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In this study, a hydrothermal process was utilized to grow mixed-valence CuFe 2 O 4 /Cu 0 nanosheets on carbon fiber paper, forming a three-dimensional hierarchical electrode (CuFe 2 O 4 /Cu 0 @CFP). The ordered array structure, coupled with the porous bowl-like structure, enhances the exposure of more electrode active sites and facilitates analyte penetration, thus enhancing the electrode sensing performance. As a binder-free sensor, the CuFe 2 O 4 /Cu 0 @CFP sensor exhibited remarkable sensitivity in detecting Malachite Green (MG), Sunset Yellow (SY) and Tartrazine (TA) over wide concentration ranges: 0.1-300 μM for MG (R 2  = 0.994), 0.005-200 μM for SY (R 2  = 0.996), and 0.005-300 μM for TA (R 2  = 0.995) with low detection limits of 0.033 μM for MG, 0.0016 μM for SY, and 0.0016 μM for TA (S/N = 3), respectively. Additionally, the 3D CuFe 2 O 4 /Cu 0 @CFP sensor detected MG, SY, and TA in a mixed solution with satisfactory results. It also performs well in beverage, fruit juice powder, and jelly samples, with results matching those from HPLC., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Rhodamine, a colorant prohibited in various consumer products due to its demonstrated carcinogenic, mutagenic, and toxic properties, necessitates the development of a straightforward, efficient, sensitive, environmentally friendly, and cost-effective analytical method. This review provides an overview of recent advancements in the pretreatment and determination techniques for rhodamine across diverse sample matrices since 2017. Sample preparation methods encompass both commonly used pretreatment techniques such as filtration, centrifugation, solvent extraction, and cloud point extraction, as well as innovative approaches including solid phase extraction, dispersive liquid-liquid microextraction, hollow fiber liquid phase microextraction, magnetic solid phase extraction, and matrix solid phase dispersion. The analytical techniques encompass high performance liquid chromatography, surface-enhanced Raman scattering, and sensor-based methods. Furthermore, a comprehensive examination is conducted to offer insights for future research on rhodamine regarding the advantages, disadvantages, and advancements in various pretreatment and determination methodologies., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Colorants, especially synthetic colorants, play a crucial role in enhancing the aesthetic qualities of food owing to their cost-effectiveness and stability against environmental factors. Ensuring the safe and regulated use of colorants is essential for maintaining consumer trust in food safety. Various preparation and analytical technologies, which are continuously undergoing improvement, are currently used to quantify of synthetic colorants in food products. This paper reviews recent developments in analytical techniques for synthetic food colorants, detection and compares the operational principles, advantages, and disadvantages of each technology. Additionally, it also explores advancements in these technologies, discussing several invaluable tools of analysis, such as high-performance liquid chromatography, liquid chromatography-tandem mass spectrometry, electrochemical sensors, digital image analysis, near-infrared spectroscopy, and surface-enhanced Raman spectroscopy. This comprehensive overview aims to provide valuable insights into current progress and research in the field of food colorant analysis., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

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., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

Natural pigments are an indicator component in the freshness indicator, which is advantageous due to their safety, renewability, and low cost. However, freshness indicator with natural pigments as pH indicators has the problems of low stability and the color rendering domain could not effectively cover the shelf life of food. This paper describes the types and structures of natural pigments commonly used in freshness indicators and their color change mechanisms under different pH conditions. Also, the preparation methods of natural pigments freshness indicators are reviewed. Based on the current limitations and shortcomings faced by natural pigments freshness indicators, this paper highlights optimization strategies to enhance their sensitivity and stability, including modification, co-pigmentation, natural pigments mixing, encapsulation, and metal-ion complexation. The exploitation of these optimization strategies can help develop natural pigment-based intelligent packaging with superior performance to meet the food industry's needs for quality and safety monitoring., Competing Interests: Declaration of competing interest No potential conflict of interest was reported by the authors., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

A new convenient method for identifying colorant compounds (CCs) in food matrices was developed using high-performance liquid chromatography with a diode array detector and quadrupole-time-of-flight mass spectrometer (HPLC-DAD-Q/TOF-MS) combined with theoretical calculations. A model sample containing three typical CCs was completely separated via HPLC-DAD. The obtained 3D ultraviolet-visible (UV-vis) spectra revealed the maximum absorption wavelengths (MAWs) of all CCs (yellow, 430 nm; red, 520 nm; blue, 620 nm) in the range of 400-800 nm, and their colors were determined based on their MAWs. Temporary structures of the CCs were obtained using Q/TOF-MS analysis. Theoretical calculations were then performed to obtain the theoretical MAWs and colors of the CCs according to their calculated UV-vis spectra based on temporary structures. The structures of the CCs were confirmed without the need for authoritative standards by comparing the consistency between their experimental and theoretical MAWs and colors. This method is particularly suitable for identifying CCs or compounds with UV-Vis absorption, including new compounds, compounds for which standards are difficult to obtain, and known compounds without reporting relevant molecular information., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier Ltd.)

