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High Performance Integrated Biosensors Based on SERS

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A special issue of Biosensors (ISSN 2079-6374). This special issue belongs to the section "Optical and Photonic Biosensors".

Deadline for manuscript submissions: closed (31 December 2023) | Viewed by 22261

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Special Issue Editors

Prof. Dr. Shunbo Li

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Guest Editor

College of Optoelectronic Engineering, Chongqing University, Chongqing, China
Interests: microfluidics and nanofluidics; biosensors; SERS
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Yuling Hu

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Guest Editor

School of Chemistry, Sun Yat-sen University, Guangzhou 510006, China
Interests: chromatographic analysis; surface-enhanced Raman spectroscopy; development of functional separation media, food and drug analysis
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Jinbo Wu

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Guest Editor

Materials Genome Institute of Shanghai University, Shanghai University, Shanghai, China
Interests: droplet microfluidics; biosensors; soft matter

Special Issue Information

Dear Colleagues,

For almost 100 years, the Raman scattering effect has been reported on, recently attracting increasingly more interest due to the development of nanotechnology to greatly enhance the scattering signal through the plasmonic resonance of nanoparticles, the enhanced technology having been termed “Surface-Enhanced Raman Spectroscopy, (SERS)”. SERS has been widely used in biosensors due to its fast detection, high sensitivity, good selectivity, multiplexing and absence of interference in water. Countless biomolecules have been detected by SERS, showing great promise in applications in biosensors for real sample detection. However, complex real samples (e.g., whole blood) always experience significant interferences between entities, since each biomolecule has its own spectrum and peak overlaps are likely to appear. This Special Issue plans to focus on the recent progress in the design of high-performance integrated biosensors based on SERS, for instance, the reliable preparation of low-cost and uniform SERS substrates, the design of sensitive SERS nanotags/probes to increase sensitivity and selectivity and, finally, the new data analysis method used to distinguish the spectra and design of integrated systems, including sample pretreatment, target separation and analyte preconcentrations before the SERS detection of biomolecules and microbes.

Prof. Dr. Shunbo Li
Prof. Dr. Yuling Hu
Prof. Dr. Jinbo Wu
Guest Editors

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Keywords

SERS
biosensor
high performance
nanoparticles
integrated systems

Published Papers (11 papers)

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Research

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11 pages, 5795 KiB

Open AccessArticle

A Three-Dimensional Hydrophobic Surface-Enhanced Raman Scattering Sensor via a Silver-Coated Polytetrafluoroethylene Membrane for the Direct Trace Detection of Molecules in Water

by Guanwei Tao, Jiajun Li, Yunyun Mu and Xinping Zhang

Biosensors 2024, 14(2), 88; https://doi.org/10.3390/bios14020088 - 05 Feb 2024

Viewed by 1107

Abstract

We report a three-dimensional (3D) SERS substrate consisting of a silver nanoparticle (AgNP) coating on the skeleton-fiber surfaces of a polytetrafluoroethylene (PTFE) membrane. Simple thermal evaporation was employed to deposit Ag onto the PTFE membrane to produce grape-shaped AgNPs. The 3D-distributed AgNPs exhibit not only strong localized surface plasmon resonance (LSPR) but also strong hydrophobic performance. High-density hotspots via silver nano-grape structures and nanogaps, the large 3D interaction volume, and the large total surface area, in combination with the hydrophobic enrichment of the specimen, facilitate high-sensitivity sensing performance of such a SERS substrate for the direct detection of low-concentration molecules in water. An enhancement factor of up to 1.97 × 10¹⁰ was achieved in the direct detection of R6G molecules in water with a concentration of 10⁻¹³ mol/L. The lowest detection limit of 100 ppt was reached in the detection of melamine in water. Such a SERS sensor may have potential applications in food-safety control, environmental water pollution monitoring, and biomedical analysis. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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10 pages, 2922 KiB

