Journal of Physical Chemistry C
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2023
·
IF 3.7
Yumiao Dong,Qinhui Xie,Shuo Wu,Junbo Li,Lei Sun,Wei Ji
p-Mercaptobenzoic acid (4-MBA) is a typical molecular probe for a surface-enhanced Raman scattering (SERS) study of the enhancement performance of semiconductor nanoparticles. Understanding the molecular adsorption mechanism of 4-MBA on a semiconductor surface is crucial to reveal the enhancement mechanism of semiconductor SERS. Herein, two types of submicrometer-sized TiO2 particles with amorphous (denoted as a-TiO2) and anatase structures (denoted as c-TiO2) were fabricated, and their potential as SERS-active substrates with high electric-field enhancement was explored based on the near-field scattering theory and finite-element method simulation. The electric field-enhanced semiconductor SERS provide a better vision for us to study the adsorption modes of molecules on the TiO2 surface. On this basis, adsorption behaviors of 4-MBA on a-TiO2 and c-TiO2 particles were systematically studied by the semiconductor SERS and density functional theory. The results demonstrated that the adsorption mechanism of 4-MBA with TiO2 surfaces is highly dependent on the exposure of acid sites of TiO2 surfaces. 4-MBA adsorbs preferentially on Brønsted acid sites of a-TiO2 through a carboxyl group, in contrast on Lewis acid sites of c-TiO2 through a sulfhydryl group. Furthermore, 4-MBA molecules may form multilayer adsorption on TiO2 surfaces through the hydrogen bond and/or π–π stacking interaction. Research results not only provide a new insight to re-evaluate the chemical enhancement mechanism for TiO2–4-MBA systems but also provide a theoretical guidance for the modification of TiO2 surface with organic molecules containing carboxyl and sulfhydryl groups.
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OPTICS EXPRESS
·
2023
·Vol. 31
·期 10
·16484-16494
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IF 3.8
Sha HaiYang,Wang Zhengkun,Zhu Yong,Zhang Jie
To achieve high sensitivity and uniformity simultaneously in a surface-enhanced Raman scattering (SERS) substrate, this paper presents the preparation of a flexible and transparent three-dimensional (3D) ordered hemispherical array polydimethylsiloxane (PDMS) film. This is achieved by self-assembling a single-layer polystyrene (PS) microsphere array on a silicon substrate. The liquid-liquid interface method is then used to transfer Ag nanoparticles onto the PDMS film, which includes open nanocavity arrays created by etching the PS microsphere array. An open nanocavity assistant soft SERS sample, “Ag@PDMS,” is then prepared. For electromagnetic simulation of our sample, we utilized Comsol software. It has been experimentally confirmed that the Ag@PDMS substrate with silver particles of 50 nm in size is capable of achieving the largest localized electromagnetic hot spots in space. The optimal sample, Ag@PDMS, exhibits ultra-high sensitivity towards Rhodamine 6 G (R6G) probe molecules, with a limit of detection (LOD) of 10−15 mol/L, and an enhancement factor (EF) of ∼1012. Additionally, the substrate exhibits a highly uniform signal intensity for probe molecules, with a relative standard deviation (RSD) of approximately 6.86%. Moreover, it is capable of detecting multiple molecules and can perform real detection on non-flat surfaces.