Ion pair-based surfactant-assisted liquid-liquid microextraction with solidification of floating organic drops has been developed to extract Allura red (AR), tartrazine (TAR), and fast green (FG) prior to spectrophotometric determination. Cetyltrimethylammonium bromide (CTAB) was employed as ion-pairing agent to enhance the hydrophobic behavior of anionic dyes. 1-undecanol and ethanol were used as the extraction and dispersion solvents, respectively. The dyes were quantitatively extracted in the presence of KCl (0.15 mol L -1 ) at pH 4.0. The method exhibits wide linearity (15.0-1500.0 μg L -1 for AR, 35.0-2000.0 μg L -1 for TAR, and 3.0-1200.0 μg L -1 for FG) with preconcentration factors of 19.6, 20.1, and 19.9, respectively. The detection limit was 3.7. 9.5, and 0.83 μg L -1 for AR, TAR, and FG, respectively. The relative standard deviation did not exceed 2.1 %. The procedure was applied for the determination of these dyes in food samples., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

The 3,3',5,5'-tetramethylbenzidine-H 2 O 2 (TMB-H 2 O 2 ) platform has gained widespread use for rapid detection of various analytes in foods. However, the existing TMB-H 2 O 2 platforms suffer from limited accuracy, as their signal output is confined to the visible region, which is prone to interference from various food colorants in real samples. To address this challenge, a novel Au@Os-mediated TMB-H 2 O 2 platform is developed for both rapid and accurate detection of analytes in foods. The prepared Au@Os NPs exhibit remarkable peroxidase-like activity, making the platform display dual absorption peaks in visible and near-infrared (NIR) regions, respectively. This Au@Os-mediated TMB-H 2 O 2 platform exhibited three linear ranges across different concentrations of ziram from 1-100, 150-600, and 800-2000 nM with limit of detection (LOD) 7.9 nM and limit of quantification (LOQ) 24.15 nM respectively. Further, the Au@Os-mediated TMB-H 2 O 2 platform was also used for rapid and accurate detection of ziram in real food samples like apple, tomato, and black tea., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

The hibiscus calyx contains 0.3-2.4% total anthocyanins, and is a promising source for naturally red food colorants. In this study, commercially available hibiscus calyces were subjected to ethanolic-aqueous extraction and chromatographic enrichment with the XAD-7HP resin, to create scalable, high-anthocyanin and low-acidity natural food colorants. Anthocyanins, organic and phenolic acids were monitored after each step using UHPLC-DAD and UHPLC-QQQ/MS. 75.67% total anthocyanins were recovered from calyces after double extractions, and the content increased by 8.50-14.90 times after the column enrichment, reaching 14.51-31.90% (by dry weight) in the final product. Chromatographic fractionation was also shown to effectively increase the total phenolic acids by 11.01-16.22 times, and remove an average of 98.58% of the total organic acids. High intensity redness at pH 2.5-3.5 indicated that the final product may be a promising, versatile natural food and beverage colorant in low pH products., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

In Chile, limited information is available on colorants in commonly consumed foods among vulnerable age groups. We developed and validated a rapid HPLC-DAD method to simultaneously evaluate 11 synthetic colorants in candies, beverages, ice cream, and cereals. The method exhibited excellent analytical performance for all 11 colorants with LOD (0.44 - 1.55 mgL -1 ), LOQ v(1.32 - 4.70 mgL -1 ), precision (4.0 and 7.3% RSD), and recovery (80 - 105%) in fortified matrices (10-50-100 mgL -1 ). The highest detection frequencies were as follows: cereals > candies > beverages > ice cream. Sunset Yellow was the most prevalent colorant in all food matrices, followed by Allura Red and Azorubine. Positive samples contained between 1 and 5 synthetic colorants. With the exception of cereals, the colorant concentrations in the remaining matrices exceeded the Codex Alimentarius regulations and the values reported in other studies worldwide, indicating the Chilean population is at risk., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)

4(5)-methylimidazole (4-MeI) is a potential carcinogen widely used in food colours. EU regulations specify a maximum allowable concentration of 200 ppm for 4-MeI in caramel colours. This study reports an electrochemical determination technique for 4-MeI in caramel colours for the first time. The effect of pH and interference from air were studied to optimize the detection conditions on a glassy carbon electrode in aqueous alkaline solutions using square wave voltammetry (SWV) technique. The concentration of 4-MeI was quantitatively measured down to 10 μM (∼0.8 ppm). Traditional methods such as HPLC, GC, spectrometry and immunoassays involve either expensive instrumentation and reagents or time consuming preparation and detection processes. This study demonstrates the possibility of rapid and simple electrochemical determination of (4-MeI) in food colours with minimum workup using a portable potentiostat., Competing Interests: Declaration of competing interest There are no conflicts to declare., (Copyright © 2024 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Aluminum is added to many food colors to change their solubility. This study compares the aluminum-containing food color carmine with its aluminum-free version carminic acid (both E 120), hypothesizing that the addition of aluminum does not only change the color's solubility, but also its effects on human cells. We could show that carmine, but not carminic acid, is taken up by gastrointestinal Caco-2 and umbilical vein endothelial cells (HUVEC). Clear differences between gene expression profiles of Caco-2 cells exposed to carmine, carminic acid or control were shown. KEGG analysis revealed that carmine-specific genes suppress oxidative phosphorylation, and showed that this suppression is associated with neurodegenerative diseases such as Alzheimer and Parkinson disease. Furthermore, carmine, but not carminic acid, increased proliferation of Caco-2 cells. Our findings show that a food color containing aluminum induces different cellular effects compared to its aluminum-free form, which is currently not considered in EU legislation., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Author(s). Published by Elsevier Ltd.. All rights reserved.)

