Red-emissive carbon dot as fluorescent probe for the sensitive detection of sunset yellow in foodstuffs.

The highly efficient red-emissive carbon dots (R-CDs) were synthesized from citric acid, polyethyleneimine, and benzil via a facile solvothermal process. The R-CDs displayed maximum fluorescence properties at excitation and emission wavelengths of 550 and 631 nm, respectively, which fall within the red wavelength range. Moreover, the R-CDs exhibited a high fluorescence quantum yield of 11.3 %, and this fluorescence was effectively quenched by Sunset Yellow (SY). Consequently, a novel fluorescent probe was developed for SY detection. This probe exhibited a linear range of 0.085-11.31 µg/mL and limit of detection of 0.026 µg/mL. The R-CDs were validated for SY quantification in various food samples, including carbonate beverages, powdered beverage, cider vinegar, fruit flavored drinks, chocolate, and hard candy samples, achieving recovery rates of 91.2-122 % and a relative standard deviation of 1.0-3.5 %. The synthesized R-CDs therefore show promise for application as a probe for the detection of SY in foods.

Enhanced Cataluminescence Sensor Based on SiO2/MIL-53(Al) for Detecting Isobutylaldehyde.

A simple, rapid, and reliable method for detecting harmful gases is urgently required in environmental security fields. In this study, a highly effective cataluminescence sensor based on SiO2/MIL-53(Al) composites was developed to detect trace isobutylaldehyde. The sensor was designed using isobutylaldehyde to generate an interesting cataluminescence phenomenon in SiO2/MIL-53(Al). Under optimized conditions, a positive linear relationship was observed between the signal intensity of the cataluminescence and isobutylaldehyde concentration. The isobutylaldehyde concentration range of 1.55-310 ppm responded well to the sensing test, with an excellent correlation coefficient of 0.9996. The minimum detectable concentration signal-to-noise ratio (S/N = 3) was found to be 0.49 ppm. In addition, the sensor was effectively utilized for analyzing trace isobutylaldehyde; the analysis resulted in recoveries ranging from 83.4% to 105%, with relative standard deviations (RSDs) of 4.8% to 9.4%. Furthermore, the mechanism of cataluminescence between SiO2/MIL-53(Al) and isobutylaldehyde was explored using GC-MS analysis and density functional theory. We expect that this cataluminescence methodology will provide an approach for the environmental monitoring of isobutylaldehyde.

Preparation of One-Emission Nitrogen-Fluorine-Doped Carbon Quantum Dots and Their Applications in Environmental Water Samples and Living Cells for ClO- Detection and Imaging.

Hypochlorite (ClO-) has received extensive attention owing to its significant roles in the immune defense and pathogenesis of numerous diseases. However, excessive or misplaced production of ClO- may pose certain diseases. Thus, to determine its biological functions in depth, ClO- should be tested in biosystems. In this study, a facile, one-pot synthesis of nitrogen-fluorine-doped carbon quantum dots (N, F-CDs) was developed using ammonium citrate tribasic, L-alanine, and ammonium fluoride as raw materials under hydrothermal conditions. The prepared N, F-CDs demonstrate not only strong blue fluorescence emission with a high fluorescence quantum yield (26.3%) but also a small particle size of approximately 2.9 nm, as well as excellent water solubility and biocompatibility. Meanwhile, the as-prepared N, F-CDs exhibit good performance in the highly selective and sensitive detection of ClO-. Thus, a wide concentration response range of 0-600 µM with a low limit of detection (0.75 µM) was favorably obtained for the N, F-CDs. Based on the excellent fluorescence stability, excellent water solubility, and low cell toxicity, the practicality and viability of the fluorescent composites were also successfully verified via detecting ClO- in water samples and living RAW 264.7 cells. The proposed probe is expected to provide a new approach for detecting ClO- in other organelles.

Solid-State Nanopore/Nanochannel Sensing of Single Entities.

