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Current Analytical Chemistry Yasmeen Mutlaq Ghazi Al Shamari 1 , Saikh Mohammad Wabaidur 1 , Abdulrahman Abdullah Alwarthan 1 , Moonis Ali Khan 1 and Masoom Raza Siddiqui 1,* 1 Chemistry Department, College of Science, King Saud University, Post Box No. 2455, Riyadh 11451 Saudi Arabia Abstract: Background: A new method has been developed for the determination of food dye tartra- zine in soft drinks. Tartrazine is determined by hyphenated technique Ultra Performance Liquid Chromatography coupled with Mass spectrometry. The solid-phase extraction was used for the ex- traction of tartrazine. Methods: For the LC-MS analysis of tartrazine acetonitrile, water (80:20) was used as a mobile phase whereas, the C-18 column was selected as the stationary phase. The chromatographic run was allowed for 1 min. The adsorbent of the solid-phase extraction was synthesized from the waste corn cob. Results: Method found to be linear in the range of 0.1 mg L -1 - 10 mg L -1 , limits of detection and quantitation were found to be 0.0165 mgL -1 and 0.055 mgL -1 , respectively. Tartrazine, in the real sample, was found to be 20.39 mgL -1 and 83.26 mgL -1 . Conclusion: The developed UPLC-MS method is rapid, simple, precise and can be used for the quantitative analysis of tartrazine. The solid-phase extraction also involves a cost-effective procedure for extraction as it does not involve the commercial cartridge. A R T I C L E H I S T O R Y Received: July 20, 2019 Revised: September 30, 2019 Accepted: October 19, 2019 DOI: 10.2174/1573411015666191028113257 Keywords: Method development, soft drinks, solid phase extraction, tartrazine, UPLC-MS, adsorbent. 1. INTRODUCTION Tartrazine, IUPAC name, trisodium 5-hydroxy-1-(4-sul- fonatophenyl)-4-[(E)-(4-sulfonatophenyl)diazenyl]-1H-pyra- zole-3-carboxylate, is a synthetic, lemon yellow-colored wa- ter-soluble dye, predominantly used as a food coloring agent. In addition to its food applications, tartrazine also finds its usage in personal care products, cosmetics products, phar- maceutical formulations and some other household products such as paper plates, crayons, face paints, etc. Moutinho et al. reported that sulfanylic acid is the prime metabolite which is identified to date [1]. The Joint FAO/WHO Expert Committee on Food Additives (JECFA), the expert commit- tee on food additive in the year 1964, has established an ac- ceptable daily permissible intake of 7.5 mg per kg of body- weight. It has been reported by Andrade et al. [2] that the highest level of tartrazine should not be more than 100.0 mg L -1 in non-alcoholic beverages. Despite several applications and numerous usage in daily life, tartrazine is reported to be *Address correspondence to this author at the Chemistry Department, Col- lege of Science, King Saud University, Post Box No. 2455, Riyadh 11451 Saudi Arabia; Tel: +966-11-4674198; E-mail: [email protected] hazardous when taken in larger amount. Several researches have highlighted the health concerns related to the consump- tion of tartrazine. It has been reported that tartrazine happens to be an allergen and causes intolerance reactions to those who are asthmatic or having aspirin intolerance [3]. Over activities among children may result when the tartrazine is conjugated with benzoic acid. Taking into consideration its use as a colorant in the soft drinks and, most importantly, the health issues related to the high amount of consumption, a new rapid method with an easy and cost-effective extraction process needs to be developed. In view of its importance in human use, tartrazine has a considerable presence in the lit- erature survey. Several methods have been developed for tartrazine determination in different matrices including the beverages. Starting with the electrochemical methods, poten- tiometric sensors involving carbon paste and coated silver electrodes were used for tartrazine determination in food- stuffs [4, 5]. Voltammetry is another important technique although a bit primitive yet used these days for different pos- itive reasons including cost-effectiveness. Tartrazine has to be assayed by different voltammetric techniques such as square wave, cyclic and differential pulse which were ap- 1875-6727/20 $65.00+.00 © 2020 Bentham Science Publishers Send Orders for Reprints to [email protected] 924 Current Analytical Chemistry, 2020, 16, 924-932 RESEARCH ARTICLE Corncob Waste Based Adsorbent for Solid Phase Extraction of Tartrazine in Carbonated Drinks and Analytical Method using Ultra Performance Liquid Chromatography-Mass Spectrometry For personal private use only. Not be distributed or uploaded to anyone or anywhere.
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Page 1: in Carbonated Drinks and Analytical Method using Ultra ...

