ANALYST
·
2024
·Vol. 149
·期 15
·4060-4071
·
IF 3.6
Jie Zhou,Huiting Wang,Yaxian Chen,Dongxue Lin,Ling Zhang,Zhiqiang Xing,Qian Zhang,Jiarui Xia
The precise quantitative analysis using surface-enhanced Raman spectroscopy (SERS) in an uncontrollable environment still faces a significant obstacle due to the poor reproducibility of Raman signals. Herein, we propose a facile method to fabricate a self-calibrating substrate based on a flexible polyvinyl alcohol (PVA) film comprising assemblies of Prussian blue (PB) and Au NPs (PB@Au) for reliable detection. PB cores were coated with an Au shell through simple electrostatic interaction, forming core–shell nanostructure PB@Au assemblies within the PVA film. The outer Au layer provided identical trends in enhancement for both the PB core and neighboring targets while PB cores served as an internal standard (IS) to correct signal fluctuations. The prevention of competitive adsorption on the metal surface between targets and ISs was achieved. The proposed PVA/PB@Au film exhibited enhanced stability of Raman signals after IS correction, resulting in improved spot-to-spot and batch-to-batch reproducibility with significantly reduced standard deviation (RSD) values from 11.42% and 25.02% to 4.43% and 9.39%, respectively. Simultaneously, a higher accuracy in the quantitative analysis of 4-mercaptobenzoic acid (4-MBA) and malachite green (MG) was achieved with fitting coefficient (R2) values improving from 0.9675 and 0.9418 to 0.9974 and 0.9832, respectively. Moreover, the PVA/PB@Au film was successfully applied to detect residual MG in real fish samples. This work opens up an avenue to improve the reproducibility of Raman signals for flexible SERS substrates in the detection of residues under various complex conditions.
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APPLIED CLAY SCIENCE
·
2024
·
IF 5.3
Hao Zhang,Chaopeng Fu,Jianhao Ding,Guoqiang Xu,Chunhui Zhou,Zhenyu He,Zhimin Ou,Dongshen Tong,Minyang Qiu,Xiangdong Zhou,Xiaonian Li
An electrostatic adsorption-based, surface-enhanced Raman scattering (SERS) assay for the detection of charged analytes was developed, which utilized Ag-deposited laponite nanoparticles (Ag@Lap NPs) as both a SERS substrate and negatively charged absorber for the capture of positively charged analytes, such as methylene blue (MB) and rhodamine B (RB). The strong electrostatic interaction between the MB analyte and the Ag@Lap NPs resulted in an effective concentration of MB on the Ag content of Ag@Lap and provided a limit of detection (LOD) sensitivity of 10 −11 M, which was more sensitive by a factor of 25,000 over the LOD of MB (0.25 × 10 −6 M) in a similar SERS assay using bare Ag NPs with low charges. Additionally, a 100-fold improvement in LOD was also observed for RB analyte on Ag@Lap NPs over that on bare Ag NPs. Unlike positively charged, the negatively charged analytes, such as direct black-168 (DB-168) and methyl orange (MO), exhibited a weaker adsorption on the same negatively charged surface of Ag@Lap NPs due to electrostatic repulsion, leading to a lower SERS sensitivity. These results indicated that the electrostatic attraction between the analytes and SERS substrate played an important role in enriching the number of analytes on the active substrate to significantly improve the SERS intensity, suggesting a new strategy, which could be easily adapted to environmental analysis and biosensor applications by concentrating and detecting charged analytes, such as pollutants and dye molecules in nanotags.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Wen Deng,Xingyue Liu,Yuzhou Yang,Liucheng Meng,Yanling Lou,Peng Li,Lei Zhang,Weibing Wu
Surface-enhanced Raman scattering (SERS) is a highly sensitive technology to detect target analytes. The construction of dynamic “hot-spots” represents a significant approach to enhancing detection sensitivity. Herein, a hybrid plasma platform with dynamic “hot-spots” was developed for SERS recognition based on the assembly of gold nanospheres (AuNSs) on temperature-sensitive bacterial cellulose (BC) film grafted with poly( N -isopropylacrylamide) (PNIPAM). The dynamic “hot-spots” structure was regulated in-situ by local conformational contraction of the grafted thermoresponsive PNIPAM around the BC backbone without changing the overall morphology of the substrate. Moreover, the heating process was simplified by utilizing the plasma photothermal effect of AuNSs to regulate the “hot-spot” structure. The dynamic regulation measured value of the Raman signal of Rhodamine 6G (R6G) was increased by 6.5-times, and the SERS substrate exhibited extremely high sensitivity with a limit of detection (LOD) of 8.47 × 10 −9 g/L and a relative standard deviation (RSD) of 9.24 %. Meanwhile, it can accurately detect the pesticide residues of thiram on apple peel with the detection limit of 6.54 × 10 −11 g/L. This dynamic “hot-spot” modulation strategy via local structural regulation has significant potential to improve the convenience, flexibility, and sensitivity of on-site SERS detection.
