MICROCHIMICA ACTA
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2019
·Vol. 186
·期 11
·1-9
·
IF 5.479
Zhen Deshuai,Jiang Ning,Geng Hongchao,Qiao Yan,Liu Yu,Zhu Xingqi,Gao Chan,Grimes Craig A.,Cai Qingyun
Cobalt-doped nanoporous carbon (Co-NPC) with dodecahedral shape was pyrolytically synthesized and applied as a sorbent and matrix for the enrichment and analysis of small molecules by surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS). Extremely low detection limits were accomplished for cetyltrimethylammonium bromide (1 fg·mL −1 ), and Rhodamine B (1 fg·mL −1 ) in water, and Malachite Green and its metabolite in fish blood and fish extracts (pg·mL −1 concentrations).
Schematic representation of cobalt-doped nanoporous carbons (Co-NPCs) applied as SALDI matrix for analysis of toxic contaminants in fish and receipt papers. The Co-NPCs have a high desorption/ionization efficiency and low limit of detection.
研究领域:
分析化学
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环境科学
·
毒理学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Zufeng Qiu,Hongsheng Zhao,Kuan Chang,Zhiwei Lin,Qin Kuang,Zhaoxiong Xie
Selective Pt deposition on TiO 2 effectively regulates photogenerated charge separation in MALDI-TOF MS nanomaterial matrices. • Photogenerated holes dominate positive ion mode, while electrons dominate negative, governing small-molecule ionization. • Carrier-dominated mechanism is validated in complex TiO 2 , enabling sensitive detection of representative pollutants. Surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS) has emerged as a powerful technique for small-molecule analysis with the introduction of inorganic nanomaterial matrices. However, its analytical performance remains highly dependent on matrix-analyte interactions, and a unified mechanistic understanding is still lacking. Here, we demonstrate that selectively deposited Pt/TiO 2 nanomatrices significantly enhance SALDI-TOF MS performance by regulating photogenerated charge carrier dynamics. Facet- and phase-selective Pt deposition promotes the spatial separation and directional migration of photogenerated electron-hole pairs, leading to pronounced signal enhancement in both positive and negative ion modes. Using amino acids as model analytes, facet-selective Pt/TiO 2 affords up to 3.4-fold enhancement for [A + K] + in the positive ion mode and 3.3-fold for [A-H] − in the negative ion mode, outperforming pristine TiO 2 and nonselectively deposited Pt/TiO 2 counterparts. Photo/electro-chemical analyses, including transient photocurrent, electrochemical impedance spectroscopy, and photoluminescence, correlate enhanced charge carrier separation with improved SALDI-TOF MS performance. Scavenger experiments further reveal that photogenerated holes play a dominant role in adduct formation in the positive ion mode, whereas photogenerated electrons govern analyte deprotonation in the negative ion mode. The proposed mechanism is validated in the structurally complex Pt/commercially available TiO 2 (Pt/P25) system via phase-selective Pt deposition, demonstrating its generality. Furthermore, the optimized Pt/TiO 2 matrix achieves sensitive detection of environmental pollutants, including antibiotics and bisphenol A (BPA), achieving a detection limit of 0.1 ppm. This study establishes a clear charge carrier-dominated mechanism for SALDI-TOF MS nanomatrices, provides rational guidance for the design of high-performance matrices, and highlights their practical potential in environmental pollutant analysis. Download: Download high-res image (107KB) Download: Download full-size image
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2019
·
IF 3.206
Chenyi Li,Hongchao Geng,Xingqi Zhu,Chan Gao,Ning Jiang,Yan Qiao,Qingyun Cai
Concerns about bioaccumulation, persistence and toxicity have led to a lot of researches on perfluorinated compounds (PFCs). In order to identity PFCs in real sample, self-assembled TiO 2 nanosheets (TiO 2 NS) were fabricated by an one-step hydrothermal method and applied as matrix for the surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS) detection of PFCs. Compared to the commercial P25 TiO 2 , the proposed self-assembled TiO 2 nanosheets matrix is better reproducibility and higher sensitivity benefiting from the unique hexagon structure of TiO 2 NS. 22 and 12 PFCs have been detected in water samples collected from locations near the outlets of a factory and a waste-water treatment plant, respectively. The proposed method can be a promising tool for high-throughput detect of trace PFCs in real samples.
