MICROCHIMICA ACTA
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2024
·Vol. 191
·期 7
·1-12
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IF 5.3
Wu Huqi,Gao Yan,Chen Qi,Yao Li,Yao Bangben,Yang Jielin,Chen Wei
The engineering of a home-made portable double-layer filtration and concentration device with the common syringe for rapid analysis of water samples is reported. The core elements of the device were two installed filtration membranes with different pore sizes for respective functions. The upper filtration membrane was used for preliminary intercepting large interfering impurities ( interception membrane ), while the lower filtration membrane was used for collecting multiple target pathogens ( enrichment membrane ) for determination. This combination can make the contaminated environmental water, exemplified by surface water, filtrated quickly through the device and just retained the target bacteria of Escherichia coli O157:H7, Staphylococcus aureus , and Listeria monocytogenes on the lower enrichment membrane. Integrating with surface-enhanced Raman spectra (SERS) platform to decode the SERS-Tags (SERS-Tag CVa , SERS-Tag R6G , and SERS-Tag MB ) already labeled on each of the enriched bacteria based the antibody-mediated immuno-recognition effect, fast separation, concentration, and detection of multiple pathogenic bacteria from the bulk of contaminated environmental water were realized. Results show that within 30 min, all target bacteria in the lake water can be simultaneously and accurately measured in the range from 10 1 to 10 6 CFU mL −1 with detection limit of 10.0 CFU mL −1 without any pre-culture procedures. This work highlights the simplicity, rapidness, cheapness, selectivity, and the robustness of the constructed method for simultaneous detecting multiple pathogens in aqueous samples. This protocol opens a new avenue for facilitating the development of versatile analytical tools for drinking water and food safety monitoring in underdeveloped or developing countries. Graphical abstract
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2024
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IF 5.4
Dechan Lu,Bohan Zhang,Zhikun Shangguan,Yudong Lu,Jingbo Chen,Zufang Huang
Exosomes, extracellular vesicles released by cells, hold potential as diagnostic markers for the early detection of lung cancer. Despite their clinical promise, current technologies lack rapid and effective means to discriminate between exosomes derived from adenocarcinoma in situ (AIS) and early-stage invasive adenocarcinoma (IAC). This challenge arises from the intrinsic structural heterogeneity of exosomes, necessitating the development of advanced methodologies for precise differentiation. Here, we demonstrate a novel approach for plasma exosome detection utilizing multi-receptor surface-enhanced Raman spectroscopy (SERS) technology to differentiate between AIS and early-stage IAC. To accomplish this, we synthesized a stable and uniform two-dimensional SERS substrate (BC/Au NPs film) by fabricating gold nanoparticles onto bacterial cellulose. We then enhanced its capabilities by introducing multi-receptor SERS functionality via modifying the substrate with both low-specificity and physicochemical-selective molecules. Furthermore, by strategically combining all capturer-exosome SERS spectra, comprehensive “combined-SERS spectra” are reconstructed to enhance spectral variations of the exosome. Combining these features with partial least squares regression-discriminant analysis (PLS-DA) modeling significantly improved discriminatory accuracy, achieving 90% sensitivity and 95% specificity in distinguishing AIS from early-stage IAC. Our developed SERS sensor provides an effective method for early detection of lung cancer, thereby paving a new way for innovative advancements in diagnosing lung cancer.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Jinglei Yang,Bohan Zhang,Qingling Nie,Ruping Zheng,Ping Lin,Chuyi Wang,Yudong Lu,Yunli Xu,Ruiyun You
Uric acid, urea, and other metabolites in urine after exercise often reflect chronic injury syndrome in athletes. However, traditional urine detection methods have issues such as high costs and low detection sensitivity. SERS can rapidly, continuously, and sensitively monitor metabolites in human urine. In this research, a combined SERS substrate (CMBCM@Ag NPs@PGA) was developed based on the carboxymethyl modification of the bacterial cellulose membrane (BCM) surface. The numerous carboxyl groups on the CMBCM surface made it easier for silver ions to be adsorbed, leading to their conversion into silver nanoparticles (Ag NPs) when a reducing agent was introduced. This process allowed the nanoparticles to firmly adhere to the CMBCM surface, forming a uniform and stable “hot spot.” “The CMBCM@Ag NPs@PGA substrate maintains excellent stability and sensitivity in the assay.” It can detect very small amounts of urea and uric acid in urine with high sensitivity, with LOD of 1.05 μM for urea and 0.0075 μM for uric acid. Additionally, it exhibits good stability, antibacterial properties, and cell compatibility. In addition, the substrate can be used as a sensor to monitor pH in real-time. This expands the use of cellulose in flexible SERS sensing and detecting human exercise metabolic health.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Chen Chen,Ximo Wang,Xinyue Wang,Geoffrey I.N. Waterhouse,Ruiqiang Wang,Yufeng Sun,Zhixiang Xu