Solid-state nanopores/nanochannels, with their high stability, tunable geometry, and controllable surface chemistry, have recently become an important tool for constructing biosensors. Compared with traditional biosensors, biosensors constructed with solid-state nanopores/nanochannels exhibit significant advantages of high sensitivity, high specificity, and high spatiotemporal resolution in the detection single entities (such as single molecules, single particles, and single cells) due to their unique nanoconfined space-induced target enrichment effect. Generally, the solid-state nanopore/nanochannel modification method is the inner wall modification, and the detection principles are the resistive pulse method and the steady-state ion current method. During the detection process, solid-state nanopore/nanochannel is easily blocked by single entities, and interfering substances easily enter the solid-state nanopore/nanochannel to generate interference signals, resulting in inaccurate measurement results. In addition, the problem of low flux in the detection process of solid-state nanopore/nanochannel, these defects limit the application of solid-state nanopore/nanochannel. In this review, we introduce the preparation and functionalization of solid-state nanopore/nanochannel, the research progress in the field of single entities sensing, and the novel sensing strategies on solving the above problems in solid-state nanopore/nanochannel single-entity sensing. At the same time, the challenges and prospects of solid-state nanopore/nanochannel for single-entity electrochemical sensing are also discussed.

Silver Nanoparticle-Functionalised Nitrogen-Doped Carbon Quantum Dots for the Highly Efficient Determination of Uric Acid.

The fabrication of efficient fluorescent probes that possess an excellent sensitivity and selectivity for uric acid is highly desirable and challenging. In this study, composites of silver nanoparticles (AgNPs) wrapped with nitrogen-doped carbon quantum dots (N-CQDs) were synthesised utilising N-CQDs as the reducing and stabilising agents in a single reaction with AgNO3. The morphology and structure, absorption properties, functional groups, and fluorescence properties were characterised by transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, ultraviolet spectroscopy, fluorescence spectroscopy, and X-ray diffraction spectroscopy. In addition, we developed a novel method based on AgNPs/N-CQDs for the detection of uric acid using the enzymatic reaction of uric acid oxidase. The fluorescence enhancement of the AgNPs/N-CQDs composite was linear (R2 = 0.9971) in the range of 2.0-60 µmol/L, and gave a detection limit of 0.53 µmol/L. Trace uric acid was successfully determined in real serum samples from the serum of 10 healthy candidates and 10 gout patients, and the results were consistent with those recorded by Qianxinan Prefecture People's Hospital. These results indicate that the developed AgNP/N-CQD system can provide a universal platform for detecting the multispecies ratio fluorescence of H2O2 generation in other biological systems.

Development of a highly efficient in-tube solid-phase microextraction system coupled with UHPLC-MS/MS for analyzing trace hydroxyl polycyclic aromatic hydrocarbons in biological samples.

Hydroxyl polycyclic aromatic hydrocarbons are considered active mutagenic and carcinogenic substances and are found in extremely low levels (ng/g) in biological samples. As a result, their determination in urine and blood samples is challenging, and a sensitive and effective method for the analysis of trace hydroxyl polycyclic aromatic hydrocarbons in complex biological matrices is required. In this work, a novel macroporous in-tube solid-phase microextraction monolith was prepared via a thiol-yne click reaction, and a highly efficient analytical method based on in-tube solid-phase microextraction coupled with UHPLC-MS/MS was developed to determine hydroxyl polycyclic aromatic hydrocarbons with low detection limits of 0.137-11.0 ng/L in complex biological samples. Four hydroxyl polycyclic aromatic hydrocarbons, namely, 2-hydroxyanthraquinone, 1-hydroxypyrene, 1,8-dihydroxyanthraquinone, and 6-hydroxychrysene, were determined in the urine samples of smokers, non-smokers, and whole blood samples of mice. Satisfactory recoveries were achieved in the range of 83.1-113% with relative standard deviations of 3.2-9.7%. It was found that implementation of the macroporous monolith gave a highly efficient approach for enriching trace hydroxyl polycyclic aromatic hydrocarbons in biological samples.

Determination of six parabens in biological samples by magnetic solid-phase extraction with magnetic mesoporous carbon adsorbent and UHPLC-MS/MS.

Although parabens are useful due to their antiseptic properties, their widespread use has caused concerns regarding their potential toxicological effects. In this study, a novel magnetic solid-phase extraction combined with ultra-high-performance liquid chromatography-tandem mass spectrometry (MSPE-UHPLC-MS/MS) was developed, based on ordered magnetic mesoporous carbon (MMC), for paraben analysis. The MMC was prepared by soft-template synthesis, with a unique pore structure and a highly specific surface response, indicating potential as an excellent adsorbent. Several parameters affecting the paraben extraction efficiency were investigated and a novel method for paraben analysis in serum and urine samples using MSPE-UHPLCMS/MS was developed. The concentrations of methylparaben, ethylparaben, isopropylparaben, and propylparaben in these samples were 0.0380-4.36, 0.460-9.65, 0.0118-0.770, and 0.0363-0.641 µg/L, respectively, whereas isobutylparaben and butylparaben were not detected. Furthermore, satisfactory recoveries of 76.4-121% with relative standard deviations (n = 5) of 1.9-8.6% were obtained. Therefore, the developed MSPE-UHPLC-MS/MS method was efficient, highly sensitive, and reliable for analysing parabens in complex biological samples.