Open AccessArticle

Colorimetric Sensing of the Peroxide Number of Milk Powder Using CsPbBr₃ Perovskite Nanocrystals

by Li Zhang, Yimeng Zhu, Zhiyong Guo, Longjie You, Chen Zhang and Xi Chen

Biosensors 2023, 13(4), 493; https://doi.org/10.3390/bios13040493 - 20 Apr 2023

Cited by 1 | Viewed by 1230

Abstract

In this study, a wavelength-shift-based colorimetric sensing approach for the peroxide number of milk powder using CsPbBr₃ perovskite nanocrystals (CsPbBr₃ NCs) has been developed. Through the fat extraction, REDOX reactions and halogen exchange, as well as the optimized experimental conditions, a colorimetric sensing method was established to determine the peroxide number of milk powder samples. The integrated process of milk powder fat extraction and the REDOX process greatly shortened the determination time. This colorimetric method has a good linear correlation in the range of the peroxide number from 0.02 to 1.96 mmol/kg, and the detection limit was found to be 3 μmol/kg. This study further deepens the application prospect of wavelength-shift-based colorimetric sensing using CsPbBr₃ NCs. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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12 pages, 3073 KiB

Open AccessArticle

Engineering a SERS Sensing Nanoplatform with Self-Sterilization for Undifferentiated and Rapid Detection of Bacteria

by Jun Cao, Wei Zhu, Ji Zhou, Bai-Chuan Zhao, Yao-Yu Pan, Yong Ye and Ai-Guo Shen

Biosensors 2023, 13(1), 75; https://doi.org/10.3390/bios13010075 - 01 Jan 2023

Cited by 1 | Viewed by 1683

Abstract

The development of a convenient, sensitive, rapid and self-sterilizing biosensor for microbial detection is important for the prevention and control of foodborne diseases. Herein, we designed a surface-enhanced Raman scattering (SERS) sensing nanoplatform based on a capture–enrichment–enhancement strategy to detect bacteria. The gold−Azo@silver−cetyltrimethylammonium bromide (Au−Azo@Ag−CTAB) SERS nanotags were obtained by optimizing the synthesis process conditions. The results showed that the modification of CTAB enabled the nanotags to bind to different bacteria electrostatically. This SERS sensing nanoplatform was demonstrated to be fast (15 min), accurate and sensitive (limit of detection (LOD): 300 and 400 CFU/mL for E. coli and S. aureus, respectively). Of note, the excellent endogenous antibacterial activity of CTAB allowed the complete inactivation of bacteria after the assay process, thus effectively avoiding secondary contamination. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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Graphical abstract

11 pages, 3839 KiB

Open AccessArticle

Optimized Design and Preparation of Ag Nanoparticle Multilayer SERS Substrates with Excellent Sensing Performance

by Ping Wen, Feng Yang, Xiaoling Hu, Yi Xu, Shu Wan and Li Chen

Biosensors 2023, 13(1), 52; https://doi.org/10.3390/bios13010052 - 29 Dec 2022

Cited by 5 | Viewed by 1355

Abstract

Nanoparticle multilayer substrates usually exhibit excellent SERS activity due to multi-dimensional plasmon coupling. However, simply increasing the layers will lead to several problems, such as complex manufacturing procedures, reduced uniformity and poor reproducibility. In this paper, the local electric field (LEF) characteristics of a Ag nanoparticle (AgNP) multilayer were systematically studied through finite element simulations. We found that, on the glass support, the LEF intensity improved with the increase in the layers of AgNPs. However, the maximum LEF could be obtained with only two layers of AgNPs on the Au film support, and it was much stronger than the optimal value of the former. To verify the simulation results, we have successfully prepared one to four layers of AgNPs on both supports with a liquid–liquid interface self-assembly method, and carried out a series of SERS measurements. The experimental results were in good agreement with the simulations. Finally, the optimized SERS substrate, the 2-AgNP@Au film, showed an ultra-high SERS sensitivity, along with an excellent signal uniformity, which had a detection ability of 1 × 10⁻¹⁵ M for the Rhodamine 6G (R6G) and a relative standard deviation (RSD) of 11% for the signal intensity. Our study provides important theoretical guidance and a technical basis for the optimized design and application of high-performance SERS substrates. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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9 pages, 1835 KiB

