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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Interfacial assembly of bilayer plasmonic films with dynamic hotspot regulation for ultrasensitive surface-enhanced Raman spectroscopy detection

Yue Fang,Guangyao Huang,Sensen Hao,Jingyuan Shao,Ying Wang,Nan Liu,Zhenxing Li,Mancun Zhao,Lanxin Bao,Junping Wang,Hongzhi Wang

Interfacial assembly enables bilayer plasmonic SERS films; • Dynamic hotspot regulation governs multilayer SERS performance; • Ultrasensitive quantitative detection demonstrated in serum. Interfacial assembly of plasmonic nanostructures provides a versatile strategy for engineering Surface-enhanced Raman Spectroscopy (SERS) substrates, yet the fundamental mechanism governing multilayer SERS enhancement remains poorly understood. Here, we report interfacially assembled bilayer plasmonic films with precisely controlled Au nanoparticle layer numbers and uncover a previously unrecognized nonmonotonic enhancement behavior, in which the bilayer configuration unexpectedly outperforms both monolayer and multilayer counterparts through a dynamic hotspot regulation mechanism. The bilayer architecture exhibits optimal SERS performance, achieving ultralow limits of detection of 1.05 × 10 −14  M for crystal violet (CV) and 1.0 × 10 −11  M for paclitaxel (PTX) with excellent reproducibility (RSD < 5%). Time-resolved SERS measurements and Raman mapping reveal that solvent-driven analyte enrichment and interlayer nanogap evolution generate temporally stabilized plasmonic hotspots, producing a robust signal plateau window and establishing a direct structure–dynamics–performance relationship fundamentally distinct from conventional static hotspot amplification models. Benefiting from this mechanism, the bilayer films enable quantitative PTX detection in human serum with a limit of detection of 6.9 × 10 −10  M and show strong agreement with LC–MS analysis in 50 clinical samples (R 2  = 98.78%). Furthermore, in an orthotopic breast cancer mouse model, SERS-guided dose adjustment maintains antitumor efficacy while reducing systemic toxicity. This work not only provides insights into a previously unexplored mechanism of hotspot regulation in multilayer plasmonic assemblies but also provides a mechanistically guided interfacial engineering strategy for designing robust SERS substrates for ultrasensitive quantitative detection in complex biological environments. Scheme 1. Dynamic hotspot regulation arising from interlayer nanogap evolution and analyte enrichment establishes a structure–dynamics–performance correlation in bilayer plasmonic films. This mechanism produces a stable signal plateau window and enables ultrasensitive and quantitative paclitaxel monitoring for precision chemotherapy. Download: Download high-res image (164KB) Download: Download full-size image

✓ 已验证 DOI 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Microplastics emerge as a hotspot for dibutyl phthalate sources in rivers and oceans: Leaching behavior and potential risks

Lujian Lin,Bo Yuan,Huiling Liu,Yue Ke,Weifeng Zhang,Hanyi Li,Haoliang Lu,Jingchun Liu,Hualong Hong,Chongling Yan

Dibutyl phthalate (DBP) as a plasticizer has been widely used in the processing of plastic products. Nevertheless, these DBP additives have the potential to be released into the environment throughout the entire life cycle of plastic products. Herein, the leaching behavior of DBP from PVC microplastics (MPs) in freshwater and seawater and its potential risks were investigated. The results show that the plasticizer content, UV irradiation , and hydrochemical conditions have a great influence on the leaching of DBP from the MPs. The release of DBP into the environment increases proportionally with higher concentrations of additive DBP in MPs, particularly when it exceeds 15 %. The surface of MPs undergoes accelerated oxidation and increased hydrophilicity under UV radiation , thereby facilitating the leaching of DBP. Through 30 continuous leaching experiments, the leaching of DBP from MPs in freshwater and seawater can reach up to 12.28 and 5.42 mg g -1 , respectively, indicating that MPs are a continuous source of DBP pollution in the aquatic environment . Moreover, phthalate pollution index (PPI) indicates that MPs can significantly increase DBP pollution in marine environment through land and sea transport processes. Therefore, we advocate that the management of MPs waste containing DBP be prioritized in coastal sustainable development .

