TALANTA
·
2025
·
IF 6.1
Jiaxin Lu,Shuzhen Dou,Chunning Chen,Yalei Wang,Jingtong Zhai,Hongkun Zhao,Nan Lu
Surface-Assisted Laser Desorption/Ionization Mass Spectrometry (SALDI-MS) is a prominent tool for detecting small molecules; however, enhancing its detection sensitivity remains a significant challenge. Two strategies are commonly employed to enhance detection sensitivity: enriching analytes through substrate modification and improving the laser desorption/ionization efficiency of the substrate. In this study, we developed a patterned composite hierarchical structure as a SALDI-MS substrate to improve detection sensitivity. The substrate consists of Si nanopillars and Au nanoparticles, and is patterned with hydrophilic spots and hydrophobic surrounding area. The signal intensity of tetrabutylammonium iodide and sulfacetamide is enhanced by 100-fold and 60-fold, respectively, compared to testing on the Si nanopillars array. The sensitivity enhancement on this substrate is primarily attributed to two factors: first, the analytes are enriched on the hydrophilic spots; and second, the laser desorption/ionization efficiency is improved by the introduction of Schottky barriers through the deposition of Au nanoparticles on Si nanopillars, which extends the lifetime of electron-holes. This design offers high sensitivity, with the lowest detection concentrations for dyes, amino acids and sulfonamides reaching the attomole level. Patterned modifications overcome common issues with super-hydrophobic substrate, such as difficult analyte addition and droplet slippage. The pattern also ensures excellent detection reproducibility, with relative standard deviations (RSD) of 2.4 % across different areas of the same substrate and 6.36 % across different substrates. The substrate is suitable for detecting trace levels of dyes and sulfonamides in river water and seafood extract, demonstrating its potential for analyzing real samples.
研究领域:
分析化学
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质谱技术
·
材料科学
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产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Jingtong Zhai,Yalei Wang,Jiaxin Lu,Chunning Chen,Jiaqi Liu,Hongkun Zhao,Nan Lu
Surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) emerges as an effective method for analyzing small molecules. At the current stage, its application is still limited by its detection sensitivity. According to the mechanism of SALDI-MS, the sensitivity highly depends on the laser desorption/ionization (LDI) efficiency. In this study, we adjust the localized surface plasmon resonance (LSPR) between particles by changing the gap, thereby improving the efficiency of LDI. The gaps of nanoparticles can be adjusted by the ionic strength in the solution. With the decrease of the gaps, the thermal effect of the nanoparticles is gradually enhanced and the number of excited electrons is also increased, which improves the sensitivity of SALDI-MS. The prepared substrate with optimized gaps has wide applicability for the detection of small biomolecules and dye molecules. Moreover, the substrate can successfully detect trace small molecules in complex samples. The analysis of sulfonamide in lake water shows the commendable performance of the substrate. The relative standard deviations (RSD) of spot-to-spot and batch-to-batch are 3.73% and 7.22% respectively, confirming the high reproducibility and the detection limit is as low as 100 pM, indicating the high sensitivity of the substrate. The results demonstrate that adjusting the LSPR of metal nanoparticles is a promising method for improving the performance of SALDI-MS.
研究领域:
分析化学
·
生物医学工程
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产品关联
DOI
高影响因子
MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 6
·1-9
·
IF 6.232
Chen Yang,Huang Ailan,Zhang Lu,Bie Zijun
A highly oriented crystalline metal-organic framework (MOF) nanofilm array was prepared and used for surface-assisted laser desorption ionization mass spectrometry (SALDI-MS) for determination of small molecules. The MOF nanofilm was characterized using scanning/transmission electron microscopy, X-ray diffraction, and ultraviolet-visible spectroscopy. Different small molecules (anthracene, n-eicosanoic acid, Rhodamine B) were successfully determined by this MOF nanofilm array with limits of detection (LOD) between 0.1–5 ng·mL −1 and limits of quantification (LOQ) between 1 and 10 ng·mL −1 . Compared to previously reported MOF-based SALDI-MS, this array exhibits better reproducibility (3.3–5.2%) and recovery (89–105%). The intensity of the MS peak remains the same after 25 repeated cycles. This indicates good repeatability. This MOF nanofilm-based SALDI-MS array can be used for determination of fatty acid and Rhodamine B in real samples with good recovery (83–106%).