Solid-state SERS sensors are desirable point-of-care tools due to their portability. However, the level of SERS sensitivity achieved in liquid phase is rarely duplicated in the solid phase. We report herein the fabrication of a SERS sensor using alumina beads as the solid support and demonstrate its high SERS sensitivity with the model analyte 4-aminophenyl disulfide (4-APDS). The key to sensitivity is a hydrophilic-hydrophobic surface gradient constructed by sequentially coating with the surfactant cetyltrimethylammonium bromide and fluorous 1H,1H,2H,2H-perfluorooctyltriethoxysilane. The surface gradient, together with chloride etching, allows the detection of 4-APDS at the low concentration of 10 -15 M. The practicality of the sensor beads is evidenced by successfully tracking the SERS fingerprints of five food colorant standards in the SERS spectra of a popular candy product. These SERS sensor beads are easy to prepare, convenient to use, and highly responsive as a SERS platform for the analysis of colorants., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

The use of artificial colorants in food is highly regulated due to their potential to harm human health. Thus, it is crucial to detect these substances effectively to ensure conformance with industrial standards. In this work, we prepared a photomultiplier tube (PMT)-based electrochemiluminescence (ECL) sensor and a charged coupled device (CCD)-based ECL sensor and compared their merits in the detection of sunset yellow (SY) dye. The sensors used C,N quantum dot-embedded g-C 3 N 4 nanosheets (QDs@NSs) as the ECL agent and K 2 S 2 O 8 as the coreactant. SY was analyzed on the basis of amplification in the QDs@NHs-K 2 S 2 O 8 ECL system. The PMT-based sensor realized ultrasensitive detection using a single electrode, especially at low concentrations of SY. A CCD-based sensor imaged the ECL phenomenon of an electrode array and provided the advantages of high throughput and time savings. Under optimized conditions, both sensors exhibited high specificity, reproducibility and stability; detection limits of 20 nM with PMT detection and 5 μM with CCD detection were determined for SY, with detection ranging over at least two decades. The practical feasibilities of these systems were confirmed by satisfactory detection of SY in real drink samples., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

A LC-Q-Orbitrap HRMS analytical method for both qualitative screening and quantitative determination of 90 synthetic dyes including ten groups of isomers in foods has been established. An in-house synthetic dyes database and characteristic ions were also developed. Based on Q-Orbitrap HRMS, mass spectrum and fragmentation patterns of synthetic dyes were studied, which indicated that double charged ions were usually the main precursor ions. Matrix effects were successfully eliminated by the C 18 d-SPE clean-up coupled with dilute and shoot approach with methanol-water (1:4, v/v) in 100-fold. For most of the compounds, mean recoveries were satisfactory between 70% and 120% with RSD < 20% at three spiked level in the range of 0.025-1.0 mg/kg. The screening detection limits ranged from 0.025 - 1.0 mg/kg. Method validation showed that the established method was efficient, rapid and high-throughput, which has been successfully applied to the monitoring of these water-soluble synthetic dyes in foods., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

In this paper, using a carbon paste electrode (CPE) modified with 1-ethyl-3-methylimidazolium chloride as an ionic liquid (IL) and NiFe 2 O 4 -rGO nanocomposite (IL/NiFe2O4/rGO/CPE), a sensitive and effective electrochemical sensor is applied to analyze Sunset Yellow. The X-ray diffraction (XRD), Scanning Electron Microscopy (SEM) with Energy Dispersive X-Ray Analysis (EDX) and Fourier-transform infrared spectroscopy (FTIR) are employed to characterize the synthesized NiFe 2 O 4 -rGO nanocomposite. The oxidation peak currents of colorants were obtained by CV and DPV techniques; and as a result, the two linear ranges from 0.05 to 30 μM (R 2  = 0.9939) and 30 to 500 μM (R 2  = 0.9953) along with LOD of 0.03 μM for Sunset Yellow is obtained. The proposed sensor is successfully applied to determine the Sunset Yellow, Tartrazine and Allura Red in PBS (pH 3). The IL/NiFe 2 O 4 /rGO/CPE displays a high performance for analysis of these dyes in hair shampoo and an orange juice as real samples with acceptable results., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