Surface-enhanced Raman spectroscopy (SERS) is a powerful tool for the detection of target analytes in foods, with the realization of “hot spots” between plasmonic metal nanoparticles (NPs) being critical for ultrasensitive detection. Herein, we proposed a new aptamer conformation-mediated SERS “hot spots” strategy. Au NPs were functionalized with strands of complementary DNA containing β-phenethylamine aptamers and the Raman reporter 4-mercaptobenzonitrile (4-MBN). This allowed DNA-driven self-assembly of an Au dumbbell dimer-based SERS aptasensor for the detection of the β-phenethylamine. After selective recognition of β-phenethylamine by the aptamer, the aptamer folded, bringing AuNPs in the dimers close together to create SERS “hot spots”. This produced an intense SERS signal in the “biologically silent” region for 4-MBN (2225 cm −1 ), the intensity of which increased linearly with the logarithm of the β-phenethylamine concentration. Under the optimized conditions, the linear range of SERS aptasensor was 10 −6 to 10 −2 mg L −1 , with a low limit of detection of 3.8 × 10 −7 mg L −1 . Further, the developed SERS aptasensor was successfully employed to determine the β-phenethylamine in a range of food samples, with the results being identical to those obtained using a high-performance liquid chromatography method.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Xiaoming Su,Xinyu Liu,Yuzhen Ouyang,Yangcenzi Xie,Mingyang Chen,Pan Chen,Jia Liu,Minghua Wu,Chien-hong Lin,Hong Zhong,Ming Li
Operative microwave ablation (MWA) has become a superior curative treatment modality for unresectable hepatocellular carcinoma (HCC). However, rapid noninvasive assessment of the MWA outcomes of HCC patients remains technically challenging. Herein, a surface-enhanced Raman spectroscopy (SERS)-lateral flow strip (LFS) immunosensor is reported for simultaneous quantification of two serum protein biomarkers – (C-C motif chemokine ligand 20) CCL20 and epidermal growth factor (EGF) proteins, which enables rapid noninvasive assessment of operative MWA outcomes of HCC patients. This biosensor is built with two test lines for CCL20 and EGF proteins using the encoded SERS probes, respectively. The integration of the SERS detection and the lateral flow immunoassay detection format yields high sensitivity, robust anti-interference ability, and ease-to-use. This biosensor achieves a limit of detection down to 0.064 ng/mL for CCL20 protein and 0.090 ng/mL for EGF protein with a wide dynamic detection range. Moreover, the SERS-LFS immunosensor is demonstrated with exceptional performance for quantitative detection of CCL20 and EGF proteins in clinical serum samples in a single test strip. The results reveal the discriminative levels of CCL20 and EGF proteins in serum samples of HCC patients undergoing complete and incomplete MWA, verifying the capability of our developed biosensor for rapid assessment of MWA outcomes. We believe that the developed SERS-LFS immunosensor could be applied to support medical professionals in clinical settings for improvement of MWA outcomes of HCC patients.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Mengqi He,Hao Wu,Xin Cai,Shuangyun Li,Shiting Cao,Xiaofang Zhao,Meifeng Xu,Chaonan Wang
In this work, hierarchical structure composed of periodic nanopillars and wrinkles was designed on flexible and transparent PDMS through a strategy combining template method and oxygen plasma treatment. Investigations on the SERS performance of the substrates obtained after Ag thermal deposition reveal both the nanopillars and the wrinkles contributed greatly to the enhancement. The formation of the periodic wrinkles followed the buckling theory. Under the condition of 30 % deformation and 40 W plasma power, by adjusting the deposition time to 30 min, dense distribution of Ag NPs on the hierarchical PDMS support was achieved while avoiding coverage of the nano wrinkles. The obtained substrate named Ag-30/PDMS-PW had an EF of 3.11×10 7 , excellent uniformity and outstanding reproducibility with an RSD of 2.13 % and 4.9 % respectively. Cyclic loading and tensile tests verify the mechanical stability and perfect elasticity of the Ag-30/PDMS-PW substrate. Coupled with the bi-direction excitation ability, the as-prepared substrate was fully qualified for in-situ detection of pesticide residues, which was demonstrated by the in-situ detection of thiram and thiabendazole on apple surface with concentrations lower than the maximum residue limits. The results manifest the proposed substrate has great potential for in-situ food safety monitoring in real-world applications.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2024