Schematic representation of the principle of crystalline MOFs nanofilm-based SALDI-MS array
研究领域:
分析化学
·
材料科学
·
质谱分析
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TALANTA
·
2019
·
IF 4.916
Ning Li,Shuzhen Dou,Lei Feng,Xueyun Wang,Nan Lu
The sensitivity of surface-assisted laser desorption/ionization (SALDI) mass spectrometry (MS) analysis depends on the efficiency of desorption and ionization of analyte molecules, which is usually limited by the low utilization efficiency of laser energy. Herein we demonstrate an efficient method to increase energy utilization efficiency for improving the efficiency of desorption and ionization of analyte molecules in SALDI-MS analysis. To increase the utilization efficiency of energy, a superhydrophobic gold film covered silicon nanocone array is fabricated and used as SALDI substrate. The nanocone array increases the absorption up to 99.65% at the wavelength of 355 nm, which is applied for SALDI-MS detection. The superhydrophobicity promotes the analyte molecules concentrated on the tips of nanocones where photon energy is confined, therefore, more energy can be provided for desorption and ionization of analytes. The energy efficiency is increased by using this substrate. The sensitivity of SALDI-MS analysis is greatly improved. For example, 100 amol/μL of rhodamine 6G , 100 fmol/μL of polyethyleneglycol, 100 ymol/μL of glutathione and 100 ymol/μL arginine still can be analyzed. The lake water containing malachite green was used as the real sample. The regression equation (Log I = 0.39 Log C + 6.58, R 2 = 0.9811) was obtained when the concentration of analyte was in the range from 10 −4 mol/L to 10 −8 mol/L. Therefore, the calculated LOD and LOQ are 1.35 × 10 −14 mol/L and 1.35 × 10 −7 mol/L, respectively. In addition, the lower relative standard deviation (0.7%, n = 10), proper recovery (113% and 91%), and low matrix effect (−1.1% and −1.1%) all demonstrate the great potential of the designed substrate in practical analysis.
研究领域:
分析化学
·
材料科学
·
质谱分析
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Shuzhen Dou,Zhongshun Wang,Qiye Chen,Nan Lu
The high sensitivity of surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) analysis depends on the enhancement of the signal intensity and the reduction of the background. Here, high-density Si nanotips were prepared as SALDI-MS substrate by taking template-free reactive ion etching for sensitive detection . The high-density Si nanotips act as tiny antennas to concentrate the laser energy and generate photo-induced electrons on a small area, which promotes desorption and ionization of molecule, enhancing the signal intensity. Additionally, the high stability of Si nanotips under laser irradiation ensures low background interference. The applicability of the substrate was demonstrated by the detection of various small molecules, e.g., fatty acids, amino acids , environmental pollutants and drugs. In addition, this substrate can be successfully applied for detecting trace small molecules in complex sample, such as 10 −9 M verapamil in serum and 10 −12 M crystal violet in lake water. Moreover, the banned fungicides left on the fish skin was also detected. The substrate is compatible with imaging, and the endogenous and exogenous substances in fingerprint were visualized by MS imaging. These results demonstrate the easily prepared high-density Si nanotips SALDI-MS substrate is of high detection sensitivity and great value toward large-scale practical applications.
研究领域:
分析化学
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生物医学工程
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材料科学
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产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Xuetong Qu,Tao Wang,Xingyue Liu,Xinrong Jiang,Xiao Liang,Jianmin Wu
Serum lipid metabolites have been emerging as ideal biomarkers for disease diagnosis and prediction. In the current stage, nontargeted or targeted lipidomic research mainly relies on a liquid chromatography–mass spectrometry (LC–MS) platform, but future clinical applications need more robust and high-speed platforms. Surface-assisted laser desorption ionization mass spectrometry (SALDI-MS) has shown excellent advantages in the high-speed analysis of lipid metabolites. However, the platform in the positive ion mode is more inclined to target a certain class of lipids, leading to the low coverage of lipid detection and limiting its practical translation to clinical applications. Herein, we proposed a dual-mechanism-driven strategy for high-coverage detection of serum lipids on a novel SALDI-MS target, which is a composite nanostructure comprising vertical silicon nanowires (VSiNWs) decorated with AuNPs and polydopamine (VSiNW-Au-PDA). The performance of laser desorption and ionization on the target can be enhanced by charge-driven desorption coupled with thermal-driven desorption. Simultaneous detection of 236 serum lipids (S/N ≥ 5) including neutral and polar lipids can be achieved in the positive ion mode. Among these, 107 lipid peaks were successfully identified. When combined with VSiNW-Au-PDA and VSiNW chips, 479 lipid peaks can be detected in serum samples in positive and negative ion modes, respectively. Based on the platform, serum samples from 57 hepatocellular carcinoma (HCC) patients and 76 healthy controls were analyzed. After data mining, 14 lipids containing different lipid types (TAG, CE, PC) were selected as potential lipidomic biomarkers. With the assistance of an artificial neural network, a diagnostic model with a sensitivity of 92.7% and a specificity of 96% was constructed for HCC diagnosis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2026