The aim of the present study was to evaluate the phenolic composition of crude lyophilized extracts (CLE) and partially purified (PPE) extracts of C. ternatea blue petals as well as the anthocyanin stability against pH, temperature and light in the presence and absence of fructooligosaccharides. Twelve compounds were tentatively identified by UHPLC-Q-TOF-MS/MS in CLE and PPE extracts. In direct/reverse spectrophotometric titration, anthocyanins showed colour changes between pH 2.25 to 10.20, and colour reversibility, maintaining antioxidant activity against the DPPH radical. The aqueous extracts at pH 3.6 and 5.4 exhibited thermal stability with the presence and absence of fructooligosaccharides with activation energy higher than 99 kJ/mol. The addition of fructooligosaccharides in the extracts at pH 5.4 exposed to light provided a protective effect against anthocyanin photodegradation. The data show the technological potential of aqueous extract of C. ternatea blue petals as a natural colourant in a functional beverage model system., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Despite the daily consumption of copper chlorophylls (E-141i), the green food colorants in foods high in fats, there is a general need for knowledge regarding their exact composition. Consequently, we have analyzed by HPLC-ESI(+)/APCI(+)-hrTOF-MS 2 the accurate composition of different commercial copper chlorophyll colorants for the first time. Data showed a favored yield of copper pheophytins from a series, while pheophytins from b series are preferentially no complexed with copper. The copper pheophytins present in the food colorants consisted mainly of three structural rearrangements. New fragmentation patterns and structural assignments have been described for several copper pheophytins. During the ingestion of copper chlorophylls, no chlorophyll derivative was present in serum nor urine except a new copper-pyroporphyrin a accumulated in a few livers. In any case, this green additive could represent the ideal food colorant, as most of the copper pheophytins are excreted in the feces showing almost no absorption of copper-chlorophylls compounds., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

A reasonable, high sensitive and accurate analytical method for the determination of 20 allergenic disperse dyes in foodstuffs was developed and validated. The obtained results showed that an ultra high liquid performance chromatography system - equipped with tandem quadrupole mass spectrometry (UHPLC-MS/MS) proved to be ideal for the selected method enabling multidimensional processing of the samples. Under optimized conditions, validation results showed excellent linearity (5-1000 µg/L, r 2  ≥ 0.997), limits of detection (LODs, 1.1-10.8 μg/kg), recoveries (60.2-110.3%) and precision (RSDs ≤ 12.6%) for the twenty disperse dyes under investigation. The developed method was successfully applied to the analysis of 20 disperse dyes in real foodstuffs demonstrating the validity and applicability of the current method for continuing monitoring of the selected dyes. The proposed UHPLC-MS/MS is thus proved to be a convenient, effective, sensitive and timesaving method for the isolation and determination of allergenic disperse dyes in edible packaging and other foodstuffs., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

A green and simple method was designed to synthesize polyethyleneimine (PEI)-modified magnetic nanoparticles (MNPs), which were later used as adsorbents in magnetic solid phase extraction (MSPE) process. A new MSPE-HPLC method was then established for the simultaneous determination of four representative synthetic colorants (Amaranth, Ponceau 4R, Sunset yellow and Allure red) in food samples. Several important factors, such as the pH of the sample solution, the amount of adsorbent, the adsorption time, and the type of the eluent were investigated in detail. Under the optimized experimental conditions, the four colorants were measured with good linearity, detection limit and quantification limit. Adsorption kinetics and isotherms were also investigated to elucidate the adsorption mechanism. The detection of four colorants in candy, jelly and carbonated drink proved that the established MSPE-HPLC method was simple and effective and can be used for the analysis of colorants in real samples., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

In current research, a sensitive screen printed electrochemical sensor on the basis of La 3+ -doped Co 3 O 4 nanocubes was fabricated to determine sudan I. The electrochemical performance of sudan I at this sensor was investigated in detail, presenting that this sensor had electrocatalytic behavior for oxidizing sudan I due to the significant peak current enhancement and the dropping of oxidation overpotential. Under the optimum conditions, the linear response range for sudan I concentrations by the modified sensor was 0.3-300.0 µM, and detection limit was 0.05 µM. Lastly, the suggested technique was also studied as a selective, easy, and exact electrochemical sensor to determine sudan I in food samples, including chili powder, tomato paste, and ketchup sauce., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