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FOOD RESEARCH INTERNATIONAL
·
2025
·
IF 8
Meng-Lei Xu,Songning Zhao,Wenshuo Ren,Mengmeng Zhang,Xiao Xia Han,Liang Su,Chengcong Chen,Yunfei Xie,Yu Gao
Degradation pathways of the pesticide pyridaben in tea caused by ultraviolet photocatalytic degradation were identified using SERS and GC–MS. Pyridaben in tea decreased from 4.50 mg/kg to 3.46 mg/kg after 2 h and to 0.62 mg/kg after 5 h, with a degradation rate of 86.22 % and a recovery rate of 90.00 %. The pyridaben degradation process involved C–S cleavage, with a SERS band of ν(C–S) at 710 cm −1 disappearing in the first hour. This was followed by cleavage of the N atom and the attached tert butyl group, resulting in the cleavage of the C-N bond in the ring, causing ring opening degradation. The presence of residual pyridaben was not necessarily related to the content of tea polyphenols; however, the UV light significantly reduced the content of theobromine, EGC, EC, and ECG but increased the content of EGCG. Ultraviolet irradiation slightly reduced the moisture content of oolong tea samples and did not significantly affect the total ash content. The content of water extract increaseing irradiation time due to the influence of moisture. UV irradiation time at the range of 60–360 min could degrade pyridaben while reducing its impact on tea quality.
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ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Dechan Lu,Zufang Huang,Jingbo Chen,Yudong Lu
Surface-enhanced Raman spectroscopy (SERS) provides a rapid and nondestructive method for biological plasma analysis, offering unparalleled sensitivity and specificity. However, most current studies predominantly employ the drop-cast method, where liquid samples are dried on the SERS substrate for spectral recording. While effective, this method is both time-consuming and inconsistent. Additionally, the Raman spectral signal of uric acid in plasma often dominates, overshadowing other crucial biomarkers necessary for disease differentiation. In this study, we present the application of label-free SERS detection for distinguishing early stage lung cancer (LC) from healthy controls (HC) using plasma samples. Plasma was diluted, adjusted to a weakly acidic pH, and combined with silver nanoparticles (Ag NPs) for SERS analysis. To maintain the plasma in a liquid state and prevent evaporation, liquid paraffin was employed. Our findings indicate that a 10-fold dilution of plasma under weakly acidic conditions significantly enhanced diagnostic performance, achieving an area under the receiver operating characteristic curve (AUC) of 0.975. This method is featured by its simplicity and high efficiency, presenting a promising strategy for the minimally invasive diagnosis of early stage LC using SERS technology.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Lingli Zhang,Yilin Yu,Xinyi Zhu,Liping Song,Yu Zhao,Lei Jiang,Xiaoyu Zhao,Bihu Lv,Yixuan Sun,Youju Huang
Electromagnetic hotspot engineering plays a crucial role in surface-enhanced Raman scattering (SERS) biosensors . However, the construction of optical hotspots with high density and the concentration of analytes into hotspot centers remain challenging tasks. Additionally, achieving high sensitivity and signal reproducibility in SERS biosensors is an ongoing challenge. In this study, we utilise Janus micro/nano arrays to develop a superhydrophobic SERS platform. The high roughness of these arrays facilitates the distribution of rich hotspots ranging from nano to microscale and encourages the concentration of analytes within hotspot centers. The Janus plasmonic micro/nano arrays were meticulously crafted through the synergy of site-specific growth and instant interfacial assembly of nanoparticles (NPs). In the realm of SERS measurements targeting organic dyes in river water , our sensing platform demonstrates high sensitivity (limit of detection (LOD): 10 −9 M) and signal reproducibility (relative standard deviation (RSD)=4.25 %). Furthermore, the SERS platform exhibited remarkable sensitivity to multiple dyes in river water . Thus, our superhydrophobic SERS platform lays the groundwork for sensitive analysis in diverse fields such as environmental analysis and healthcare monitoring.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2024
·
IF 4
Dongjian Li,Mulinde Timothy Ezra,Haoran Li,Yifei Chen,Chengyun Si,Xuefang Luo
