Surfaces and Interfaces
·
2023
·
IF 6.2
Qingyan Han,Yunxiang Li,Ye Chen,Shixing Fan,Yibin Hu,Ronghua Yan,Wei Gao,Chengyun Zhang,Wenwen Zhang,Jun Dong
Surface-enhanced Raman scattering (SERS) has tremendous significance in the fields of ultrasensitive detection and real-time in situ monitoring in catalysis. However, it remains a challenge to simultaneously achieve higher-quality SERS and excellent plasmonic catalytic properties in a nano/microstructure substrate under random excitation light. Here, we propose the design of a three-dimensional (3D) popcorn-like silver (Ag) microstructure (MS) with diameter of 1.2 ± 0.1 µm and a unique rough surface topography , realize a wide surface plasmon resonance (SPR) band ranging from 300 nm to 1100 nm, approximating a full spectrum. The popcorn-like Ag MSs with full-spectrum property effectively broaden the spectral overlap between the SPR band and wavelength of excitation light or absorption of probe molecules. Moreover, the 3D popcorn-like Ag MSs were used to construct a monolayer film array substrate on silicon wafer with a good homogeneity over large areas by an interfacial self-assembly method. The monolayer Ag MSs film array substrate can provide abundant “hot spots” and present excellent SERS performance for sensitive detection of Rhodamine 6G (Rh6G) with a low detection limit of 10 −9 M. The single-layer Ag MSs film array with superior SERS activity is utilized for in situ monitoring the plasmonic catalytic kinetics of 4-nitrothiophenol (4-NTP) dimerized into 4, 4′-dimercaptoazobenzene (DMAB) under 532 nm and 785 nm excitation, respectively. The mechanism on plasmonic catalytic reaction of the popcorn-like Ag MSs substrate is systemically investigated by experimental and theoretical simulations aspects. The Ag MSs film array substrate will offer a new strategy to further explore applications of SERS in sensors, photocatalysis , and bio/chemical analysis.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2023
·
IF 4.3
Chen Yi,Jiang Cailing,Huang Feixiang,Yu Zizhen,Jiang Li
Combining the unique advantages of two-dimensional transition metal carbon/nitrogen compounds (MXene) and the excellent surface-enhanced Raman scattering (SERS) performance of noble metal materials, MXene/Ag NPs films were proposed as nanocarriers for SERS-traceable drug delivery. The films were prepared by two-step self-assembly on positively charged silicon wafers using virtue of the high evaporation of ethyl acetate, the Marangoni effect, and an oil/water/oil three-phase system. With 4-mercaptobenzoic acid (4-MBA) as the probe molecule, the SERS detection limit was 10 −8 M and had shown a good linear relationship in the range of 10 −8 –10 −3 M. Simultaneously, the film had good uniformity, repeatability, and stability. When Ti 3 C 2 T x /Ag NPs films were used as nanocarriers, the anticancer drug doxorubicin (DOX) was loaded onto the surface through 4-MBA, and the tracking and monitoring were realized by SERS. The addition of glutathione (GSH) triggered the thiol exchange reaction, resulting in the shedding of 4-MBA from the surface of the film, which indirectly achieved the efficient release of DOX. Furthermore, the loading of DOX and the drug release effect triggered by GSH maintained a certain stability in serum, which provided a potential possibility for the subsequent loading and release of drugs by films with three-dimensional structures as scaffolds in biological therapy. Graphical abstract
Self-assembled MXene/Ag NPs film nanocarriers for SERS-traceable drug delivery and GSH-triggered high-efficiency drug release
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 11
·4288
·
IF 4.6
Yongping Li,Haohui Liao,Shaobing Wu,Xiaoyu Weng,Yiping Wang,Liwei Liu,Junle Qu,Jun Song,Shuai Ye,Xiantong Yu,Yu Chen
ReS2, as a new member of transition metal dichalcogenides (TMDCs), has emerged as a promising substrate for semiconductor surface-enhanced Raman spectroscopy (SERS) due to its unique optoelectronic properties. Nevertheless, the sensitivity of the ReS2SERS substrate poses a significant challenge to its widespread application in trace detection. In this work, we present a reliable approach for constructing a novel ReS2/AuNPs SERS composite substrate, enabling ultrasensitive detection of trace amounts of organic pesticides. We demonstrate that the porous structures of ReS2nanoflowers can effectively confine the growth of AuNPs. By precisely controlling the size and distribution of AuNPs, numerous efficient and densely packed “hot spots” were created on the surface of ReS2nanoflowers. As a result of the synergistic enhancement of the chemical and electromagnetic mechanisms, the ReS2/AuNPs SERS substrate demonstrates high sensitivity, good reproducibility, and superior stability in detecting typical organic dyes such as rhodamine 6G and crystalline violet. The ReS2/AuNPs SERS substrate shows an ultralow detection limit of 10−10M and a linear detection of organic pesticide molecules within 10−6–10−10M, which is significantly lower than the EU Environmental Protection Agency regulation standards. The strategy of constructing ReS2/AuNPs composites would contribute to the development of highly sensitive and reliable SERS sensing platforms for food safety monitoring.Keywords:ReS2nanoflowers;ReS2/AuNPs complexes;surface-enhanced Raman spectroscopy;quantitative detection