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IF 4.3
Weinan Dong,Jinsheng Guo,Chun Yu,Bao Guo,Kaixi Jiang
In the minerals processing industry, the surface chemistry of mineral particles and its real-time detection can significantly enhance process performance, and ultimately leading to automotive and intelligent control. The adsorption of collector molecule onto bulk mineral specimens could be investigated with the help of shell-isolated nanoparticle enhanced Raman spectroscopy (SHINERS). However, this method is unsuitable for the online detection of particles fluid consisted of micro-sized chalcocite that encountered in industrial production processes. In this work, a novel strategy of shell-isolated nanoparticles synthesis by electrodeposition of gold nanoparticles film and isolation of this film with crosslinked silica monolayer was proposed. The adsorption of 2-mercaptobenzothiazole (MBT), a typical flotation collector, onto a copper sulfide mineral, chalcocite was measured in-situ with the help of such a SERS substrate. Enhancement factors of 10 6 –10 7 was calculated based on an idealized model. Furthermore, we discussed the stability of the silica isolation monolayer under high-power laser irradiation.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Runzi Zhang,Shunbi Xie,Xiang He,Ying Gao,Mengjun Wang,Minghang Jiang,Xiaojun Luo,Yi He
Chloramphenicol (CAP), as a broad-spectrum antibiotic, is genotoxic to humans. In this paper, a “Y-shaped” SERS biosensor based on magnetic plasmonic superstructures Fe3O4@SiO2@Ag flowers and the highly efficient isothermal amplification strategy of exponential amplification reaction (EXPAR) technology was proposed for ultrasensitive detection of CAP in milk. This was achieved by forming a stable “Y-shaped” structure on the abundant sharp tips of Fe3O4@SiO2@Ag flowers through specific three-part assembly (Probe 1 connected to the magnetic substrate, Signal Probe 2 Au@4-NTP, and the EXPAR amplification product Amplicon). When the CAP was present, the Amplicon obtained from EXPAR amplification could form a “Y-shaped” structure with the magnetic material and the signal probe. Benefiting from the abundant branching, extensive surface area, and rough surface of the magnetic Fe3O4@SiO2@Ag flower, it offers a multitude of “hot spots” for plasmonic coupling in the electromagnetic field gap region and significantly reduces the nanogap between the signal probe and the silver nanoflowers by constructing a “Y”-shaped structure, thereby maximizing the amplification of the Raman signal. Enabling the detection range of CAP to be between 10–6 and 10–13 M with a detection limit of 17.9 fM. This strategy provided an avenue for trace detection of CAP in food.
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Analytical Methods
·
2025
·
IF 2.6
Shuxian Ren,Jihong Fu,Guoqi Liu,Haipeng Zhang,Boshen Wang,Junli Yu
The unreasonable use of organic dye leads to excessive residues in environmental water, which seriously threatens human health and the natural environment. In this paper, a spherical flower-like magnetic Fe3O4@CoNi layered double hydroxide@silver nanoparticle (Fe3O4@CoNi LDH@Ag NPs) SERS substrate was successfully fabricated via electrostatic self-assembly and applied for the sensitive detection of methylene blue (MB) in environmental water. The rapid concentration and separation of the SERS substrate from the water sample could be achieved using an external magnet. The Fe3O4@CoNi LDH@Ag NPs could not only rapidly enrich the trace analytes because of their outstanding absorptive capacity but also effectively enrich the cationic dye molecules to the “hot spots” through electrostatic interactions, resulting in higher SERS selectivity. Excellent SERS performance was observed, which exhibited a high enhancement factor (EF) of 5.81 × 108 and a low detection limit (LOD) of 1 × 10−11 mol L−1 with R6G as the probe molecule, and also possessed exceptional reproducibility and stability for at least 28 days. The Fe3O4@CoNi LDH@Ag NPs were used to detect MB, which displayed wide linearity (1 × 10−10 to 1 × 10−4 mol L−1) and high recoveries (89.68–103.72%). This Fe3O4@CoNi LDH@Ag NP substrate offers easy separation and selective detection of cationic dyes, providing potential application for the detection of environmental contaminants.