Neonicotinoids (NEOs) are widely used in agricultural cultivation, and the presence of residual NEOs poses a serious threat to consumer health. Therefore, trace detection of NEOs is particularly important. In this study, a response surface experimental design was employed to develop AgNP with high enhancement factor and surface height anisotropy, effectively enhancing the Raman signals of acetamiprid (ACE) and thiacloprid (THI) through densely populated hotspots on the surface. Gaussian simulation calculations were used to assign peaks in the ACE and THI spectra. Subsequently, convolutional neural network, backpropagation neural network, and AlexNet neural network were employed to identify the ACE, THI, and mixed component spectra, successfully distinguishing the spectra of the three compounds and achieving qualitative analysis of unknown spectra. Furthermore, genetic algorithm-partial least squares was used to model the spectral data, achieving a correlation coefficient of 0.97. The method was applied for the detection of spiked tea samples, achieving a precision RSD of 4.84 %. Therefore, this sensor combined with intelligent algorithms can be used for spectral identification and trace detection of mixed pesticide samples with structurally similar compounds.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Kai Liu,Qikui Fan,Zhun Qiao,Zhixue Zhang,Yongzhao Zhang,Zhiqun Chen,Hao Ma,Zemin He,Zongcheng Miao,Jiaofei Huo,Duqiang Xin,Jianxin Guo,Chuanbo Gao
Plate-like metal nanomaterials have attracted much interest due to their anisotropy, high aspect ratio and large surface area. The synthesis of non-noble metal nanocrystals with high purity remains challenging due to the poor regulation mechanism of their seeds, which limits their property and application studies. This paper presents a selective etching mechanism that effectively facilitates the identification and dissolution of non-target seeds during the synthesis of Cu nanoplates. This innovative approach not only enables the production of highly pure nanoplates but also allows for the shape transformation of nanoparticles into nanoplates. The resulting Cu nanoplates exhibit tunable localized surface plasmon resonance (LSPR) characteristics and high enhanced performance in surface-enhanced Raman scattering (SERS). This method offers a novel approach to the synthesis and purification of metal nanocrystals.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Zhou Jinyu,Zha Xiuling,Ma Siying,Wu Sihui,Ma Chunlan,Chen Gaoyuan,Chen Zhigang,Zhang Taoyang,Chen Zhiwei,Wang Di,Yan Yuxiang,Sun Yuqing,Ren Hengdong,Sun Hongzhao,Wu Xinglong,Zhao Zhigang,Cong Shan
Metal single atoms have been demonstrated to induce surface-enhanced Raman scattering (SERS) due to their effectiveness in the modification of electronic structure. However, precisely modulating the relative positions of metal single atoms on sub-nanolattices remains a formidable challenge, which makes SERS studies of metal single atoms dependent on localized environments still lacking. Herein, we rely on polyethylene glycol (PEG) as a soft template to achieve the modulation of the relative positions of W atoms on titanate nanotubes (W-TNTs) and probe the local-environment-dependent SERS induced by metal single atoms based on this technique. We find that the relative position of the W single atoms greatly affects their SERS performance. This phenomenon has been attributed to the difference in charge transfer ability between single W atoms of different configurations, with isolated W atoms inducing a significantly higher density of electronic states near the Fermi energy than associated W atoms, leading to an enhanced polarization of the probe molecule and subsequently a stronger Raman signal. Our findings demonstrate a technique to effectively control the relative positions of single atoms and provide insights into single-atom-induced SERS associated with localized environments, which will facilitate the rational design of SERS substrates based on metal single atoms.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yansheng Liu,Yunjie Zhan,Haonan Hu,Guofu Wang,Xiaobo Jia,Jin Zhou,Hongqi Li,Haixin Chang,Zhaoxu Li