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JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Qi He,Dandan Wang,Jing Shao,Yi Li,Ming Cheng,Lihui Dong,Yunhui Li,Jianwei Zhu,Hongji Li
A novel imprinting membrane (Ag/CuO/CNTs/Eggshell membrane -Molecularly Imprinted polymeric Membrances, ACCE-MIMs) based on surface enhanced Raman scattering (SERS) is successfully synthesized for the specific detection of spiramycin (SP). Firstly, CNTs and CuO are successively loaded on eggshell membrane (ESM) to increase the uniformity and sensitivity by virtue of the unique reticular structure of CNTs and excellent chemical enhancement of CuO. Through the abundant amino and carboxyl groups on ESM, Ag nanoparticles (Ag NPs) are anchored and growth on the surface of membrane by two in-situ reduction process and form a three-dimensional (3D) architecture. Eventually, the ACCE-MIMs are synthetized by silicon-based sol-gel method. With the help of imprinted polymers, the ACCE-MIMs present anti-interference performance during selective detection. The sensor presents a great liner relationship (R 2 = 0.9965) between SP concentration and the Raman peak intensity when the concentration of SP ranges between 1 × 10 −6 M ∼1 × 10 −12 M. The limit of detection concentration is 1 × 10 −12 M and the enhancement factor (EF) is 0.2956 × 10 7 . The ACCE-MIMs exhibits sensitive detection property and this procedure provides a promising future for detection process.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 30
·16212-16220
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IF 11.9
Le Tang,Xiancheng Pan,Man Luo,Ruyu Yang,Lulu Guo,Zixu Sun,Shenlong Jiang,Jun Jiang,Guozhen Zhang,Qing Zhu
Metal oxide semiconductors have emerged as promising candidates for surface-enhanced Raman scattering (SERS) to replace conventional noble metal substrates. Here, we demonstrate an insulator to quasi-metallic phase transition in electron-rich WO3 doped with group 1 elements (H, Li, Na, and K) to amplify the Raman response of adsorbed probe molecules. In this category, the lithium-doped WO3 (LWO) exhibited excellent balance between SERS sensitivity and photostability, with enhancement factors (EFs) up to 4.3 × 106 and a limit of detection (LOD) of 10−8 M. Based on theoretical simulations and advanced experimental characterizations, we identified its non-discrete band arrangement and high free carrier concentration (1.3 × 1021 cm3), which create not only efficient migration channels for interfacial charge-transfer (CT) enhancement, but also a surface localized surface plasmon resonance (LSPR) effect-induced strong electromagnetic field that further amplified the Raman response via an electromagnetic (EM) mechanism. Our strategy greatly refines and expands the scope of existing metal oxide materials, offering new insights for designing efficient and robust non-noble metal-based SERS substrates.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Pan Tao,Kaixin Ge,Xing Dai,Danni Xue,Yang Luo,Shixun Dai,Tiefeng Xu,Tao Jiang,Peiqing Zhang
Surface-enhanced Raman scattering (SERS) has great potential in the field of rapid detection of pesticide residues in food. In this paper, a fiber optic SERS sensor excited by evanescent waves was proposed for efficient detection of thiram. Silver nanocubes (Ag NCs) were prepared as SERS active substrates, which had much stronger electromagnetic field intensity than nanospheres under laser excitation due to much more “hot spots”. By using the method of electrostatic adsorption and laser induction, Ag NCs were uniformly assembled at the fiber taper waist (FTW) for enhancing the Raman signal. Different from the traditional way of stimulation, evanescent wave excitation greatly increased the interaction area between the excitation and analyte, while reducing the damage of the excited light to the metal nanostructures. The methods proposed in this work have been successfully used to detect the pesticide residues of thiram and showed good detection performance. The detection limits for 4-Mercaptobenzoic acid (4-MBA) and thiram were determined to be 10–9 and 10–8 M, the corresponding enhancement factor could be 1.64 × 105 and 6.38 × 104. Low concentration of thiram was detected in the peels of tomatoes and cucumbers, indicating its feasibility in actual sample detection. The combination of evanescent waves and SERS provides a new direction for the application of SERS sensors, which had great application potential in the field of pesticide residue detection.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Mingyi Yao,Jian Liu,Narengaowa,Yonggu Li,Feng Zhao
Accurate detection of natural dyes in archaeological textiles is challenging due to limited sample availability. In situ detection of fibers by surface-enhanced Raman scattering (SERS) can overcome this challenge. In this study, we present two methods for the preparation of SERS substrates based on the laser photoreduction reaction and the galvanic displacement reaction, respectively. Our results show that the substrates prepared by these methods, including 450 nm-AgNPs, Cu-based Ag, and Zn-based Ag, offer several advantages such as rapid preparation, easy handling, low cost, high sensitivity and excellent reproducibility. Using these substrates, we successfully detected anthraquinones (alizarin, purpurin), indigoids (indigotin, indirubin), and protoberberine-type dyes in archaeological textiles from the Wei and Jin Dynasties. Notably, we were able to detect both indigo and protoberberine-type dyes in one archaeological fiber. The minimally invasive, in situ analytical approach developed provides a valuable tool for analytical applications where sampling is limited to microscopic amounts.