CAS / MDL: 109-99-9
研究领域: 环境科学 · 海洋生物学
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BIOSENSORS & BIOELECTRONICS · 2025 · IF 10.5

Hotspot-enhanced SERS Biosensor: Triplex noble nanoparticle-aptamer supramolecules on micropatterned silicon for simultaneous detection of foodborne pathogens

Ningtao Cheng,Yuling Deng,Xinmei Cao,Yi Tao

Foodborne pathogens significantly impact public health and cause substantial economic losses globally, necessitating rapid, sensitive, and multiplex detection techniques. This study presents a novel surface-enhanced Raman spectroscopy (SERS) biosensor enabling highly sensitive and simultaneous detection of Salmonella enteritidis ( S. enteritidis ) and Pseudomonas aeruginosa ( P. aeruginosa ). The biosensor utilizes sculpted triangular silicon substrates (stSi) decorated uniformly with silver (Ag) and gold (Au) nanoparticles (stSi@Ag-Au), fabricated through electrochemical reduction and galvanic displacement methods, creating robust electromagnetic hotspots. Functional gold nanostars synthesized via a seed-mediated growth method were deposited onto stSi@Ag-Au, forming a Raman-active substrate, which was further modified with pathogen-specific aptamers and distinct Raman probes—5,5′-dithiobis(2-nitrobenzoic acid) (DTNB) for S. enteritidis and 4-(mercaptomethyl)benzonitrile (MMBN) for P. aeruginosa . These components assemble into supramolecular complexes capable of specifically recognizing target pathogens, generating intense, unique Raman signals in a concentration-dependent manner, enabling concurrent quantitative analysis of both pathogens. The developed method achieves rapid detection within 45 min, demonstrates a broad linear detection range (10°–10 5  CFU mL −1 ) with detection limits of 1.33 CFU mL −1 ( Salmonella enteritidis ) and 1.12 CFU mL −1 ( Pseudomonas aeruginosa ), and has been successfully validated in practical applications in diverse matrices, including drinking water, orange juice, and Dendrobium nobile Lindl. juice samples, underscoring its effectiveness for rapid food safety assessments. Overall, this supramolecular-based SERS biosensing strategy provides a highly sensitive, rapid, and reliable solution for simultaneous pathogen detection, significantly advancing capabilities in foodborne disease prevention and control.

CAS / MDL: 69-78-3
研究领域: 生物传感器 · 纳米技术 · 分析化学 · 食品安全 · 微生物学 · 表面增强拉曼光谱(SERS) · 超分子化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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NEW JOURNAL OF CHEMISTRY · 2025 · IF 2.5

Synergistic effect of boric acid affinity magnetic materials and multi-hotspot SERS substrates for high sensitivity detection of glucose

Zhiyuan Sun,Gege Zhao,Ming Guan,Huixian Li,Fang Mi,Xiaobo Ma,Yajun Zhao,Han Song

In this work, boric acid affinity magnetic materials and Au nanorods capped by Ag (AuNRs@Ag) core-shell structure were used to construct the sandwich structure to obtain surface-enhanced Raman scattering (SERS) sensor for detecting glucose. The AuNRs@Ag modified with 4-mercaptophenylboronic acid (4-MPBA) as SERS substrate, illustrating the efficient electromagnetic enhancement. Moreover, the boric acid affinity magnetic materials (FMNPs) were further functionalized with knife bean lectin as “capture probe”, which illustrated the high adsorption capacity to glucose. The maximum adsorption amount can reach 33.3 mg/g. The conditions for preparing SERS platform as well as glucose detection were optimized. Under the optimal experimental conditions, the detection linear range for glucose is 1.0×10-11 ~ 1.0×10-3 mol/L with a limit of detection (LOD) 1.8×10-12 mol/L (S/N = 3). In addition, the developed SERS sensor was further applied for determination of glucose in human urine with recoveries in the range from 97.5% to 101.5%. As expected, the prepared sandwich SERS sensor was successfully employed to recognize and detect glucose with high sensitivity.

研究领域: 分析化学 · 生物医学工程 · 纳米技术
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BIOSENSORS & BIOELECTRONICS · 2024 · IF 10.7

Enhanced quasi-meshing hotspot effect integrated embedded attention residual network for culture-free SERS accurate determination of Fusarium spores

Yehang Wu,Pan Li,Tao Xie,Rui Yang,Rui Zhu,Yulong Liu,Shengyu Zhang,Shizhuang Weng