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高影响因子
ANALYST
·
2023
·Vol. 148
·期 14
·3295-3305
·
IF 4.2
Yong Huang,Zhengqing Liu,Xiaogang Qin,Jia Liu,Yan Yang,Wei Wei
Highly sensitive protein biomarker detection is critical for the diagnosis of gastric cancer (GC), however the accurate and sensitive detection of low-abundance proteins in early-stage GC is still a challenge. Herein, a surface-enhanced Raman scattering frequency shift assay was performed on a developed microfluidic chip for the detection of GC protein biomarkers carcinoembryonic antigen (CEA) and vascular endothelial growth factor (VEGF). The chip is made up of three groups of parallel channels and each parallel channel consists of two reaction regions, enabling the simultaneous analysis of multiple biomarkers in multiple samples. The presence of CEA and VEGF in the sample can be captured by the 4-mercaptobenzoic acid (4-MBA)-conjugated antibody functionalized gold nano-sheet (GNS-) substrate, resulting in the Raman frequency shift. As a result, a typical Raman frequency shift of 4-MBA presented a linear relationship with the concentration of CEA and VEGF. The limit of detection (LOD) of the proposed SERS microfluidic chip reaches as low as 0.38 pg mL−1 for CEA and 0.82 pg mL−1 for VEGF. During the detection process, only one step of sample addition is involved, which eliminates the multiple reaction step-induced nonspecific adsorption and significantly increases the convenience and specificity. In addition, serum samples from GC patients and healthy subjects were tested and the results were in good agreement with the current gold-standard method ELISA, suggesting the potential application of the SERS microfluidic chip in clinical settings for early diagnosis and prognosis of GC.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yu-Fei Li,Can-Jun Zou,Xing-Biao Liu,Feng Gan,Ping-Ping Fang
The detection of pharmaceuticals has been a matter of concern among scientists and health researchers in the past few decades. However, it is still difficult to realize the sensitivity and selectivity detection of pharmaceuticals with similar structures. Herein, the pharmaceutical molecules of 2-mercaptobenzimidazole (MBI) and 2-mercaptobenzothiazole (MBT) with so similar structures can be selectively detected by surface-enhanced Raman spectroscopy (SERS) taking advantage of the fingerprint identification on Au/MIL-101(Cr), with sensitive detection limits of 0.5 ng·mL–1 for MBI and 1 ng·mL–1 for MBT. MBI is selectively enriched by Au/MIL-101(Cr) from the mixture solution and detected by SERS below 30 ng·mL–1. MBI can also be selectively detected in the serum samples with a detection limit of 10 ng·mL–1. Density functional theory calculations combined with the SERS experiments explained that the high sensitivity and selectivity are caused by the intrinsic differences in Raman intensity and different adsorption energies from the pharmaceutical molecules adsorbed on Au/MIL-101(Cr), respectively. This study provides an effective way to enrich and detect pharmaceutical molecules with similar structures.
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TALANTA
·
2023
·
IF 6.1
Keyu Yi,Zilin Fan,Qimeng Ran,Kun Jia,Xiaobo Liu,Lei Wang
Flexible surface enhanced Raman spectroscopy (SERS) nanosensors, constructed by integration of plasmonic nanostructures with polymeric substrates, have received increasing research interests for recent decades. When compared to abundant works on optimization of the plasmonic nanostructures, the research involving the influence of polymeric substrates on analytical performance of resultant flexible SESR nanosensors is unexpectedly limited. Herein, the ultra-thin silver layer has been deposited on the electrospun polyurethane (ePU) nanofibrous membranes via vacuum evaporation to prepare the flexible SRES nanosensors. Interestingly, we find that the molecular weight and polydispersion index of synthesized PU play important roles in regulating the fine morphology of electrospun nanofibers , which in turns determine the Raman enhancement of resultant flexible SERS nanosensors. Specifically, the optimized SERS nanosensor, obtained by evaporating 10 nm silver layer on top of nanofibers derived from electrospinning of PU with a weight-average molecular weight of 140,354 and polydispersion index of 1.26, enables label-free detection of the carcinogen of aflatoxin down to 0.1 nM. Thanks to its scalable fabrication and good sensitivity, the current work opens new way for design of cost-effective flexible SERS nanosensors for environmental monitoring and food security applications.