The current study performed simultaneous identification of semisynthetic chlorophyllin (Cu-Chl) and synthetic food colorants in food matrices. The quantitative assessment of these synthetic and semisynthetic colorants was determined by using analytical method based on reverse-phase high-performance liquid chromatography (RP-HPLC) equipped with UV-visible detection. The concentration of Cu-Chl in hard candy was 3.334 mg/kg and 4.489 mg/kg in the soft candy, while contents of other colorants i.e. Tartrazine and Brilliant Blue were within 4.74-140.284 mg/kg. The extraction of Cu-Chl and synthetic colorants from different food matrixes was performed with a recovery range of 90-97% and RSD of 1-9%. Overall, the current developed RP-HPLC method could detect both green coloured synthetic and semisynthetic food colorants by a single run and could be used for monitoring different colorants in other complex matrices. This is the first report in India to determine Cu-Chl in foodstuffs and beverages by using RP-HPLC with UV-vis detector., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Magnetic textile solid phase extraction, based on the use of magnetically modified non-woven textile impregnated with chitosan, was successfully employed for the preconcentration of acid food dyes from water solutions. The photos of textile squares with the adsorbed dye were taken with a mobile phone. The image analysis of the photos was performed using appropriate freeware. The values of saturation, obtained through the HSB color space, were proportional to the dye concentration in the analyzed samples. Described inexpensive, simple and elution free assay enables analysis of dyes concentration in various solutions. This novel method has a potential to be a useful alternative to existing semiquantitative determination procedures, especially for dyes analysis., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Color additives are used widely by the food industry to confer a desirable appearance. Some of the most used colorants (Tartrazine (E102), Sunset Yellow (E110), Red Allure (E129) and Blue Brilliant (E133)) were determined in this study using microemulsion electrokinetic capillary chromatography (MEEKC). Regression coefficients were greater than 0.9981; intra- and inter-day precisions, in terms of percentage RSD, were less than 7.01% and 8.55%, respectively; recoveries were between 90 and 100% in most cases. LODs and LOQs ranged from 0.24 to 1.21 mg L -1 and from 0.80 to 4.03 mg L -1 , respectively. Moreover, MEEKC consumed less solvent than HPLC, making the analysis more environmentally friendly. The proposed method is suitable for the determination of colorants in a wide variety of foods. Results showed that consumers should be aware of colorants to avoid consumption exceeding recommended amounts., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Vaccinium bracteatum leaves (VBTL) are traditionally used in China to dye rice grains, which assume a deep blue color, named 'Wu mi'. Information on the mechanism of pigment formation is limited. In this study, CIELAB color space parameters were used to represent the color of 'Wu mi'. Precursor compounds of pigments formed during the dyeing process were identified by UPLC Q-TOF MS analysis. The changes in co-factors for pigment formation in VBTL were measured at different growth stages. The L ∗ and b ∗ values of dyed rice increased as the leaves aged, whereas a ∗ values showed irregular changes. Six compounds were tentatively identified as pigment precursors by UPLC Q-TOF MS analysis. The pH and β-glucosidase activity at different growth stages of VBTL were indicated to be crucial co-factors for pigment formation. A tentative hypothesis is presented that iridoid glycosides are hydrolyzed by acids and β-glucosidases to form a dialdehyde structure that binds covalently with amino residues of lysine side chains in rice protein molecules., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Ambient mass spectrometry using an interchangeable thermal desorption/electrospray ionization source (TD-ESI) is a relatively new technique that has had only a limited number of applications to date. Nevertheless, this direct-analysis technique has potential for wider use in analytical chemistry (e.g., in the rapid direct detection of contaminants, residues, and adulterants on and in food) when operated in dual-working mode (pretreatment-free qualitative screening and conventional quantitative confirmation) after switching to a TD-ESI source from a conventional ESI source. Herein, we describe the benefits and challenges associated with the use of a TD-ESI source to detect adulterants on traditional Chinese pastries (TCPs), as a proof-of-concept for the detection of illegal colorants. While TD-ESI can offer direct (i.e., without any sample preparation) qualitative screening analyses for TCPs with adequate sensitivity within 30 s, the use of TD-ESI for semi-quantification is applicable only for homogeneous matrices (e.g., tang yuan)., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

A novel, unique electroanalytical method was developed for the simultaneous quantification of the dyes indigo carmine (IC) and allura red (AR) in candies by coupling flow injection analysis and multiple pulse amperometry with a cathodically pretreated boron-doped diamond electrode, using 0.30 mol L -1 H 2 SO 4 as supporting electrolyte. A dual-potential waveform was employed, causing the electrooxidation of either IC solely or IC and AR simultaneously. Thence, subtraction of current signals was used to quantify IC and AR in the concentration ranges of 70.0-1000 nmol L -1 and 40.0-770 nmol L -1 , with limits of detection of 40.0 nmol L -1 and 7.0 nmol L -1 , respectively. The proposed method, which permits up to 153 determinations per hour with good precision, was successfully applied in the quantification of these dyes in samples of commercial candies; their obtained contents were similar (at a 95% confidence level) to those from a comparative HPLC method., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

In this study, a rapid and reliable pretreatment method called dispersive liquid-liquid microextraction (DLLME) was developed for the determination of 4(5)-methylimidazole (4-MeI) in beverages. The clean-up samples were analyzed by a high performance liquid chromatography coupled with triple quadrupole mass spectrometer (HPLC-MS/MS) using a reversed-phase C18 column (250 mm × 4.6 mm, 5 μm). The matrix effects and the fault of DLLME operation were corrected by the isotope dilution technique. The developed method exhibited the limit of quantification (0.3 μg L -1 ) and excellent linearity (R 2  = 0.999). In addition, the recovery values of 4-MeI in carbonated beverage were ranging from 102.60% to 113.22%, in soft drinks were ranging from 103.24% to 108.85%. The content 4-MeI was detected in thirteen beverage samples treated with DLLME and solid phase extraction method (SPE) (ranging from 6.4 to 165.5 μg L -1 ). The consistent result of 4-MeI content detected by DLLME and SPE method concluded that the established method on the basis of DLLME was rapid, robust and accurate for the trace 4-MeI determination in beverages., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