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Analytical Methods
·
2023
·Vol. 15
·期 24
·2915-2924
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IF 3.1
Wei Xu,Yu Zhang,Dianhai Hou,Jianjun Shen,Jinhua Dong,Zhiqin Gao,Honglin Liu
Simultaneous and ultrasensitive detection of multiple microRNA (miRNA) biomarkers is an essential precondition for early cancer diagnosis and treatment. Here we developed a sandwich surface-enhanced Raman scattering (SERS) sensor based on Au@Ag core–shell nanorods combined with duplex specific nuclease-mediated signal amplification (DSNSA) for quantitative detection of multiple breast cancer miRNA biomarkers. The DSNSA strategy enables quantitative detection of target miRNA through rehybridizing the capture probe DNA-SERSnanotag conjugates to trigger signal amplification. The Au@Ag core–shell nanorods coated with an Ag shell exhibit excellent SERS performance, implying that molecules can be concentrated by the Ag shell at the hot spots. By monitoring the Raman signal attenuation of hot spots in the presence of target miRNAs, three breast cancer associated miRNAs (miR-21, miR-155, and let 7b) were simultaneously determined using the sandwich SERS sensor, and their detection limits (LODs) were 0.05 fM, 0.063 fM and 0.037 fM, respectively. These results indicated that our sandwich SERS sensor combined with the DSNSA strategy holds remarkable promise for multiplex detection of cancer biomarkers and contributes to early diagnosis of cancer.
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ACS Sensors
·
2023
·
IF 8.9
Xin Liu,Alei Dang,Tiehu Li,Yiting Sun,Tung-Chun Lee,Weibin Deng,Shaoheng Wu,Amir Zada,Tingkai Zhao,Hao Li
High sensitivity, good signal repeatability, and facile fabrication of flexible surface enhanced Raman scattering (SERS) substrates are common pursuits of researchers for the detection of probe molecules in a complex environment. However, fragile adhesion between the noble-metal nanoparticles and substrate material, low selectivity, and complex fabrication process on a large scale limit SERS technology for wide-ranging applications. Herein, we propose a scalable and cost-effective strategy to a fabricate sensitive and mechanically stable flexible Ti3C2Tx MXene@graphene oxide/Au nanoclusters (MG/AuNCs) fiber SERS substrate from wet spinning and subsequent in situ reduction processes. The use of MG fiber provides good flexibility (114 MPa) and charge transfer enhancement (chemical mechanism, CM) for a SERS sensor and allows further in situ growth of AuNCs on its surface to build highly sensitive hot spots (electromagnetic mechanism, EM), promoting the durability and SERS performance of the substrate in complex environments. Therefore, the formed flexible MG/AuNCs-1 fiber exhibits a low detection limit of 1 × 10–11 M with a 2.01 × 109 enhancement factor (EFexp), signal repeatability (RSD = 9.80%), and time retention (remains 75% after 90 days of storage) for R6G molecules. Furthermore, the l-cysteine-modified MG/AuNCs-1 fiber realized the trace and selective detection of trinitrotoluene (TNT) molecules (0.1 μM) via Meisenheimer complex formation, even by sampling the TNT molecules at a fingerprint or sample bag. These findings fill the gap in the large-scale fabrication of high-performance 2D materials/precious-metal particle composite SERS substrates, with the expectation of pushing flexible SERS sensors toward wider applications.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2023
·
IF 5.8
Ningtao Cheng,Bin Lou,Hongyang Wang
By its many virtues, non-biomarker-reliant molecular detection has recently shown bright prospects for cancer screening but its clinical application is hindered by the shortage of measurable criteria that are analogous to biomarkers. Here, we report a digital biomarker, as a new-concept serum biomarker, of hepatocellular carcinoma (HCC) found with SERS-based biosensors and a deep neural network “digital retina” for visualizing and explicitly defining spectral fingerprints. We validate the discovered digital biomarker (a collection of 10 characteristic peaks in the serum SERS spectra) with unsupervised clustering of spectra from an independent sample batch comprised normal individuals and HCC cases; the validation results show clustering accuracies of 95.71% and 100.00%, respectively. Furthermore, we find that the digital biomarker of HCC shares a few common peaks with three clinically applied serum biomarkers, which means it could convey essential biomolecular information similar to these biomarkers. Accordingly, we present an intelligent method for early HCC detection that leverages the digital biomarker with similar traits as biomarkers. Employing the digital biomarker, we could accurately stratify HCC, hepatitis B, and normal populations with linear classifiers, exhibiting accuracies over 92% and area under the receiver operating curve values above 0.93. It is anticipated that this non-biomarker-reliant molecular detection method will facilitate mass cancer screening.