A substantial increase of analytical throughput in capillary electrophoresis throughput by separation-interrupted sequential injections.

How to further improve the throughput of capillary electrophoresis (CE) is a fascinating question. Herein an idea to substantially increase the throughput of CE has been proposed together with theory and experimental demonstration. The key is to introduce samples for CE, one after another, by a short suspension of voltage application, which was hence termed separation-interrupted sequential injections (Sisi). The idea was demonstrated to be feasible on a laboratory-built CE instrument coupled with tandem C4D (contactless capacitively-coupled conductivity) detectors. At least 50 injections of a testing sample (mixture of NH4+, K+, Ca2+, Na+ and Mg2+) were successfully separated in only a single run. The separation took 145 min in total, equivalent to 2.9 min per analysis which is only 21% of that of normal CE. Quantification of the separated ions was performed, with a limit of detection of 1.1-2.6 µM, a limit of quantification of 3.2-8.9 µM, and a linear range up to 1000 µM (R2 > 0.99). The recovery was between 88% and 112% measured by spiking standards into samples at low, middle and high levels. The real applicability of Sisi-CE was evaluated by direct injection and analysis of 45 mineral water samples also in a single run. Its clinical application potential was demonstrated by high throughput assay of the calcium and zinc gluconate oral solution formula, and the blood potassium of hyperkalemia and hypokalemia from patients with renal failure disease. This method can be extended to other applications such as omics studies through the use of more suitable detectors. The theory proposed may also be applicable to other high throughput methods.

A stable version of capillary electrophoresis for determining human hemoglobin chains aiming at the screening and diagnosis of thalassemia.

As a fast, high-performance and cost-effective separation technique, capillary electrophoresis (CE) is applicable to the screening and diagnosis of diseases such as thalassemia. However, it is often not preferred due to its unrepeatable and/or irreproducible migration times. Herein, we propose a stable version of CE that uses migration charge density instead of the migration time to plot the electropherogram. The peak position is now independent of the applied voltage or current and the capillary geometry and is also insensitive to temperature. Its applicability was demonstrated in the quantitative analysis of human hemoglobin. On a laboratory-built device, with a running buffer simply consisting of 3.0 M acetic acid and 0.1% (w/v) hydroxyethyl cellulose, it allows a direct injection of whole blood samples and all the concerned globin chains, α, ß, Aγ and Gγ can be well separated in 15 minutes. The resolution of α/ß, ß/Aγ, and Aγ/Gγ reached 4.4, 3.1 and 5.3, respectively. The intra- and inter-day precisions for the peak position based on the migration charge densities were below 0.6%. Its diagnostic applicability was validated in the analysis of several real blood samples from newborns, children and adults, and its capacity was demonstrated to screen and define the type of thalassemia.

Synthesis of Novel Fluorescent Carbon Quantum Dots From Rosa roxburghii for Rapid and Highly Selective Detection of o-nitrophenol and Cellular Imaging.

A novel carbon quantum dots (CQDs) were successfully synthesized by one-step hydrothermal reaction using Rosa roxburghii as a biomass-based precursor. The CQDs have an average size of 2.5 nm and a narrow size distribution. They display strong blue fluorescence with a quantum yield of 24.8% and good biocompatibility. Notably, these CQDs were capable of detecting trace o-nitrophenol in surface water and sewage with high sensitivity and specificity. The linear range is 0.08-40 µmol/L, and the limit of detection is 15.2 nmol/L. Furthermore, this CQDs was successfully applied for o-nitrophenol analysis in river water and sewage samples. Additionally, Hep3B cells, a human hepatocellular carcinoma cell line, can be easily imaged with high resolution using the as-prepared CQDs as nanoprobes. These results reveal that the as-prepared CQDs have potential applications for detecting o-nitrophenol and cell imaging.

A Highly Sensitive and Selective Isobutyraldehyde Sensor Based on Nanosized Sm2O3 Particles.