Surface Enhanced Raman Scattering (SERS) spectroscopy technology is widely used in materials analysis, environmental monitoring, biomedical, food security and other fields. Flower-shaped silver nanoparticles have been successfully synthesized by a simple aqueous phase silver nitrate reduction by ascorbic acid in the presence of polyvinylpyrrolidone (PVP) surfactant. The nanoparticles diameters were adjusted from 450 to 1000nm with surface protrusions up to 10-25nm. The flower-shaped silver nanostructures obtained were used as stable SERS substrates with high SERS activity for detecting Rhodamine 6G (R6G), at a concentration of only 10 -9 mol/L, where the SERS signal is still clear. SERS spectroscopy of four different food colorants (e.g. food blue, tartrazine, sunset yellow, acid red) were analysed and the characteristic bands were identified. An improved principle component analysis (PCA) was used for four different food colorants detection, at concentrations down to about 10 -8 mol/L. Thus, the LOD of food blue, tartrazine, sunset yellow and acid red are 79.285μg/L, 5.3436μg/L, 45.238μg/L and 50.244μg/L, respectively., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

We have focused on exploring pH- and ionic strength-modulated binding of acid red 1 (AR1) and acid green 50 (AG50) with bovine serum albumin (BSA) by fluorescence, UV-vis absorption and FTIR spectra. The results implied that the quenching mechanism of BSA-AR1/AG50 system was a static quenching, electrostatic force dominated the formation of BSA-AR1/AG50 complex, and the binding affinity of AR1 was greater than that of AG50 on the subdomain IIA of BSA. Moreover, their true thermodynamic binding constant (Keq), true free energy change (ΔG(0)I→0), and effective charge (ZP) in the anion receptor pocket of BSA were calculated using Debye-Hückel limiting law. The local charge bound by AR1/AG50 rather than the overall or surface charge of BSA played a key role in determining their interaction strength. Besides, the thermal and structural stabilization of BSA was discussed by analyzing the changes of Tm and Hurea without/with the addition of AR1/AG50, respectively., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

A multi-residue method based on two different extraction procedures was developed and compared with liquid chromatography electrospray ionization tandem mass spectrometry analysis of eighteen water-soluble artificial colours including Tartrazine (E102), Chrysoine (E103), Quinoline Yellow (E104), Yellow 2G (E107), Sunset Yellow (E110), Azorubine (E122), Amaranth (E123), Ponceau 4R (E124), Erythrosine (E127), Red 2G (E128), Allura Red (E129), Patent Blue V (E131), Indigo Carmine (E132), Brilliant Blue (E133), Green S (E142), Fast Green (E143), Brilliant Black (E151), and Black 7984 (E152) in sugar and gummy confectionary, ice-cream, and chocolate sweets. Sample preparation included SPE clean-up and liquid-liquid extraction for ice-cream and chocolate sweets. Accuracy was evaluated by recovery experiments. Correlation between response and concentration was obtained with R(2)>0.98 for all but six colours. Limits of quantification were within the 10-50 μg/kg range for E129; 20-200 μg/kg for E152; 10-250 μg/kg for E103; 10-500 μg/kg for E102, E104, E107, E110, E122, E123, E124, E127, E128, E131, E133; 20-800 μg/kg for E132, 142, 151; and 10-1000 μg/kg for E143. CV for repeatability ranged from 4.0% to 51.0%, while the CV for intermediate reproducibility ranged from 5.8% to 41.4%. Finally, recoveries varied from 84.3% to 166.0%. Together, these demonstrate that the method has been validated for complex matrices and is, thus, fit-for-purpose., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Fast Green FCF (FCF), Patent Blue V (PBV) and Acid Blue 1 (AB1) are used as food colorants. Multiple spectroscopic techniques were employed to probe in depth the affinity of FCF/PBV/AB1 with BSA in different pH and/or salt concentrations. The results showed that FCF/PBV/AB1 quenched the intrinsic fluorescence of BSA by a static process, and electrostatic force dominated the formation of BSA-FCF/PBV/AB1 complex which was confirmed by the effects of salt on their interactions. Subdomain IIA was the primary binding site for FCF/PBV/AB1 on BSA in the pH range of 5.5-7.4, while both Trp 212 and Trp 134 residues of BSA might be bound by FCF/PBV/AB1 at pH 4.8. The K values suggested that the binding ability of three food colorants with BSA was FCF>PBV>AB1. The results of UV-vis absorption, synchronous fluorescence, 3D fluorescence and FT-IR spectra proved that the structure of BSA altered by FCF/PBV/AB1., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

This article reports on a method to determine synthetic dyes in yogurts and milk drinks. Initially a method for extraction of artificial dyes was developed to pretreat samples in order to extract most of the artificial colorants. Then, the colorants were analyzed by HPLC-PAD using gradient elutions. The method was linear in the range of 0.5-25mgL(-1) colorants (0.9991

