li,Guobao Huang,Zhihui Luo

A surface-enhanced Raman scattering (SERS) tag is proposed for high-sensitivity detection of gibberellin A3(GA3). Silver nanoparticles (AgNPs) were synthesized using citrate reduction. 4-Mercaptobenzoic acid (MBA) was used for the Raman-labeled molecules, which were coupled to the surface of the AgNPs using sulfydryls. MBA was coated with silica using the Stöber method to prevent leakage. GA3antibodies were attached via the active functional groups N-Hydroxysuccinimide (NHS) and N-Ethyl-N’-(3-dimethylaminopropyl)carbodiimide hydrochloride (EDC) to construct a novel[email protected]2SERS tags. The captured SERS substrates were fabricated through Fe3O4nanoparticles and gold nanoparticles (AuNPs) using chemical methods. These nanoparticles were characterized using ultraviolet-visible spectroscopy (UV–Vis), dynamic light scattering, Raman spectroscopy, transmission electron microscope (TEM), and X-ray diffraction (XRD). This[email protected]2SERS tags has a strong SERS signal based on characterizations via Raman spectroscopy. Based on antigen-antibody reaction, the[email protected]3O4nanoparticles can capture the GA3and[email protected]2SERS tags. Due to the increasing number of captured nanoprobes, the SERS signal from MBA was greatly enhanced, which favored the sensitive detection of GA3. The linear equation for the SERS signal was y = −13635x + 202211 (R2= 0.9867), and the limit of detection (LOD) was 10−10M. The proposed SERS tags are also applicable for the detection of other food risk factors.Keywords:surface-enhanced Raman scattering;[email protected]2core-shell nanoparticles;[email protected]3O4nanoparticle;gibberellin

研究领域: 分析化学 · 纳米技术 · 生物传感器 · 植物科学
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