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Yasmeen Mutlaq Ghazi Al Shamari1, Saikh Mohammad Wabaidur1, Abdulrahman Abdullah Alwarthan1, Moonis Ali Khan1 and Masoom Raza Siddiqui1,*

1Chemistry Department, College of Science, King Saud University, Post Box No. 2455, Riyadh 11451 Saudi Arabia

Abstract: Background: A new method has been developed for the determination of food dye tartra-zine in soft drinks. Tartrazine is determined by hyphenated technique Ultra Performance Liquid Chromatography coupled with Mass spectrometry. The solid-phase extraction was used for the ex-traction of tartrazine.

Methods: For the LC-MS analysis of tartrazine acetonitrile, water (80:20) was used as a mobile phase whereas, the C-18 column was selected as the stationary phase. The chromatographic run was allowed for 1 min. The adsorbent of the solid-phase extraction was synthesized from the waste corn cob.

Results: Method found to be linear in the range of 0.1 mg L-1 - 10 mg L-1, limits of detection and quantitation were found to be 0.0165 mgL-1 and 0.055 mgL-1, respectively. Tartrazine, in the real sample, was found to be 20.39 mgL-1 and 83.26 mgL-1.

Conclusion: The developed UPLC-MS method is rapid, simple, precise and can be used for the quantitative analysis of tartrazine. The solid-phase extraction also involves a cost-effective procedure for extraction as it does not involve the commercial cartridge.

A R T I C L E H I S T O R Y

Received: July 20, 2019 Revised: September 30, 2019 Accepted: October 19, 2019 DOI: 10.2174/1573411015666191028113257

Keywords: Method development, soft drinks, solid phase extraction, tartrazine, UPLC-MS, adsorbent.

1. INTRODUCTION

Tartrazine, IUPAC name, trisodium 5-hydroxy-1-(4-sul- fonatophenyl)-4-[(E)-(4-sulfonatophenyl)diazenyl]-1H-pyra- zole-3-carboxylate, is a synthetic, lemon yellow-colored wa-ter-soluble dye, predominantly used as a food coloring agent. In addition to its food applications, tartrazine also finds its usage in personal care products, cosmetics products, phar-maceutical formulations and some other household products such as paper plates, crayons, face paints, etc. Moutinho et al. reported that sulfanylic acid is the prime metabolite which is identified to date [1]. The Joint FAO/WHO Expert Committee on Food Additives (JECFA), the expert commit-tee on food additive in the year 1964, has established an ac-ceptable daily permissible intake of 7.5 mg per kg of body-weight. It has been reported by Andrade et al. [2] that the highest level of tartrazine should not be more than 100.0 mg L-1 in non-alcoholic beverages. Despite several applications and numerous usage in daily life, tartrazine is reported to be

*Address correspondence to this author at the Chemistry Department, Col-lege of Science, King Saud University, Post Box No. 2455, Riyadh 11451 Saudi Arabia; Tel: +966-11-4674198; E-mail: [email protected]

hazardous when taken in larger amount. Several researches have highlighted the health concerns related to the consump-tion of tartrazine. It has been reported that tartrazine happens to be an allergen and causes intolerance reactions to those who are asthmatic or having aspirin intolerance [3]. Over activities among children may result when the tartrazine is conjugated with benzoic acid. Taking into consideration its use as a colorant in the soft drinks and, most importantly, the health issues related to the high amount of consumption, a new rapid method with an easy and cost-effective extraction process needs to be developed. In view of its importance in human use, tartrazine has a considerable presence in the lit-erature survey. Several methods have been developed for tartrazine determination in different matrices including the beverages. Starting with the electrochemical methods, poten-tiometric sensors involving carbon paste and coated silver electrodes were used for tartrazine determination in food-stuffs [4, 5]. Voltammetry is another important technique although a bit primitive yet used these days for different pos-itive reasons including cost-effectiveness. Tartrazine has to be assayed by different voltammetric techniques such as square wave, cyclic and differential pulse which were ap-

1875-6727/20 $65.00+.00 © 2020 Bentham Science Publishers

Send Orders for Reprints to [email protected] 924

Current Analytical Chemistry, 2020, 16, 924-932

RESEARCH ARTICLE

Corncob Waste Based Adsorbent for Solid Phase Extraction of Tartrazine in Carbonated Drinks and Analytical Method using Ultra Performance Liquid Chromatography-Mass Spectrometry

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Page 2: in Carbonated Drinks and Analytical Method using Ultra ...