Determination of Fusarium spores is essential for precision control of Fusarium head blight and ensuring agri-food safety. As a highly sensitive real-time detection technique with rich fingerprint information and little influence from water, surface-enhanced Raman spectroscopy (SERS) has been widely applied in the determination of microorganisms. However, fungi determination faces significant challenges including low sensitivity, and poor specificity. The enhanced quasi-meshing hotspot effect (EQMHE) integrated with the embedded attention residual network (EARNet) was proposed to realize a label-free and accurate SERS determination of various Fusarium spores. The EQMHE can promote the binding of spores and nanoparticles to form numerous hotspots, significantly enhancing signal quality and improving the detection limit by at least four orders of magnitude. The key factors inducing EQMHE were validated through various characterization techniques. Moreover, due to its excellent feature extraction and recognition capabilities, EARNet successfully overcomes the limitations of spectral similarity, achieving determination accuracies of 100% in the training set, 98.33% in the validation set, and 100% in the prediction set for three Fusarium species from actual samples. EARNet requires only a small amount of training data and provides rapid and accurate diagnostics. Throughout the process, the spores do not require culturing or lysing, providing an effective determination method for the practical determination of mixed fungal spores. Overall, the proposed strategy effectively addresses challenges such as the need for fungal spore cultivation, difficulties in SERS hotspot formation, and suboptimal signal quality, and it holds significant promise for applications in disease control, food safety, and agricultural production.

CAS / MDL: 7761-88-8 68-04-2
研究领域: 植物病理学 · 食品安全 · 农业科学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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ANALYST · 2023 · IF 4.2

Highly sensitive and selective SERS detection of caspase-3 during cell apoptosis based on the target-induced hotspot effect

Yueyuan Zhuang,Han Dong,Tianqing Liu,Yongmei Zhao,Yan Xu,Xiaojuan Zhao,Dan Sun

Caspase-3 is an important biomarker for the process of apoptosis, which is a key target for cancer treatment. Due to its low concentration in single cells and the structural similarity of caspase family proteins, it is exceedingly challenging to accurately determine the intracellular caspase-3 during apoptosis in situ. Herein, a biosensing strategy based on the target-induced SERS “hot spot” formation has been developed for the simultaneous highly sensitive and selective detection of intracellular caspase-3 level. The nanosensor is composed of gold nanoparticles modified with the probe molecule 4-mercaptophenylboronic acid (4-MPBA) and a peptide chain. The well-designed peptide chain contains two distinct functional domains, one with a sulfhydryl group for bonding to the gold nanoparticles and the other a fragment specifically recognized by caspase-3. When caspase-3 is present, the negatively charged segment (NH2–Asp–Asp–Asp–Glu–Val–Asp–OH) of the peptide chain is specifically hydrolyzed, leaving a positively charged fragment coated on the surface of the gold nanoparticles. At this time, the golden nanoparticles undergo significant coupling aggregation due to the electrostatic interaction, resulting in a large number of SERS “hot spot” formation. The SERS signal of the 4-MPBA located at the nano-gap is significantly boosted because of the local plasma enhancement effect. The highly sensitive determination of caspase-3 can be achieved according to the altered SERS signal intensity of 4-MPBA. The turn-on of the SERS signal-induced target contributes to the excellent selectivity and the formation of the SERS “hot spot” effect that further improves the sensitivity of caspase-3 detection. The advantages of this biosensing technique allow for the precise in situ monitoring of the dynamic changes in caspase-3 levels during apoptosis. In addition, the differences in caspase-3 levels during the apoptosis of various cell types were compared. Monitoring the caspase-3 levels can be used to track the cellular apoptosis process, evaluate the effect of drugs on cancer cells in real time, and provide guidance for the selection of the appropriate drug dosage.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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BIOORGANIC CHEMISTRY · 2022 · IF 5.307

Directed evolution of a carbonyl reductase LsCR for the enantioselective synthesis of (1S)-2-chloro-1-(3,4-difluorophenyl) ethanol

Hua-Tao Liu,Chun-Yue Weng,Shen-Yuan Xu,Shu-Fang Li,Ya-Jun Wang,Yu-Guo Zheng

Traditional screening methods of enzyme engineering often require building large mutant libraries to screen for potentially beneficial sites, which are often time-consuming and labor-intensive with low mining efficiency. In this study, a novel enzyme engineering strategy was established to modify carbonyl reductase Ls CR for the synthesis of (1 S )-2-chloro-1-(3,4-difluorophenyl) ethanol (( S )-CFPL), which is a key intermediate of anticoagulant drug ticagrelor. The strategy was developed by combining HotSpot, FireProt and multiple sequence alignment, resulting in the construction of a “small and smart” mutant library including 10 mutations. Among them, 5 mutations were positive, resulting in a 50% mining accuracy of beneficial sites. Finally, a highly active mutant Ls CR M3 (N101D/A117G/F147L) was obtained by further screening through saturation mutation and iterative mutation. Compared with wild type (WT) Ls CR, the catalytic activity of Ls CR M3 was increased by 4.7 times, the catalytic efficiency k cat / K M value was increased by 2.9 times, and the half-life t 1/2 at 40 °C was increased by 1.3 times. Due to the low aqueous solubility of the substrate 2-chloro-1-(3,4-difluorophenyl) ethanone (CFPO), isopropanol was used as not only the co-substrate but also co-solvent. In the presence of 40% ( v / v ) isopropanol, Ls CR M3 completely reduced 400 g/L CFPO to enantiomerically pure CFPL (99.9%, e.e. ) in 11 h with a space–time yield (STY) as high as 809 g/L∙d.