A novel poly (diallyldimethylammonium chloride) functionalized reduced graphene oxide (PDDA-RGO) nanocomposite modified electrode was fabricated, and applied for the electrochemical determination of quinoline yellow (QY). The formation of PDDA-RGO nanocomposite was confirmed by SEM, FTIR and Raman spectroscopy. The electrocatalytic activity of PDDA-RGO nanocomposite to the oxidation of QY was evaluated using cyclic voltammetry and differential pulse voltammetry. Under the optimal conditions, the proposed sensor exhibited excellent electrochemical performance towards detection of QY. The linear range is from 0.01 to 10 μM, and the detection limit is down to 0.002 μM (S/N=3). The proposed sensor also exhibited excellent anti-interference property, repeatability and stability. In addition, the proposed electrochemical sensor was successfully applied to determination of QY in soft drink., (Copyright © 2015. Published by Elsevier Ltd.)

Reliable methods for quantification of synthetic water-soluble colors in complex food matrices are currently not available. The present work describes the development and validation of an improved protocol for the analysis of synthetic food colorants in complex food matrices presenting high protein and/or fat content. The method developed employs an extraction stage, followed by a subsequent sonification, centrifugation and concentration step. A final clean up via SPE on polyamide cartridges was also employed. The isolated colorants were separated and analyzed by an RP-HPLC/DAD system. High and consistent recoveries (min. 81%) and low RSDs (max. 6%) were achieved for all studied colorants. The issue of high fat content matrices was also addressed showing the need for an additional defatting step in the procedure. Overall, the protocol presented shows high precision and accuracy of detection and can provide the basis for future development of similar methods in other complex food matrices., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

A rapid and effective method of aqueous two-phase systems based on ionic liquid microextraction for the simultaneous determination of five synthetic food colourants (tartrazine, sunset yellow, amaranth, ponceau 4R and brilliant blue) in food samples was established. High-performance liquid chromatography coupled with an ultraviolet detector of variable wavelength was used for the determinations. 1-alkyl-3-methylimidazolium bromide was selected as the extraction reagent. The extraction efficiency of the five colourants in the proposed system is influenced by the types of salts, concentrations of salt and [CnMIM]Br, as well as the extracting time. Under the optimal conditions, the extraction efficiencies for these five colourants were above 95%. The phase behaviours of aqueous two-phase system and extraction mechanism were investigated by UV-vis spectroscopy. This method was applied to the analysis of the five colourants in real food samples with the detection limit of 0.051-0.074 ng/mL. Good spiked recoveries from 93.2% to 98.9% were obtained., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

In the present work, a new method for the determination of Sudan I has been developed based on a conducting poly(p-aminobenzene sulphonic acid) (poly(p-ABSA)) film modified electrode. The new electrochemical sensor showed strong accumulation ability and excellent electrocatalytic activity for Sudan I. Electrochemical oxidation signal of Sudan I at the poly(p-ABSA) modified glassy carbon electrode (poly(p-ABSA)/GCE) was significantly increased when compared to that at the bare GCE. The experimental conditions such as amount of alcohol, pH of buffer solution, accumulation time, and instrumental parameters for square wave anodic stripping voltammetry were optimised for the determination of Sudan I. Under optimum conditions, the linear regression equation of Sudan I was ip=1.868+0.1213c (ip: μA, c: μgL(-1), R=0.9981) from 1 to 500 μg L(-1) with a detection limit of 0.3 μg L(-1). Finally, this sensor was successfully employed to detect Sudan I in some hot chili and ketchup samples., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

In this work, a simple, rapid and sensitive analytical method for the determination of rhodamine B in chili-containing foodstuffs is described. The dye is extracted from samples with methanol and analysed without further cleanup procedure by high-performance liquid chromatography (HPLC) coupled to fluorescence detection (FLD). The influence of matrix fluorescent compounds (capsaicin and dihydrocapsaicin) on the analysis was overcome by the optimisation of mobile-phase composition. The limit of determination (LOD) and limit of quantification (LOQ) were 3.7 and 10 μg/kg, respectively. Validation data show a good repeatability and within-lab reproducibility with relative standard deviations <10%. The overall recoveries are in the range of 98-103% in chili powder and in the range of 87-100% in chili oil depending on the concentration of rhodamine B in foodstuffs. This method is suitable for the routine analysis of rhodamine B due to its sensitivity, simplicity, reasonable time and cost., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Synthetic food colourings were analyzed on commercial carbonated orange and grape soft drinks produced in Ceará State, Brazil. Tartrazine (E102), Amaranth (E123), Sunset Yellow (E110) and Brilliant Blue (E133) were extracted from soft drinks using C18 SPE and identified by thin layer chromatography (TLC), this method was used to confirm the composition of food colouring in soft drinks stated on label. The concentration of food colouring in soft drink was determined by ion-pair high performance liquid chromatography with photodiode array detection. The results obtained with the samples confirm that the identification and quantification methods are recommended for quality control of the synthetic colours in soft drinks, as well as to determine whether the levels and lables complies with the recommendations of food dyes legislation., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