Corncob Waste Based Adsorbent for Solid Phase Extraction of Tartrazine Current Analytical Chemistry, 2020, Vol. 16, No. 7 925

plied to study either alone or in combination with other dyes, [6-10]. Poly (p-aminobenzenesulfonic acid)/zinc oxide na-noparticles were employed in the carbon paste electrode as a sensor for the quantitative analysis of tartrazine in soft drinks [11]. Partial least squares method and principal component regression multivariate calibration methods were used to determine tartrazine spectrophotometrically where calibra-tion range of tartrazine was in between 1.6-20.0 mg L-1 [12]. A similar type of work was also reported for the simultane-ous determination of tartrazine along with patent blue V and indigo [13]. A first derivative method is reported where tar-trazine is determined at 454 nm while the zero-order spec-trum was used for brilliant blue determination at 630 [14]. Tartrazine has been analyzed by HPLC in different food samples including soft drinks. Tartrazine, along with sunset yellow, were determined by HPLC post coupling with ionic liquid-based aqueous two-phase systems where the target matrices were soft drinks, powder drinks and candy; other method reports tartrazine along with eight colorants using gradient elution [15, 16]. The hyphenated chromatographic technique (UFPLC-MS/MS) has been applied for tartrazine estimation in buns without using the solid phase extraction [17] while structure elucidation of its degradation product identified to be 2,5-dihydroxy-1-phenyl-3-(phenyldiazenyl)-2,3-dihydro-1H-pyrazole-4-carboxylic acid [18]. LC/MS, along with cloud point extraction, were used for the analysis tartrazine along with few other coloring agents in all the three forms of liquid, solid and semi-solid foods [19]. In ad-dition to the method development, validation and determina-tion studies, this communication also involves the applica-tion of corncob as adsorbent material used in the solid-phase extraction of the dye. Several other materials were used pre-viously as an adsorbent for solid-phase extraction of differ-ent compounds it involves, cigarette filters, magnetic multi-walled carbon nanotubes and eggshell membrane templating of the mixed hemimicelle/admicelle of linear alkylbenzene-sulfonates [20-22].

2. EXPERIMENTAL

2.1. Chemicals

Tartrazine, methanol, acetonitrile, ethanol and acetone used during the study were procured from Sigma-Aldrich. Avonchem (U.K) manufactured ammonia solution was used to make the basic methanol solution to be used during the tartrazine elution process. NaOH used during the trails was manufactured by BDH (U.K). Water used throughout the study was obtained from a Millipore water system. The corncob was obtained from the local sweetcorn shop situated in Riyadh, Saudi Arabia.

2.2. Standard Solution

The standard tartrazine stock solution was prepared by dissolving 12.5 mg of tartrazine in 250 mL of Milli Q gener-ated water. Standard solution of the tartrazine for the calibra-tion preparation purpose was further prepared by appropri-ately diluting the stock solution to get nine calibration solu-tions of varied concentrations including 0.1, 0.4, 0.9, 1.3, 2.0, 3.0, 5.0, 7.5 and 10.0 mg L-1. Keeping in mind the pos-

sible stability issues, the stock and the standard solution were stored at the refrigerated condition with aluminum foil wrapped around the standard flask.

2.3. Instrumentation

Ultra Performance Liquid Chromatography-Mass spec-trometric technique was used to analyze the dyes in the soft drink. The instrumentation involves a combination of two techniques involving liquid chromatography and mass spec-trometry, where the previous one has the capabilities of physical separation while the later has the mass analyzing ability. Prior to the determination process, the extraction process was carried out to get the interference-free analysis of tartrazine.

2.4. Chromatographic Conditions

The chromatographic part of the study includes instru-mentation and experimental conditions. In the liquid chroma-tographic analysis, the experiment was carried out using the LC equipment (Acquity UPLC) manufactured by Waters Corps. USA. The binary solvent manager and sample man-ager remain part of the LC system. Proper selection of chro-matographic columns remains an important contributor for the separation of tartrazine, where Waters BEH C18 column (50 × 2.1 mm: 1.7 µm) was used for the determination pro-cess. Acetonitrile and water, with the contribution of former being 80% and that of water was 20%, were used as an iso-cratic mobile phase. A run time of 1 minute was fixed while the retention time of the tartrazine was found to be 0.36 minutes.