·
IF 4
Mingyi Du,Xiran Chen,Yaming Sun,Jiadu Hu,Wenlin Wen,Hanhong Xu,Zhibin Yin,Xinzhou Wu
MBSA-SiO2@Au nanoshells enabled selective enrichment and SALDI-MS of QACs. • The bifunctional platform served as both adsorbent and ionization matrix. • The method achieved 0.5–1.5 ng/mL LODs with 20–40-fold sensitivity enhancement. • Recoveries of 87.0–108.8% were achieved in white radish, carrot, and potato matrices. The widespread use and persistence of quaternary ammonium compounds (QACs) in food environments raise concerns about their detection at trace levels in complex matrices. In this study, we developed a negatively charged 4-mercaptobenzenesulfonic acid functionalized SiO 2 @Au core-shell nanocomposite (MBSA-SiO 2 @Au) that serves as both a selective adsorbent and an efficient surface-assisted laser desorption/ionization (SALDI) matrix. The sulfonate modified gold shell provides a stable negative surface potential to promote electrostatic interactions with cationic QACs, and their plasmonic properties synergistically enhance laser energy absorption and ionization efficiency. Critical enrichment parameters, including adsorbent amount, solution pH, adsorption time, and redispersion volume, were optimized. The optimized method achieved limits of detection of 0.5 ng/mL for paraquat (PQ), dodecyltrimethylammonium chloride (DTAC), and didodecyldimethylammonium chloride (DDAC), and 1.5 ng/mL for dodecyldimethylbenzylammonium chloride (DBAC), with excellent linearity (R 2 ≥ 0.9843), achieving an enrichment factor of approximately 33.3, and a 20- to 40-fold sensitivity enhancement after enrichment. Application to real food samples, including white radish, carrot, and potato, revealed no detectable QAC residues and satisfactory recoveries ranging from 87.0 to 108.8%. The bifunctional MBSA-SiO 2 @Au-based SALDI platform minimizes organic solvent consumption and offers a rapid, green, and sensitive approach for monitoring QACs in food safety applications.
✓ 已验证
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Jingtong Zhai,Chunning Chen,Jiaxin Lu,Hongkun Zhao,Nan Lu
The sensitive detection of small molecule pollutants in environment and food is crucial for safeguarding public health and maintaining ecological balance. Although surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) has shown great potential in small molecule analysis, its widespread application is hindered by limited laser desorption/ionization (LDI) efficiency and poor signal repeatability. A key challenge lies in developing substrates that can overcome these limitations. In this study, we address this critical issue by preparing an ordered plasmonic bowl structure as an advanced SALDI-MS substrate. The unique bowl structure significantly enhances localized surface plasmon resonance effects—particularly at the edges, bottoms, and inter-bowl gaps—facilitating the efficient generation and migration of hot electrons, which improves LDI efficiency. Additionally, the large contact area of the bowl structures increases the hotspot density, thereby amplifying analyte signal intensity. This substrate enables the sensitive detection of small molecule pollutants (dye molecules, antibiotics, and pesticides) over a broad concentration range from 1 mM to 100 nM. The ordered plasmonic bowl substrate presents a promising platform for the rapid and sensitive detection of small molecule pollutants in environmental and food samples.
研究领域:
分析化学
·
环境科学
·
食品安全
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产品关联
DOI
高影响因子
ANALYST
·
2015
·Vol. 141
·期 9
·2712-2726
·
IF 4.107
Min Hong,Lidan Xu,Fangli Wang,Zhirong Geng,Haibo Li,Huaisheng Wang,Chen-zhong Li
Silver nanoparticles (AgNPs) and reduced graphene oxide (rGO) hybrid nanoporous structures fabricated by the layer-by-layer (LBL) electrostatic self-assembly have been applied as a simple platform for the rapid analysis of carboxyl-containing small molecules by surface-assisted laser desorption/ionization (D/I) mass spectrometry (SALDI-MS). By the simple one-step deposition of analytes onto the (AgNP/rGO)9 multilayer film, the MS measurements of various carboxyl-containing small molecules (including amino acids, fatty acids and organic dicarboxylic acids) can be done. In contrast to other energy transfer materials relative to AgNPs, the signal interferences of a Ag cluster (Agn+ or Agn−) and a C cluster (Cn+ or Cn−) have been effectively reduced or eliminated. The effects of various factors, such as the pore structure and composition of the substrates, on the efficiency of D/I have been investigated by comparing with the (AgNP)9 LBL nanoporous structure, (AgNP/rGO)9/(SiO2NP)6 LBL multilayer film and AgNP/prGO nanocomposites.