A method for simultaneously determining four artificial food colourants [Red Nos. 2 (R2) and 40 (R40), Yellow Nos. 5 (Y5) and 6 (Y6)] and three carotenoids [lycopene, lutein, and β-carotene] was developed. They were successfully separated by the developed high pressure liquid chromatography (HPLC) method combined with a photo diode array detector. The detection limit (at signal to noise>4) was from the lowest of 0.2 ng/mL for lutein to the highest of 50.0 ng/mL for R40. With a two-phase solvent and ultrasound-assisted extraction, the recoveries of the artificial and natural pigments in fifteen different types of food products were between 80.5-97.2% and 80.1-98.4%, respectively. This HPLC method with the ultrasound-assisted extraction protocol could be used as a sensitive and reliable analysis technique in simultaneously identifying and quantifying the reddish and yellowish pigments in different foods regardless of they are artificial food colourants or/and natural carotenoids., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

A method was developed for the simultaneous determination of 14 fat-soluble dyes in chilli products. The samples were extracted with hexane/acetone. The cleanup was performed with gel permeation chromatography (GPC) cleanup system. A HPLC separation was performed using variable wavelength detector and a gradient elution with 0.1% formic acid and methanol-acetonitrile (1:1, v/v) as the mobile phases. Good linearity (R² ≥ 0.995) was observed between 0.1 and 5.0 μg/mL. Detection limits of the investigated dyes, which were evaluated at signal to noise ratio of 3, were in the ranges of 11-71 μg/kg. The recoveries of the 14 synthetic colourants in three matrices ranged from 73.4% to 103.5%. Relative standard deviations ranged from 3.7% to 12.3%. The method has been successfully used for the determination of banned dyes in real samples., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Currently, synthetic colourants draw much attention as food additives. This paper investigated the simultaneous electrocatalytic oxidation of sunset yellow and tartrazine, two yellow colourants commonly present in food together, with a novel voltammetric sensor based on graphene and mesoporous TiO2 modified carbon paste electrode. Due to the high accumulation effect and great catalytic capability of graphene and mesoporous TiO2, the developed sensor exhibited well-defined and separate square wave voltammetric peaks (i.e., 272 mV) for sunset yellow tartrazine. The peak currents of sunset yellow and tartrazine increased linearly with their concentration in the ranges of 0.02-2.05 μM and 0.02-1.18 μM, respectively. And the detection limit was 6.0 and 8.0 nM for sunset yellow and tartrazine, respectively. This new sensor was applied to determine sunset yellow and tartrazine in several food sample extracts. Results suggested that the proposed sensor was sensitive, rapid and reliable., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

A novel and simple rapid shaking-based method of ionic liquid dispersive liquid phase microextraction for the determination of six synthetic food colourants (Tartrazine, Amaranth, Sunset Yellow, Allura Red, Ponceau 4R, and Erythrosine) in soft drinks, sugar- and gelatin-based confectionery was established. High-performance liquid chromatography coupled with an ultraviolet detector was used for the determinations. The extraction procedure did not require a dispersive solvent, heat, ultrasonication, or additional chemical reagents. 1-Octyl-3-methylimidazolium tetrafluoroborate ([C8MIM][BF4]) was dispersed in an aqueous sample solution as fine droplets by manual shaking, enabling the easier migration of analytes into the ionic liquid phase. Factors such as the [C8MIM][BF4] volume, sample pH, extraction time, and centrifugation time were investigated. Under the optimum experimental conditions, the proposed method showed excellent detection sensitivity with limits of detection (signal-to-noise ratio=3) within 0.015-0.32 ng/mL. The method was also successfully used in analysing real food samples. Good spiked recoveries from 95.8%-104.5% were obtained., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Tartrazine dye Na(3)TZ in foodstuff products was determined by a new modified carbon paste electrode, encoded sensor A, and a coated silver wire electrode, encoded sensor B, based on tartrazine TZ- cetryltrimethyl ammoniumbromide CTAB as a chemical modifier TZ-CTA. The electrodes exhibit the following characteristics listed respectively: a Nernstian slope of 17.9±0.5 and 19.4±0.2 mV/decade for tartrazine ion over a wide concentration range from 4.3×10(-7) to 1.0×10(-2) and 1.1×10(-7) to 1.0×10(-2) M. The lower detection limits: 3.2×10(-7) and 5.5×10(-8) M. Short response time (5-8 s) over the pH range 3.8-7.7 and 4.2-8.1. The proposed sensors display significantly high selectivity for TZ ion over a wide variety of sugars, some anions, common organic, inorganic compounds and additives. The developed electrodes were applied to the potentiometric determination of tartrazine ion in different kinds of foodstuffs: solid jelly (strawberry and custard) powder samples and soft drink (orange) samples with satisfactory results., (Copyright © 2012 Elsevier Ltd. All rights reserved.)