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CELLULOSE
·
2023
·Vol. 30
·期 8
·5187-5200
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IF 5.7
Li Jie,Lu Dechan,Yang Jinglei,You Ruiyun,Chen Jingbo,Weng Jingzheng,Lu Yudong
We developed a method for the fabrication of in-situ reduced bacterial cellulose membrane (BCM) for the simple synthesis of three-dimensional (3D) flexible SERS substrate. Ag NPs with high density were in-situ grown and uniformly distributed on the 3D BCM nanofibers through a controlled “silver mirror reaction” and “volume shrinkage” treatment, which created highly stable and uniform hot spots in the networked SERS substrate. “Hydrogel” BCM was formed by soaking in ammonia solution to hydrolyze the hemiacetal structure of cellulose, followed by in-situ reduction in silver trifluoroacetate (CF 3 COOAg) solution, the BCM enriched with silver nanospheres (Ag NPs-BCM) substrate was prepared. The results showed that the optimized Ag NPs-BCM substrate exhibited high SERS activity, and displayed an average EF of 5.3 × 10 8 and RSD of 11.0%, especially when protected from light for 45 days, the SERS performance kept steady. The Ag NPs-BCM substrate was used to detect glutathione (GSH). Interestingly, adding Ellman's reagent (DTNB) to serum, we clearly distinguished the amount of GSH content in cancer and normal using Ag NPs-BCM substrate. This has provided the opportunity to use flexible substrate in rapid biomedical assays.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2023
·
IF 4.3
Baihui Wang,Huan Jiang,Ruyi Tang,Yaoyu Tan,Xuemin Xia,Xia Zhang
The activity of nanozymes is dependent on their surface for catalysis, and bioconjugation or adsorption of DNA aptamers will promote their activity. This paper aims to develop a novel aptamer sensor, for rapid, sensitive and specific detection of histamine. The design of the aptamer biosensor is based on the adsorption of histamine aptamers onto the surface of Au NPs by bioconjugation, which promotes the peroxidase activity of the nanozymes. Since histamine is strongly selective and specific for histamine aptamers, the histamine aptamer can be detached from the surface of Au NPs and bound to histamine, during which the catalytic activity of the nanozymes falls back due to the detachment of the histamine aptamer, which can be quantitative analysis by the TMB-H 2 O 2 system. The decrease in enzyme catalytic activity became larger with increasing histamine concentration, with a good linear correlation. Finally, the histamine aptamer biosensor was constructed, which has the advantages of ultrasensitive, high-accuracy, and wide linear range. The linear range and detection limit are 10 −11 ∼10 −3 M and 1.22 × 10 −12 M, respectively. With reference to this aptamer sensor design, this approach can also be extended to other schemes where the aptamer is combined with Au NPs as a way to detect the corresponding molecules.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Mingchun Lv,Nisar Hussain,Da-Wen Sun,Hongbin Pu
An optimum SERS performance is mainly dependent on the development of innovative substrates that show high spectral reproducibility and stability. The current study involves the synthesis of core–shell nanorods (Au@AgNRs) functionalized with mercaptoacetic acid (MAA) to increase the stability and sensitivity of the substrate for cost-effective and sensitive assessment of paraquat (PQ) residues in fruit samples. The morphological analysis of the substrate using TEM and STEM-EDS images indicated the uniformity in size and structure of the prepared nanoparticles. Further the modified substrate, MAA/Au@AgNRs showed excellent stability and sensitivity in comparison with its unmodified counterpart. For the evaluation of PQ residues in pear and apple fruit samples the modified substrate exhibited R 2 values of 0.9954 and 0.9914 with a low limit of detections of 0.012 and 0.024 ppm, and good percent recoveries of 80–110 % and 81–104 %, respectively. Thus, the study proved the effectiveness of the proposed MAA/Au@AgNRs substrate for assessing residues of herbicide in complex foods.
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