Open AccessCommunication

Multifold Enhanced Raman Detection of Organic Molecules as Environmental Water Pollutants

by Yunyun Mu, Miao Liu, Jiajun Li and Xinping Zhang

Biosensors 2023, 13(1), 4; https://doi.org/10.3390/bios13010004 - 21 Dec 2022

Cited by 1 | Viewed by 1218

Abstract

Organic molecules, including the benzene series, have been identified as pollutants in environmental water. Due to their very low solubility, they have very small concentrations in water, and they are difficult to be detected by conventional techniques. In particular, there is a lack of real-time, accurate, and rapid detection methods for such molecules in water. However, they are detrimental to human health in many aspects. Toluene has been an important indicator of such environmental pollution detections. In this work, we propose a 3D SERS scheme consisting of a hollow fiber that is coated on the inner wall with densely arranged silver nanoparticles, which supplies multifold Raman enhancement by the plasmonic microcavity. Strong confinement of excitation laser energy and strongly enhanced Raman signals with the bidirectional collection are utilized to achieve high-sensitivity detection of toluene molecules in water. Raman signal with a reasonable signal-to-noise ratio has been measured for a concentration of 0.53 mg/L, indicating a detection limit even lower than this value for such a Raman spectroscopic technique. The corresponding enhancement factor is higher than 6 × 10³ with respect to the available systems. Thus, this device not only enables direct trace detection and real-time monitoring of the water-polluting status by organic molecules but also supplies a practical approach for biological sensing. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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13 pages, 2861 KiB

Open AccessArticle

Nanoenzyme Reactor-Based Oxidation-Induced Reaction for Quantitative SERS Analysis of Food Antiseptics

by Linmin Chen, Meihuang Zeng, Jingwen Jin, Qiuhong Yao, Tingxiu Ye, Longjie You, Xi Chen, Xiaomei Chen and Zhiyong Guo

Biosensors 2022, 12(11), 988; https://doi.org/10.3390/bios12110988 - 08 Nov 2022

Cited by 1 | Viewed by 1852

Abstract

Nanoenzyme reactors based on shell-isolated colloidal plasmonic nanomaterials are well-established and widely applied in catalysis and surface-enhanced Raman scattering (SERS) sensing. In this study, a “double wing with one body” strategy was developed to establish a reduced food antiseptic sensing method using shell-isolated colloidal plasmonic nanomaterials. Gold nano particles (Au NPs) were used to synthesize the colloidal plasmonic nanomaterials, which was achieved by attaching ferrous ions (Fe²⁺), ferric ions (Fe³⁺), nitroso (NO⁻) group, cyanogen (CN⁻) group, and dopamine (DA) via coordinative interactions. The oxidation-induced reaction was utilized to generate •OH following the Fe²⁺-mediated Fenton reaction with the shell-isolated colloidal plasmonic nanomaterials. The •OH generated in the cascade reactor had a high oxidative capacity toward acid preservatives. Importantly, with the introduction of the signal molecule DA, the cascade reactor exhibited also induced a Raman signal change by reaction with the oxidation product (malondialdehyde) which improved the sensitivity of the analysis. In addition, the stable shell-isolated structure was effective in realizing a reproducible and quantitative SERS analysis method, which overcomes previous limitations and could extend the use of nanoenzymes to various complex sensing applications. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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20 pages, 4907 KiB

Open AccessArticle

Label-Free Detection of the Receptor-Binding Domain of the SARS-CoV-2 Spike Glycoprotein at Physiologically Relevant Concentrations Using Surface-Enhanced Raman Spectroscopy

by Andrey K. Sarychev, Alyona Sukhanova, Andrey V. Ivanov, Igor V. Bykov, Nikita V. Bakholdin, Daria V. Vasina, Vladimir A. Gushchin, Artem P. Tkachuk, Galina Nifontova, Pavel S. Samokhvalov, Alexander Karaulov and Igor Nabiev