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RARE METALS
·
2025
·
IF 11
Guo Jing,Mu Zhi-Mei,Yu Jing,Sun Guan-Liang,Hou Lin-Rui,Qiao Xue-Zhi,Yang Shi-Kuan,Zhang Xing-Shuang,Xu Guan-Chen,Liu Guo-An,Yang Fan,Yuan Chang-Zhou,Liang Xiu
Metal–organic framework materials exhibit considerable potential as molecularly selective surface-enhanced Raman spectroscopy (SERS) substrates because of their microporous structures, which enrich small molecules while excluding larger ones. In this study, we develop a template-assisted chemical-etching strategy to prepare layered tuneable SERS substrates based on hierarchical porous zeolitic imidazolate framework-67 (HP-ZIF-67) with a rhombic dodecahedral structure. The synergistic SERS enhancement mechanisms of HP-ZIF-67, which combine electromagnetic (EM) and chemical (CM) effects, were systematically studied through numerical simulations and experiments. Calculations revealed that under 633-nm laser excitation, the contributions of the EM and CM effects to the total SERS enhancement factor of HP-ZIF-67 were 60% and 40%, respectively. The hierarchical porous structure enhanced the fluid-flow flux over the microporous ZIF-67 because the increased pore radius reduced the viscous resistance and facilitated rapid molecular transport through the interconnected macro-meso-channels. Precise modulation of the CM and EM effects, combined with enhanced mass transfer, facilitated the development of HP-ZIF-67 and HP-ZIF-67@Au as efficient SERS sensors. An investigation of the relationship between pore-size distribution and EM effects revealed the pivotal role of light confinement by whispering-gallery-mode microcavities in enhancing the SERS performance. The optimised HP-ZIF-67@Au composites functioned as flexible and highly sensitive in situ SERS sensors for gases and liquids, including volatile organic-compound gas and liquid-pesticide residues. This study introduces a novel design concept and provides a robust theoretical foundation for the future development of exhaled-breath point-of-care diagnostic devices and sweat-based wearable biomedical sensors. Graphical abstract
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Jing Shang,Feina Niu,Zhiwei Cai,Yindong Tan,Yaxing Zhang,Runan Tan,Hanping He,Yunbin He,Gang Chang
Surface-enhanced Raman scattering (SERS) technology is limited in the direct detection of molecules with weak Raman scattering such as methyl parathion (MP). Development of an indirect detection strategy for weakly Raman active substances is essential. Herein, a novel SERS detection method was developed for the inhibition-type indirect detection of MP with ZrO 2 -coated silver nanowires (AgNWs@ZrO 2 ) as substrate. The mechanism relies on specific MP adsorption through Zr 4+ Lewis acid sites and P/S-ZrO 2 interactions, which spatially and electronically suppresses 4-MBA probe signals, and then the quantitative relationship between the measured object and the decline value of Raman intensity can be established. With the gradual increase of MP concentration in the range of 0.5 ng/mL ∼ 1 μg/mL, the SERS intensity of 4-MBA decreased accordingly, showing a good linear relationship (R 2 = 0.996), and the analytical enhancement factor (AEF) reached 1.6 × 10 6 , overcoming traditional SERS limitations for the molecules with weak Raman scattering. The ZrO 2 layer maintains electromagnetic coupling while preventing oxidation, thereby enhancing the reproducibility, uniformity and stability of the substrate during the analysis process. The prepared AgNWs@ZrO 2 was successfully applied for trace detection of MP residues in pear peel and apple juice. This study is expected to provide a simple and feasible method for trace detection of the molecules with weak SERS activity.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Xiaoya Yuan,Mantang Chen,Yuhan Guo,Xiaoyu Wang,Junwei Guo,Fuwei Xie,Cong Nie,Qin Shuai,Lei Ouyang
The trace detection of both aqueous and gaseous nicotine is significant for health monitoring and environmental analysis. In this study, a novel covalent organic framework (COF)-based composite was designed to enrich and detect nicotine using surface-enhanced Raman scattering. The negatively charged TpPa-SO 3 H exhibited exceptional enrichment capabilities for nicotine, demonstrating an adsorption capacity of 148.0 mg·g −1 . Chemical interactions, including π-π stacking and acid-base interactions, were observed between the COFs and nicotine molecules. Furthermore, chemical enhancement induced by electron transfer between TpPa-SO 3 H and nicotine was corroborated through energy level analysis. By leveraging the bimetallic synergism between core-shell Au and Ag to achieve electromagnetic enhancement, the TpPa-SO 3 H-Au@Ag composite achieved a detection limit of 6.0 × 10 −10 mol·L −1 for aqueous nicotine. The detection of nicotine in e-cigarette oil and Cambridge filter demonstrates its application capability for different kinds of real samples. By the crosslinking with chitosan, the synthesized aerogel was successfully applied for the on-site gaseous nicotine detection in cigarette smoke. Additionally, the plasmonic aerogel enabled the identification of different kinds of cigarettes using artificial intelligence-assisted gaseous fingerprint spectra recognition and classification.
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