研究领域:
分析化学
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环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Yuanxia Lv,Xiaohuan Qin,Kun Hu,Fanggui Ye,Shulin Zhao
This study proposes a surface-assisted laser desorption ionization time-of-flight mass spectrometry (SALDI-TOF MS) method using an ultrastable microporous hydrogen-bonded organic frameworks (MP-HOFs) for selective and sensitive analysis of two common organic pesticides: paraquat (PQ) and chlormequat (CQ) in real samples. MP-HOFs are formed by H-bonding self-assembly of co-planar π-conjugated large aromatic tectons with carboxylate groups. They can not only efficiently absorb and transfer laser energy, but also specifically capture and isolate target analytes from complicated systems. The proposed SALDI-TOF MS method exhibited high salt tolerance and low background. The selective enrichment performance of MP-HOFs was demonstrated by analyzing PQ and CQ in real samples. Simultaneous analysis results of PQ and CQ showed satisfactory reproducibility with relative standard deviations (RSDs) of 3.2–9.2% and 5.7–12.3% for spot-to-spot and sample-to-sample, good linearity (R 2 > 0.99), and high sensitivity with a limit of detection of 0.001 and 0.05 ng mL −1 , respectively. The detection limits of PQ and CQ test analytes were three and two orders of magnitude lower than those of non-enriched PQ and CQ, respectively. Furthermore, the possible ionization mechanism was discussed, and the presented approach was successfully applied for PQ and CQ detection in tap water, river water, and soil, confirming its potential in practical applications.
研究领域:
分析化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2018
·
IF 4.244
Chan Gao,Deshuai Zhen,Ni He,Zhengbin An,Qiulan Zhou,Chenyi Li,Craig A. Grimes,Qingyun Cai
High surface area (136 m 2 g −1 ) nanoporous two-dimensional TiO 2 nanoflakes are applied as an adsorbent and meanwhile a matrix for toxic small molecule analysis using positive-ion surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS). The TiO 2 nanoflakes enable one-step enrichment and analysis, greatly simplifying the analysis technique. Due to the high enrichment efficiency and low background noise, small molecule organic contaminants at ppt or even sub-ppt concentrations such as malachite green (10 pg/mL), leucomalachite green (10 pg/mL), cetyltrimethylammonium bromide (0.001 pg/mL), rhodamine B (0.001 pg/mL), and crystal violet (0.1 pg/mL) were detected. In addition, malachite green and its metabolite leucomalachite green at ng/mL concentrations were successfully detected from fish blood and fish extracts, and crystal violet and its homologues at ng/cm 2 concentrations were detected from inks on thermal receipt papers obtained from local supermarket.
研究领域:
分析化学
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环境科学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Zifang Peng,Wenfen Zhang,Dan Yin,Xu Zhang,Shuo Liu,Wuduo Zhao,Jian Mao,Yanhao Zhang,Jianping Xie
A novel magnetic single-layer nano-MXene (SNM@Fe 3 O 4 ) was prepared for the first time with small size, high surface area, abundant active sites and excellent energy absorption/transfer capability. The combined experimental and theoretical investigation revealed SNM@Fe 3 O 4 could be served as a highly effective adsorbent for enrichment and a new surface-assisted laser desorption/ionization-time of flight-mass spectrometry (SALDI-TOF-MS) matrix for rapid analysis of p -Phenylenediamine (PPD) antioxidants, a kind of emerging environmental contaminants, in actual water samples from North and South China. The SNM@Fe 3 O 4 -based SALDI-TOF-MS approach featured free matrix interference, acceptable linearity (R 2 ≥ 0.97), high sensitivity (LOD at ng mL −1 level) and qualified precision (RSD ≤ 8.46 %) for the four PPDs’ detection. The corresponding determined pollution levels also revealed the widespread occurrence of PPDs in Chinese water system. Compared to previous works, SNM@Fe 3 O 4 -based method achieved reproducible and more rapid analysis of PPDs in water, demonstrating a considerable potential of our self-synthesized nanomaterial for sensitive analysis of low-concentration organic small-molecule compounds in complicated sample matrix.
研究领域:
环境科学
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分析化学
·
纳米技术
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2015
·
IF 6.723
Guiju Xu,Shengju Liu,Jiaxi Peng,Wenping Lv,Ren’an Wu
In this work, a novel core–shell structured gold@graphitized mesoporous silica nanocomposite (Au@GMSN) was synthesized by in situ graphitization of template within the mesochannels of mesoporous silica shell on gold core and demonstrated to be promising nanomaterials for surface-assisted laser desorption/ionization time-of-flight mass spectroscopy (SALDI-TOF MS). The integration of the graphitized mesoporous silica with the gold nanoparticles endowed Au@GMSN with large surface areas of graphitic structure, good dispersibility, and strong ultraviolet (UV) absorption. Au@GMSN exerted the synergistic effect on the efficient detection of small-molecular-weight analytes including amino acids, neutral saccharides, peptides, and traditional Chinese medicine. The Au@GMSN-assisted laser desorption/ionization exhibited the following superiorities: high ionization efficiency, low fragmentation interference, favorable salt tolerance, and good reproducibility. Moreover, because of the large hydrophobic inner surface area of the graphitized mesoporous silica shell, the Au@GMSN demonstrated its promising capacity in the pre-enrichment of aromatic analytes prior to SALDI-TOF MS, which favored rapid and sensitive detection.
研究领域:
纳米技术
·
分析化学
·
质谱学
·
材料科学
✓ 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）