A highly sensitive and selective sensor for isobutyraldehyde (IBD) is demonstrated based on intensive cataluminescence (CTL) emission from the surface of nanosized Sm2O3 particles. The characteristics and optimum conditions for the CTL sensor, including the working temperature, wavelength, and flow rate, were investigated in detail. Under the optimized experimental conditions, the CTL intensity varied linearly with the concentration of IBD, in the two-order-of-magnitude range of 0.015-3.9 µg/mL, with a correlation coefficient (r) of 0.99991 and a limit of detection (LOD), at a signal-to-noise ratio (S/N = 3) of 4.6 ng/mL. The sensor was quite specific: butyraldehyde, methanol, ethanol, acetone, formaldehyde, acetaldehyde, benzene, ethylbenzene, and cumene could not produce significant CTL intensities; specifically, butyraldehyde, ethanol, acetone, and acetaldehyde produced low CTL intensities, with values that were 3.8%, 2.8%, 0.60%, and 0.57% that of IBD. As a test of sensor stability, we found that the relative standard deviation (RSD) of 30 measurements of the CTL at an IBD concentration of 1.6 µg/mL within a period of 72 h was 2.2%, indicating good stability and long service life of the sensor. The sensor was tested against spiked samples containing IBD, and recoveries between 89.7% and 97.4% were obtained with an RSD of 6.1%-8.6%. The performance of the sensor indicated its utility for practical sample analysis.

Covalently bonded aptamer-functionalised magnetic mesoporous carbon for high-efficiency chloramphenicol detection.

A novel aptamer-modified magnetic mesoporous carbon was prepared to develop a specific and sensitive magnetic solid-phase extraction method through combination with ultra-high performance liquid chromatography-tandem mass spectrometry for the analysis chloramphenicol in complex samples. More specifically, the chloramphenicol aptamer-modified Mg/Al layered double hydroxide magnetic mesoporous carbon was employed as a novel magnetic solid-phase extraction sorbent for analyte enrichment and sample clean-up. The extraction solvent, extraction time, desorption solvent, and desorption time were investigated. It was found that the mesoporous structure and aptamer-based affinity interactions resulted in acceptable selective recognition and a good chemical stability toward trace amounts of chloramphenicol. Upon combination with the ultra-high performance liquid chromatography-tandem mass spectrometry technique, a specific and sensitive recognition method was developed with a low limit of detection (0.94 pmol/L, S/N = 3) for chloramphenicol analysis. The developed method was successfully employed for the determination of chloramphenicol in complex serum, milk powders, fish and chicken samples, giving recoveries of 87.0-107% with relative standard deviations of 3.1-9.7%.

NH2-MIL-53(Al) Polymer Monolithic Column for In-Tube Solid-Phase Microextraction Combined with UHPLC-MS/MS for Detection of Trace Sulfonamides in Food Samples.

In this study, a novel monolithic capillary column based on a NH2-MIL-53(Al) metal-organic framework (MOF) incorporated in poly (3-acrylamidophenylboronic acid/methacrylic acid-co-ethylene glycol dimethacrylate) (poly (AAPBA/MAA-co-EGDMA)) was prepared using an in situ polymerization method. The characteristics of the MOF-polymer monolithic column were investigated by scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, X-ray diffractometry, Brunauer-Emmett-Teller analysis, and thermogravimetric analysis. The prepared MOF-polymer monolithic column showed good permeability, high extraction efficiency, chemical stability, and good reproducibility. The MOF-polymer monolithic column was used for in-tube solid-phase microextraction (SPME) to efficiently adsorb trace sulfonamides from food samples. A novel method combining MOF-polymer-monolithic-column-based SPME with ultra-high performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS) was successfully developed. The linear range was from 0.015 to 25.0 µg/L, with low limits of detection of 1.3-4.7 ng/L and relative standard deviations (RSDs) of < 6.1%. Eight trace sulfonamides in fish and chicken samples were determined, with recoveries of the eight analytes ranging from 85.7% to 113% and acceptable RSDs of < 7.3%. These results demonstrate that the novel MOF-polymer-monolithic-column-based SPME coupled with UHPLC-MS/MS is a highly sensitive, practical, and convenient method for monitoring trace sulfonamides in food samples previously extracted with an adequate solvent.

The Application of Green-Synthesis-Derived Carbon Quantum Dots to Bioimaging and the Analysis of Mercury(II).