研究领域:
分析化学
·
纳米生物技术
·
质谱分析
·
分子诊断
·
材料科学
✓ 已验证
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Xian-Na Wang,Bin Li
Surface-assisted laser desorption/ionization mass spectrometry (SALDI MS) has been successfully applied in the analysis of various small molecules. In this work, gold nanoparticles/thiol-β-cyclodextrin-functionalized TiO2 nanowires (AuNPs/SH-β-CD-TiO2 NWs) were prepared to enhance the performance of SALDI MS and mass spectrometry imaging (MSI). A monolithic TiO2 film was first grown on an indium tin oxide (ITO) glass slide via a modified sol–gel method and treated in an alkaline environment to form nanowires. TiO2 NWs were chemically modified by SH-β-CD for immobilizing AuNPs densely and strongly. Compared with the conventional organic matrix 2,5-dihydroxybenzoic acid (DHB), the prepared AuNPs/SH-β-CD-TiO2 NWs showed superior performances on detection sensitivity, repeatability, and analyte coverage. Analytes typically detectable with negative-ion matrix-assisted laser desorption/ionization (MALDI) MS could also be observed using AuNPs/SH-β-CD-TiO2 NWs in the positive ion mode. Its successful usage efficiently enhanced the SALDI MS detection of various small molecules such as carbohydrates, fatty acids, and bile acids in the positive ion mode. The developed SALDI substrate was further used to characterize and discriminate the natural and in vitro cultured Calculus Bovis, as well as natural and artificial Moschus. Furthermore, the spatial distribution of several natural products in spearmint leaves and potato tubers was explored by tissue imprinting and deposition on the AuNPs/SH-β-CD-TiO2 NW surface for SALDI MSI in dual-polarity mode, respectively. The wide application and satisfied detection sensitivity make AuNPs/SH-β-CD-TiO2 NWs ideal for SALDI MS and MSI of various natural products.
研究领域:
分析化学
·
质谱技术
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Jingxuan Pei,Yibo Sun,Xiang Yu,Zhenfei Tian,Shuting Zhang,Songbo Wei,Yanfang Zhao,Rabah Boukherroub
Development of reliable sensing strategy combining surface-enhanced Raman scattering (SERS) and surface-assisted laser desorption/ionization-mass spectrometry (SALDI-MS) is of significant interest to distinguish cysteine enantiomers in body fluid for understanding their physiological roles and toxicity hazards. In this work, a SERS/SALDI-MS dual-mode sensing platform of gold nanoparticles (Au NPs) decorated holey carbon nitride (hg-C 3 N 4 ) was fabricated for sensitive detecting cysteine. The designed Au@hg-C 3 N 4 matrix featured a uniform distribution of Au NPs with the help of anchoring effect of hg-C 3 N 4 holey structure, which was conducive to produce highly repeatable signals. Moreover, the combination of Au NPs and holey g-C 3 N 4 endowed this matrix with superior enrichment capacity, enhanced charge transfer and strong UV absorption. These merits allowed the matrix to acquire high sensitivity and enhanced reproducibility for l -cysteine by means of SERS/SALDI-MS. Likewise, reliable detection of l -cysteine and efficient recognition of d -cysteine in human serum jointly revealed its prospect for detecting cysteine enantiomers in body fluids. This work offers a reliable SERS/SALDI-MS strategy for determining L/D-cysteine enantiomers, and the designed Au@hg-C 3 N 4 matrix becomes a potential application candidate for selective detection of bio-enantiomers.
研究领域:
分析化学
·
生物传感器
·
材料科学
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TALANTA
·
2023
·
IF 6.1
Qiong Wu,Jing Yu,Mingjin Zhang,Yinran Xiong,Lijia Zhu,Bo Wei,Ting Wu,Yiping Du
The liver is a major organ in metabolism, and alterations in serum lipids are associated with liver disorders. Here, a rapid, easy, and reliable screening technique based on lipidomic profiling was developed using machine learning and surface-assisted laser desorption ionization mass spectrometry (SALDI MS) for liver cancer diagnosis. A graphitized carbon matrix (GCM) was created for serum lipid profiling in SALDI MS and demonstrated a better performance for neutral lipids analysis than conventional organic matrices. The fingerprint of serum lipids, including triacylglycerols (TGs), diacylglycerols (DGs), cholesteryl esters (CEs), glycerophospholipids (GPs), and other components, could be directly obtained by GCM-assisted LDI MS without extraction. Five machine learning methods were applied to distinguish liver cancer (LC) patients from healthy controls (HC) and chronic hepatitis B (CHB) patients. The best diagnostic performance was attained by linear discriminant analysis (LDA), which has a confusion matrix accuracy of 98.3 %. The receiver operating characteristic (ROC) curve for liver cancer exhibited an area under the curve (AUC) of 0.99, indicating a high degree of prediction accuracy. One-way ANOVA analysis revealed that numerous TGs were down-regulated in LC group. The results demonstrated the viability of GCM-assisted LDI MS as a valuable diagnostic tool for liver cancer.
研究领域:
医学诊断
·
质谱技术
·
机器学习
·
癌症研究
·
脂质组学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）