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Nanomaterials
·
2023
·Vol. 13
·期 11
·1733
·
IF 5.3
Pei Zeng,Mengjie Zheng,Hao Chen,Guanying Chen,Zhiwen Shu,Lei Chen,Huikang Liang,Yuting Zhou,Qian Zhao,Huigao Duan
Seeking sensitive, large-scale, and low-cost substrates is highly important for practical applications of surface-enhanced Raman scattering (SERS) technology. Noble metallic plasmonic nanostructures with dense hot spots are considered an effective construction to enable sensitive, uniform, and stable SERS performance and thus have attracted wide attention in recent years. In this work, we reported a simple fabrication method to achieve wafer-scale ultradense tilted and staggered plasmonic metallic nanopillars filled with numerous nanogaps (hot spots). By adjusting the etching time of the PMMA (polymethyl methacrylate) layer, the optimal SERS substrate with the densest metallic nanopillars was obtained, which possessed a detection limit down to 10−13M by using crystal violet as the detected molecules and exhibited excellent reproducibility and long-term stability. Furthermore, the proposed fabrication approach was further used to prepare flexible substrates; for example, a SERS flexible substrate was proven to be an ideal platform for analyzing low-concentration pesticide residues on curved fruit surfaces with significantly enhanced sensitivity. This type of SERS substrate possesses potential in real-life applications as low-cost and high-performance sensors.Keywords:SERS;hot spots;large-scale production;sensitivity;flexible substrate
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Huanhuan Sun,Hongyan Yu,Boyang Han,Junjie Ma,Rensheng Wang,Yanping Song
Pressure-induced surface-enhanced Raman spectroscopy (PI-SERS) is among the foremost achievements of high-pressure fields, benefiting from the advantage that pressure-modulated interactions between substrates and molecules overcome the weakness of individual substrates or molecules. However, the pressure corresponding to PI-SERS enhancement is currently still at a low-pressure stage within 8 GPa. Therefore, how to realize PI-SERS enhancement under higher or ultrahigh pressure remains a huge challenge. Here, we applied few-layer WS2 (FL-WS2) nanosheets as PI-SERS substrates and selected 4-mercaptobenzoic acid (4-MBA) molecules with a big energy gap as probes to explore PI-SERS enhancement in more depth. The experimental results indicate that the PI-SERS signals increase gradually as pressure increases and reaches a maximum at 18 GPa, which has set a pressure record for the PI-SERS field so far. Different from the C exciton resonance-induced SERS intensities at ambient conditions, the charge-transfer transition between FL-WS2 and 4-MBA is strengthened via the pressure-induced increase in the band gap of FL-WS2 and decrease in the highest-occupied molecular orbital–lowest unoccupied molecular orbital (HOMO–LUMO) energy gap of 4-MBA, thus enhancing PI-SERS signals accordingly. Therefore, this strategy will be beneficial for practical applications in the field of optoelectronics and for the design of other PI-SERS sensors for trace detection in complex and extreme environments.
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VIBRATIONAL SPECTROSCOPY
·
2023
·
IF 2.5
Tian Wang,Hong-Mei Li,Bao-Ying Wen,Rajapandiyan Panneerselvam,Yue-Jiao Zhang,An Wang,Fan-Li Zhang,Shangzhong Jin,Jian-Feng Li
Dioxin is a highly toxic and carcinogenic pollutant created during industrial production and waste incineration . Pollutant monitoring has made extensive use of surface-enhanced Raman spectroscopy (SERS) as a quick, non-destructive, sensitive, and affordable analytical method. However, the fabrication of a SERS substrate with ultrahigh sensitivity is a challenging task, the detection cost is expensive. Currently, these are the challenges faced by SERS technique for the detection of dioxin pollutants. In this paper, we present Au nanocakes (Au NCs) as an easy-to-build SERS substrate for sensitive SERS detection of dioxins in real samples. Based on three-dimensional finite-difference time-domain (3D-FDTD) calculations, the enhancement factor of the substrate following aggregation is approximately 10 10 . Using a portable Raman spectrometer, the limit of detection for dioxins such as 1-chloro-dibenzo-p-dioxin (1-CDD), 2,8-dichloro-dibenzo-p-dioxin (2,8-DCDD), and 2,3,7-trichloro-dibenzo-p-dioxin (2,3,7-TrCDD) in clean water reached as low as 5, 5, and 10 ng/mL, respectively. As a real-world application, the same toxic pollutants were detected in sewage water samples. Our findings could lead to the development of novel SERS-based sensors for the rapid detection of dioxins in real-world scenarios. Moreover, a portable Raman spectrometer is used to detect the pollutants, which is easy to use and inexpensive.