This study reports a SERS-based microfluidic chip for the cyclic detection of histamine with high specificity. Easily fabricated Au nanoparticles (AuNPs) were synthesized on Si substrates by using a thermally treating approach. The designed probe DNA (pDNA) functionalized AuNPs is used as a sensing surface. The Cyanine 3 (Cy3) functionalized complementary DNA (cDNA) is modified on the chemically synthesized AuNPs and the complex cDNA/AuNPs are used as nanotags. Due to the hybridization between the pDNA and the cDNA, nanotags-pDNA/AuNPs structure is formed and illustrates a high SERS intensity of Cy3. With the presence of the histamine, due to the stronger affinity between cDNA and histamine, nanotags-pDNA/AuNPs structure is destroyed and the nanotags are separated from the sensing surface resulting in a decrease in the SERS intensity of Cy3. By adding fresh nanotags, nanotags-pDNA/AuNPs structure is regenerated, and a new detection cycle can be performed. By utilizing the proposed SERS-based microfluidic chip, the limit of detection (LOD) of histamine in DI water is 1 × 10 −9 g/mL. The concentration is well below the U.S. Food and Drug Administration (FDA) histamine toxicity threshold of 5 × 10 −5 g/mL. Moreover, the proposed SERS-based microfluidic chip can be reused 7 times. Furthermore, this chip has accuracy and applicability were validated through its application in beer samples. Indicating that this method has great potential for histamine detection.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Haiqian Xia,Lingzi Xiong,Ruoyu Huang,Ning Liu,Muhammad Muhammad,Jingfang Hong,Qing Huang
Breast cancer remains a global health challenge, with an increasing number of cases necessitating innovative approaches to streamline patient management prior to treatment. In this study, we present a comprehensive aptamer-involved surface-enhanced Raman spectroscopy (aptamer-SERS)-based protocol specifically designed for large-scale clinical screening of the circulating protein MUC1 overexpressed in the majority of breast cancer cases. Central to our approach was a “sandwich” assay, where MUC1 was anchored between aptamer-functionalized bimetallic core-shell nanoparticles (NPs) and magnetic nanobeads. The biosensor was applied to monitor MUC1 in serum samples through SERS signals from the reporter molecule 4-ATP, exhibiting a strong linear correlation across a wide dynamic range and the lower the limit of detection (LOD) of 2.96 fg/mL. To support clinical decision-making, the protocol was integrated with a machine learning (ML)model for the classification of SERS signal patterns, demonstrating performance metrics of 96% accuracy and 93.7% specificity when applied to diverse serum samples. This integration enabled robust, non-invasive preclinical screening that informs therapeutic regulation and patient monitoring long before clinical symptoms present. By establishing a scalable framework for continuous monitoring of MUC1 levels across large populations, our study offered a forward-thinking tool, namely, dual-aptamer-SERS biosensor, that may optimize individualized treatment planning and improve overall clinical management strategies.
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BIOSENSORS & BIOELECTRONICS
·
2025
·
IF 10.5
Haoran Zheng,Heng Zhang,Jingyi Wu,Zhen Jiao,Yi Chen
Nanoengineering of plasmonic/magnetic nanocrystals plays a pivotal role in advancing biomolecular detection, offering emerging strategies for cancer diagnostics and therapeutic monitoring. Early and precise detection of cancer biomarkers is critical for timely intervention. Yet conventional immunoassays are often hindered by limited sensitivity, nonspecific binding, and inefficient target enrichment, reducing their clinical reliability. Herein, we develop a self-reporting bimetallic plasmonic nanoflowers-based SERS immunoassay that integrates magnetic enrichment and plasmonic field amplification for ultrasensitive detection of total prostate-specific antigen (t-PSA). The bimetallic Ag-Au nanoflowers were synthesized through a novel nanocrystal engineering approach that integrates the structural stability of gold with the superior plasmonic enhancement of silver, while intrinsically incorporating self-reporting SERS labels on the surface. Serving as intrinsic Raman probes, these nanoflowers eliminate the need for external labeling, thereby simplifying the detection process and enhancing reproducibility. Simultaneously, antibody-functionalized magnetic nanoparticles facilitate efficient target separation and enrichment, significantly improving detection sensitivity. This synergistic strategy achieves an ultra-low detection limit of 100 fg mL −1 and enables precise quantification within the diagnostic gray zone (4.0–10.0 ng mL −1 ), a critical range for early prostate cancer screening. Furthermore, the reliability of the SERS immunoassay was further confirmed by testing t-PSA-spiked serum samples, showing consistent analytical performance and excellent agreement with conventional ELISA measurements. The combination of self-reporting plasmonic nanostructures, magnetic-assisted biomarker capture, and hotspot-driven SERS amplification offers promising and highly sensitive biosensing nanoprobes for early prostate cancer diagnosis.
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