Biosensors 2022, 12(5), 300; https://doi.org/10.3390/bios12050300 - 05 May 2022

Cited by 9 | Viewed by 2562

Abstract

Surface-enhanced Raman scattering (SERS) spectroscopy is a surface- or cavity-enhanced variant of Raman scattering spectroscopy that allows the detection of analytes with a sensitivity down to single molecules. This method involves the use of SERS-active surfaces or cavities capable of concentrating incident radiation into small mode volumes containing the analyte. Here, we have engineered an ultranarrow metal–dielectric nano-cavity out of a film of the receptor-binding domain (RBD) of SARS-CoV-2 spike (S) glycoprotein and a silver surface, held together by interaction between reduced protein sulfhydryl groups and silver. The concentration of light in this nano-cavity allows the label-free recording of the characteristic Raman spectra of protein samples smaller than 1 pg. This is sufficient for the ultrasensitive detection of viral protein antigens at physiologically relevant levels. Moreover, the protein SERS signal can be increased by several orders of magnitude by coating the RBD film with a nanometer-thick silver shell, thereby raising the cavity Q-factor. This ensures a sub-femtogram sensitivity of the viral antigen detection. A simple theoretical model explaining the observed additional enhancement of the SERS signal from the silver-coated protein is proposed. Our study is the first to obtain the characteristic Raman and SERS spectra of the RBD of S glycoprotein, the key SARS-CoV-2 viral antigen, directly, without the use of Raman-reporter molecules. Thus, our approach allows label-free recording of the characteristic spectra of viral antigens at concentrations orders of magnitude lower than those required for detecting the whole virus in biological media. This makes it possible to develop a high-performance optical detection method and conformational analysis of the pathogen and its variants. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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10 pages, 635 KiB

Open AccessCommunication

Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase

by Chuhang Zhang

Biosensors 2022, 12(5), 282; https://doi.org/10.3390/bios12050282 - 28 Apr 2022

Cited by 1 | Viewed by 1290

Abstract

Metallic nanoclusters (NCs) have been predicted to achieve the best Surface-Enhanced Raman Scattering (SERS) due to the controllable amount of atoms and structures in NCs. The Local Surface Plasmon Resonance (LSPR) effect on silver metal NCs (Ag

_{n}

) enables it to be [...] Read more.

_{n}

) enables it to be a promising candidate for manipulating the LSPR peak by controlling the size of NCs, which in turn demands a full understanding of the formation mechanism of Ag

_{n}

. Here, we apply an extended Smoluchowski rate equation coupled with a fragmentation scheme to investigate the growth of size-selected silver NCs generated via a modulated pulsed power magnetron sputtering (MPP-MSP). A temperature-dependent fragmentation coefficient D is proposed and integrated into the rate equations. The consistency between the computational and experimental results shows that in relative low peak power (

P_{p} \leq 800

W), the recombination of cation and anion species are the dominant mechanism for NC growth. However, in the higher

P_{p}

region (≥800 W), the fragmentation mechanism becomes more impactful, leading to the formation of smaller NCs. The scanning electron microscopy observation shows the Ag

_{36}

is successfully soft-landed and immobilized on a strontium titanate crystal, which facilitates the application of the Ag

_{n}

/STO to the SERS research. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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Review