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TALANTA
·
2023
·
IF 6.1
Jiaqi Liu,Zhongshun Wang,Ya'nan Meng,Chunning Chen,Qiye Chen,Yalei Wang,Shuzhen Dou,Xiaoyang Liu,Nan Lu
Trace analysis has great promise in the fields of disease diagnosis and environment protection. Surface-enhanced Raman scattering (SERS) has wide range of utilization due to its reliable fingerprint detection. However, the sensitivity of SERS still needs to be enhanced. Raman scattering of target molecules around hotspots, the area with extremely strong electromagnetic field , can be highly amplified. Therefore, to increase the density of hotspots is one of the major approaches for enhancing the detection sensitivity of target molecules. In this paper, an ordered array of Ag nanocubes was assembled on a thiol modified silicon substrate as a SERS substrate, which provided high-density hotspots. The detection sensitivity is demonstrated by the limit of detection, which is down to 10 −6 nM with Rhodamine 6G as probe molecule. The wide linear range (10 −7 –10 −13 M) and low relative standard deviation (<6.48%) indicate the good reproducibility of the substrate. Furthermore, the substrate can be used for the detection of dye molecules in lake water. This method provides an approach for increasing hotspots of SERS substrate, which could be a promising method to achieve good reproducibility and high sensitivity.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Shuang Lin,Xiaoyu Fang,Guoqiang Fang,Fengping Liu,Haoyu Dong,Haiyan Zhao,Jing Zhang,Bin Dong
SERS as a promising sensing technique still faces challenges in the precise identification of trace-amount molecules due to the limitation of sensitivity and cleanliness of SERS substrate. Here, we report a precise and ultrasensitive identification of multiple pollutants via 3D clean cascade-enhanced nanosensor assisted by machine learning algorithms . This SERS substrate could achieve cascading electromagnetic energy with a remarkable enhancement factor as high as 8.35 × 10 9 , which is attributed to the combination of micro-level polystyrene sphere (PS) porous array and nano-level Au-Ag clusters of this substrate. Benefitting from high cleanliness and ultra-sensitivity, multiple hazardous pollutants with similar geometry and Raman peaks at ultra-low concentration were successfully distinguished assisted by principal component analysis (PCA). As a result, this efficient and clean SERS substrate together with artificial intelligence could promote the application of SERS technology in the accurate identification of trace contaminants. Data Availability Data will be made available on request.
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MATERIALS & DESIGN
·
2023
·
IF 8.4
Shuang Xiong,Dalei Wang,Hangkai Qiu,Tao He,Chao Wang,Yueyue Wang,Chaoqing Dai,Wei Liu
The overuse of mixed pesticides poses a threat to both the ecosystem and human health, yet general pesticide detection methods are complex in terms of steps, such as the need for pretreatment and cleaning. Surface-enhanced Raman scattering (SERS) has been used for real-life trace detection of residues due to its rapid detection and ultra-high sensitivity. Here, we prepared a novel Ti 3 C 2 Tx (MXene)-noble metal hybrid flexible substrate with a layer of MXene on top of flower-like Ag nanoparticles (AgNFs), and finally grew Au nanoparticles (AuNPs) by galvanic replacement and self-reduction reactions. The limit of detection (LOD) can be as low as 2 × 10 -12 M by detecting 4-mercaptobenzoic acid (4MBA). For efficient sampling, transparent and flexible platform made of polydimethylsiloxane (PDMS) were used for the extraction and detection of thiabendazole (TBZ), thiram, methyl parathion (MP) and their mixtures. Notably, the lowest concentrations detected by swabbing on the tomato surface (3.7 ng/mL, 2.8 ng/mL) were lower than the EU maximum permissible limits of pesticides on raw fruits and vegetables (4.0 mg/L, 6.33 mg/mL). This high performance Ti 3 C 2 Tx-noble metal hybrid flexible substrate offers a great advantage in the trace detection of molecules.
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