研究领域: 酶工程 · 生物催化 · 化学生物学 · 药物化学
✓ 已验证 DOI PubMed 高影响因子
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BIOSENSORS & BIOELECTRONICS · 2024 · IF 10.7

CRISPR/dCas9-based hotspot self-assembling SERS biosensor integrated with a smartphone for simultaneous, ultrasensitive and robust detection of multiple pathogens

Han Jiang,Xiaofan Zhu,Jingran Jiao,Chao Yan,Kaiyong Liu,Wei Chen,Panzhu Qin

Accurate detection of multiple pathogens in the early stages of infection is critical for guiding treatment and saving patients' lives, but current methods are still challenged by low sensitivity, poor robustness and long turnaround times. Here, we report a CRISPR/dCas9-based hotspot self-assembling surface-enhanced Raman scattering (SERS) biosensor (called dCasSERS) and its integration with a smartphone to address these challenges. In this design, bacterial DNA was pre-amplified by loop-mediated isothermal amplification (LAMP), and the repeat sequences of the amplicons were recognized by CRISPR/dCas9, providing abundant sites for the assembly of gold nanoparticles (AuNPs) and forming numerous hotspots for SERS analysis. Using AuNPs labeled with different Raman molecules as reporters, the presence of Staphylococcus aureus ( S. aureus ), Pseudomonas aeruginosa ( P. aeruginosa ) and Escherichia coli O157:H7 ( E. coli O157:H7) could be dexterously converted into distinguishable SERS signals. CRISPR/dCas9-based amplicon-specific recognition and SERS hotspot self-assembly improved the specificity and sensitivity, enabling the biosensor to simultaneously detect three target pathogens down to 1 CFU/mL without any cross-reactivity. By introducing a rapid extraction procedure and a smartphone-integrated handheld Raman spectrometer, rapid on-site analysis of multiple pathogens could be achieved in less than 50 min. The accuracy and robustness of the biosensor were demonstrated by 500 real urine specimens. This study displays a new paradigm for CRISPR/Cas-based self-assembly of SERS hotspots and provides insight into the future development of pathogen screening tools.

CAS / MDL: 69-78-3
研究领域: 分子生物学 · 医学诊断 · 纳米技术
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2024 · IF 4.3

Development of Fe3O4/DEX/PDA@Au(Raman reporters)@Au-MPBA nanocomposites based multi-hotspot SERS probe for ultrasensitive, reliable, and quantitative detection of glucose in sweat

Lun Han,Xu Wang,Bin Yu,Xiaoyuan Qin,Baocheng Liu,Xu Han,Huifen Yuan,Bin Yu,Zhiqi Zhao

Glucose is a key biomarker of diabetes, and effective glucose monitoring methods are crucial to the prevention and management of diabetes. Therefore, in this paper, Fe 3 O 4 /DEX/PDA@Au (Raman reporters) @Au nanocomposites were synthetized that with DTNB (5,5′-dithiobis(2-nitrobenzoic)), MMTA (2-mercapto-4-methyl-5-thiazole acetic acid), MBA (4-mercaptobenzoic acid) and 4-Mpy(4-Mercaptopyridine) were used separately as Raman reporters. Fe 3 O 4 and PDA (Polymerized dopamine) could supply more high surface area of active sites and high SERS (Surface-Enhanced Raman Scattering) substrate, which has high stability and reproducibility. Dextran coating is an effective way to prepare biocompatible materials TEM, XRD, TG and VSM were used to analyze the size, morphology and magnetic properties of the nanocomposites. Fe 3 O 4 /DEX/PDA@Au(Raman reporters)@Au that integrates a multi-hotspot structure and magnetic separation techniques were studied the enhancement effect of Raman spectra, and glucose solutions with different concentrations were tested. Furthermore, the optimal Fe 3 O 4 /DEX/PDA@Au(Raman reporters)@Au nanocomposites were supplied as SERS substrates for detection of glucose accurately and quickly in sweat. SERS signal intensity is linearly correlated with glucose concentration within the measurement range of 5 × 10 -3 to 10 mM, and the minimum detectable concentration is 5 µM. The Fe 3 O 4 /DEX/PDA@Au(Raman reporters)@Au nanocomposites exhibit high reliability, specificity and repeatability of the strategy were then verified by practical detection of sweat.

研究领域: 生物医学工程 · 分析化学
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