Jump to: Research

34 pages, 7564 KiB

Open AccessReview

Plasmonic Nanoparticle-Enhanced Optical Techniques for Cancer Biomarker Sensing

by Li Fu, Cheng-Te Lin, Hassan Karimi-Maleh, Fei Chen and Shichao Zhao

Biosensors 2023, 13(11), 977; https://doi.org/10.3390/bios13110977 - 08 Nov 2023

Viewed by 2158

Abstract

This review summarizes recent advances in leveraging localized surface plasmon resonance (LSPR) nanotechnology for sensitive cancer biomarker detection. LSPR arising from noble metal nanoparticles under light excitation enables the enhancement of various optical techniques, including surface-enhanced Raman spectroscopy (SERS), dark-field microscopy (DFM), photothermal imaging, and photoacoustic imaging. Nanoparticle engineering strategies are discussed to optimize LSPR for maximum signal amplification. SERS utilizes electromagnetic enhancement from plasmonic nanostructures to boost inherently weak Raman signals, enabling single-molecule sensitivity for detecting proteins, nucleic acids, and exosomes. DFM visualizes LSPR nanoparticles based on scattered light color, allowing for the ultrasensitive detection of cancer cells, microRNAs, and proteins. Photothermal imaging employs LSPR nanoparticles as contrast agents that convert light to heat, producing thermal images that highlight cancerous tissues. Photoacoustic imaging detects ultrasonic waves generated by LSPR nanoparticle photothermal expansion for deep-tissue imaging. The multiplexing capabilities of LSPR techniques and integration with microfluidics and point-of-care devices are reviewed. Remaining challenges, such as toxicity, standardization, and clinical sample analysis, are examined. Overall, LSPR nanotechnology shows tremendous potential for advancing cancer screening, diagnosis, and treatment monitoring through the integration of nanoparticle engineering, optical techniques, and microscale device platforms. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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22 pages, 4339 KiB

Open AccessReview

Recent Progress of Surface-Enhanced Raman Spectroscopy for Bacteria Detection

by Lulu Liu, Wenrui Ma, Xiang Wang and Shunbo Li

Biosensors 2023, 13(3), 350; https://doi.org/10.3390/bios13030350 - 06 Mar 2023

Cited by 13 | Viewed by 3416

Abstract

There are various pathogenic bacteria in the surrounding living environment, which not only pose a great threat to human health but also bring huge losses to economic development. Conventional methods for bacteria detection are usually time-consuming, complicated and labor-intensive, and cannot meet the growing demands for on-site and rapid analyses. Sensitive, rapid and effective methods for pathogenic bacteria detection are necessary for environmental monitoring, food safety and infectious bacteria diagnosis. Recently, benefiting from its advantages of rapidity and high sensitivity, surface-enhanced Raman spectroscopy (SERS) has attracted significant attention in the field of bacteria detection and identification as well as drug susceptibility testing. Here, we comprehensively reviewed the latest advances in SERS technology in the field of bacteria analysis. Firstly, the mechanism of SERS detection and the fabrication of the SERS substrate were briefly introduced. Secondly, the label-free SERS applied for the identification of bacteria species was summarized in detail. Thirdly, various SERS tags for the high-sensitivity detection of bacteria were also discussed. Moreover, we emphasized the application prospects of microfluidic SERS chips in antimicrobial susceptibility testing (AST). In the end, we gave an outlook on the future development and trends of SERS in point-of-care diagnoses of bacterial infections. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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23 pages, 4443 KiB

Open AccessReview

Recent Progress on Solid Substrates for Surface-Enhanced Raman Spectroscopy Analysis

by Kun Ge, Yuling Hu and Gongke Li

Biosensors 2022, 12(11), 941; https://doi.org/10.3390/bios12110941 - 30 Oct 2022

Cited by 11 | Viewed by 3151

Abstract

Surface-enhanced Raman spectroscopy (SERS) is a powerful vibrational spectroscopy technique with distinguished features of non-destructivity, ultra-sensitivity, rapidity, and fingerprint characteristics for analysis and sensors. The SERS signals are mainly dependent on the engineering of high-quality substrates. Recently, solid SERS substrates with diverse forms have been attracting increasing attention due to their promising features, including dense hot spot, high stability, controllable morphology, and convenient portability. Here, we comprehensively review the recent advances made in the field of solid SERS substrates, including their common fabrication methods, basic categories, main features, and representative applications, respectively. Firstly, the main categories of solid SERS substrates, mainly including membrane substrate, self-assembled substrate, chip substrate, magnetic solid substrate, and other solid substrate, are introduced in detail, as well as corresponding construction strategies and main features. Secondly, the typical applications of solid SERS substrates in bio-analysis, food safety analysis, environment analysis, and other analyses are briefly reviewed. Finally, the challenges and perspectives of solid SERS substrates, including analytical performance improvement and largescale production level enhancement, are proposed. Full article

(This article belongs to the Special Issue High Performance Integrated Biosensors Based on SERS)

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