Ginkgo leaves were used as precursors for the hydrothermal synthesis of carbon quantum dots (CQDs), which were subsequently characterized by transmission electron microscopy as well as Fourier-transform infrared, X-ray powder diffraction, and X-ray photoelectron spectroscopy. The prepared CQDs exhibited a fluorescence quantum yield of 11% and superior water solubility and fluorescence stability, as well as low cytotoxicities and excellent biocompatibilities with A549 and HeLa cells; these CQDs were also used to bioimage HeLa cells. Moreover, owing to the experimental observation that Hg2+ quenches the fluorescence of the CQDs in a specific and sensitive manner, we developed a method for the detection of Hg2+ using this fluorescence sensor. The sensor exhibited a linear range for Hg2+ of 0.50-20 µM, with an excellent coefficient of determination (R 2 = 0.9966) and limit of detection (12.4 nM). In practice, the proposed method was shown to be highly selective and sensitive for the monitoring of Hg2+ in lake water and serum samples.

Synthesis of Nano-Praseodymium Oxide for Cataluminescence Sensing of Acetophenone in Exhaled Breath.

In this work, we successfully developed a novel and sensitive gas sensor for the determination of trace acetophenone based on its cataluminescence (CTL) emission on the surface of nano-praseodymium oxide (nano-Pr6O11). The effects of working conditions such as temperature, flow rate, and detecting wavelength on the CTL sensing were investigated in detail. Under the optimized conditions, the sensor exhibited linear response to the acetophenone in the range of 15-280 mg/m3 (2.8-52 ppm), with a correlation coefficient (R2) of 0.9968 and a limit of detection (S/N = 3) of 4 mg/m3 (0.7 ppm). The selectivity of the sensor was also investigated, no or weak response to other compounds, such as alcohols (methanol, ethanol, n-propanol, iso-propanol, n-butanol), aldehyde (formaldehyde and acetaldehyde), benzenes (toluene, o-xylene, m-xylene, p-xylene), n-pentane, ethyl acetate, ammonia, carbon monoxide, carbon dioxide. Finally, the present sensor was applied to the determination of acetophenone in human exhaled breath samples. The results showed that the sensor has promising application in clinical breath analysis.

Aptamer-modified magnetic metal-organic framework MIL-101 for highly efficient and selective enrichment of ochratoxin A.

A facile and efficient strategy is developed to modify aptamers on the surface of the magnetic metal-organic framework MIL-101 for the rapid magnetic solid-phase extraction of ochratoxin A. To the best of our knowledge, this is the first attempt to create a robust aptamer-modified magnetic MIL-101 with covalent bonding for the magnetic separation and enrichment of ochratoxin A. The saturated adsorption of ochratoxin A by aptamer-modified magnetic MIL-101 was 7.9 times greater than that by magnetic metal-organic framework MIL-101 due to the former's high selective recognition as well as good stability. It could be used for extraction more than 12 times with no significant changes in the extraction efficiency. An aptamer-modified magnetic MIL-101-based method of magnetic solid-phase extraction combined with ultra high performance liquid chromatography with tandem mass spectrometry was developed for the determination of trace ochratoxin A with limit of detection of 0.067 ng/L. Ochratoxin A of 4.53-13.7 ng/kg was determined in corn and peanut samples. The recoveries were in the range 82.8-108% with a relative standard deviation (n = 5) of 4.5-6.5%. These results show that aptamer-modified magnetic MIL-101 exhibits selective and effective enrichment performance and have excellent potential for the analysis of ultra-trace targets from complex matrices.

A Facile Synthesis of Highly Nitrogen-Doped Carbon Dots for Imaging and Detection in Biological Samples.

A facile, green, and high-output hydrothermal synthesis was proposed for the fabrication of highly fluorescent nitrogen-doped carbon quantum dots (N-doped CDs). The nitrogen content in N-doped CDs reached 19.2% and demonstrated strong blue fluorescence emission was obtained with fluorescence quantum yield (QY) of up to 32.9%, which exhibit high fluorescence quantum yield, high photostability, and excellent biocompatibility. The N-doped CDs possess high photostability, low toxicity, and excellent biocompatibility, based on which the N-doped CDs were successfully applied as a fluorescence probe for cell imaging. Moreover, it was then successfully demonstrated for sensitive and selective detection of Fe3+ in serum.

In Situ Synthesis of a Magnetic Graphene Platform for the Extraction of Benzimidazoles from Food Samples and Analysis by High-Performance Liquid Chromatography.

A novel method was proposed for the determination of five benzimidazoles (oxfendazole, mebendazole, flubendazole, albendazole, and fenbendazole) using magnetic graphene (G-Fe3O4). G-Fe3O4 was synthesized via in situ chemical coprecipitation. The properties of G-Fe3O4 were characterized by various instrumental methods. G-Fe3O4 exhibited a great adsorption ability and good stability towards analytes. Various experimental parameters that might affect the extraction efficiency such as the amount of G-Fe3O4, extraction solvent, extraction time, and desorption conditions were evaluated. Under the optimized conditions, a method based on G-Fe3O4 magnetic solid-phase extraction coupled with high-performance liquid chromatography was developed. A good linear response was observed in the concentration range of 0.100-100 µg/L for the five benzimidazoles, with correlation coefficients ranging from 0.9966 to 0.9998. The limits of detection (S/N = 3) of the method were between 17.2 and 32.3 ng/L. Trace benzimidazoles in chicken, chicken blood, and chicken liver samples were determined and the concentrations of oxfendazole, mebendazole, flubendazole, and fenbendazole in these samples were 13.0-20.2, 1.62-4.64, 1.94-6.42, and 0.292-1.04 ng/g, respectively. The recovery ranged from 83.0% to 115%, and the relative standard deviations were less than 7.9%. The proposed method was sensitive, reliable, and convenient for the analysis of trace benzimidazoles in food samples.

Efficient and Selective Enrichment of Ultratrace Cytokinins in Plant Samples by Magnetic Perhydroxy-Cucurbit[8]uril Microspheres.

Cytokinins play a critical role in controlling plant growth and development, but it is difficult to be determined in plant samples due to the extremely low concentration level of picomole/gram. So it is important for efficient sample preparation with selective enrichment and rapid separation for accurate analysis of cytokinins. Herein, a supramolecular perhydroxy-cucurbit[8]uril (PCB[8]) was fabricated into the Fe3O4 magnetic particles via chemical bonding assembly and magnetic perhydroxy-cucurbit[8]uril (MPC) materials were obtained. The MPC had good enrichment capability to cytokinins and the enrichment factors were more than 208. The interaction of MPC and cytokinins was investigated by adsorption test and density functional theory (DFT) calculation, the results showed that the main drive forces were the host-guest interaction and hydrogen-bonding interaction between the perhydroxy-cucurbit[8]uril with analytes. Combined with ultra performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS), the MPC was used as a sorbent of magnetic solid-phase extraction for the analysis of cytokinins in plant samples. A sensitive and selective UPLC-MS/MS method was developed with low detection limits of 0.14-0.32 ng/L for cytokinins analysis. Five cytokinins including zeatin riboside, meta-topolin, kinetin, kinetin riboside, and zip with 6.12-87.3 ng/kg were determined in the soybean sprout and Arabidopsis thaliana. The recoveries were in the range of 76.2-110% with relative standard deviations (n = 5) of 2.3-9.7%. On the basis of these results, magnetic perhydroxy-cucurbit[8]uril materials with selective enrichment capability have good potential on the analysis of ultratrace targets from complicated sample matrixes.

Acrylamide-modified graphene for online micro-solid-phase extraction coupled to high-performance liquid chromatography for sensitive analysis of heterocyclic amines in food samples.

Heterocyclic amines (HAs) are considered as potential mutagens and carcinogens, and are found in trace quantities (ng/g level) in food samples. Therefore, it is important to develop a selective and effective method to determine trace HAs in complex matrices. In this study, acrylamide-modified graphene (AMG) was successfully synthesised and showed good stability and permeability in aqueous and organic phases. AMG was used as an efficient adsorbent in the online micro-solid-phase extraction (µ-SPE) of trace HAs. The enrichment factors of the AMG µ-SPE column were determined as 78-166 for six HAs. An online method based on AMG µ-SPE coupled to high-performance liquid chromatography was developed. The limits of detection ranged from 0.70 to 2.5 ng/L. Trace HAs in spicy salted duck, baked fish, and fried chicken samples were determined and the concentrations of 2-amino-3-methylimidazo[4,5-f]quinoine, 2-amino-3,4-dimethylimidazo[4,5-f]quinoine, and 2-amino-3,8-dimethylimidazo[4,5-f]quinoxaline in these samples were 4.7-37.3, 8.1-15.4, and 43.3-109 ng/g, respectively. The recoveries for the six HAs ranged from 65.9% to 118%, and the relative standard deviation (RSDs) were less than 10.8%. The proposed online method was sensitive, reliable, and convenient for the analysis of trace HAs in food samples.