2.5. MS Conditions

Detection of the target analyte, tartrazine was executed using a mass spectrometer, Quattro Premier-triple quadru-pole with electrospray ionization source (Micro mass, Mil-ford, USA). To get the best detection results, the MS pa-rameters were optimized and since the tartrazine contains positive ion (Na+) in its moiety, negative ionization mode produced the best detection results. To initiate the MS tuning process, 5 µgmL-1 was infused into the mass spectrometry. The infused samples were mixed with the mobile phase with varying condition and finally getting the best results with the parameters mentioned in Table 1, and the optimized experi-mental parameters include, but not limited to, capillary volt-age, cone voltage, extractor voltage, source temperature and desolvation temperature.

2.6. Sample Collection and Preparation

Four liquid brands of soft drinks were collected from the local store in Riyadh. All the drinks were carbonated in na-ture. All the four samples were transferred in a 500 mL beaker and were allowed to degas by keeping the soft drinks sample for five minutes in an ultrasonic bath, with a precau-tion of bubbling out during degassing. To make the soft drink sample ready for the extraction process, the pH of all the samples was adjusted to pH 2.0.

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926 Current Analytical Chemistry, 2020, Vol. 16, No. 7 Shamari et al.

Table 1. Tuning/ source and analyzer condition for determi-nation of Tartrazine.

S. No. Parameter Values

01. Capillary voltage (kV) 3.0

02. Cone voltage (v) 16

03. Extractor voltage (v) 1

04. RF lense (V) 0.0

05. Source temperature (°C) 120

06. Desolvation temperature (°C) 250

07. Desolvation gas flow (L/h) 500

08. Cone gas flow (L/h) 50

09. LM resolution 1 15.0

10. HM resolution 1 15.0

11. Ion energy 0.6

12. Gain 1.0

2.7. Adsorbent Preparation and Solid-phase Extraction Process

Adsorbent for the solid-phase extraction of tartrazine was prepared to form the waste corncob, previously used for the adsorptive removal of the tartrazine [23]. Waste corncob was obtained from the local sweetcorn shop. The corncob was cut into small pieces and grounded using a domestically used grinder. The grounded corncob was sieved to collect uni-form-sized particles which passed through the 0.212 mm. Finally, the corncob was treated with hydrogen peroxide, washed thoroughly, dried and stored in a plastic container to be used as sorbent material in solid-phase extraction.

2.8. Solid-phase Extraction Set up and Extraction of the Real Samples

Corncob adsorbent, 0.1 g weight of which was taken in a 6 mL column where the sorbent was placed between the two coupling pieces. After the preparation of the column, it was washed using demineralized water and dried which makes the column ready for the extraction process. The prepared column was arranged in the Supelco vesiprepTM solid-phase extraction setup. Extraction of the real sample was checked by taking a suitable amount of degassed carbonated drinks whose pH was pre-adjusted to 2.0. After passing all the soft drinks, the column was washed at the same rate with milli Q generated water. Followed by the procedure for the extrac-tion of the adsorbed tartrazine, to get information on the best extraction, several solvents such as methanol, ethanol, ace-tonitrile and acetone were used, all of them failed to provide the enthusiastic result where there was little to no elution of the tartrazine. However, methanol with ammonia in the ratio (97:03) provided the best recovery of dyes from the adsor-bent. The eluted dye was dried, preconcentrated and was subjected to UPLC-MS analysis post-filtration and the same

was diluted when required considering the linear range of the target analyte, and final results were prepared considering the dilution factor.

3. RESULT AND DISCUSSION

3.1. Separation Conditions Optimization

Detection and accurate quantitation of any analyte re-quire the best experimental conditions to be chosen. For the selection of the best experimental conditions, all the experi-mental conditions need to be optimized to get the most sensi-tive chromatographic peaks as well as the detection of the precursor ion. The most accurate chromatographic analysis of any analyte is characterized by the highest sensitive peak obtained with good peak shape. To obtain such peaks for tartrazine, different mobile phases such as methanol-water, acetonitrile-water, acetonitrile- formic acid (of varied con-centration) and ammonium acetate- acetonitrile were tried taking both C8 and C18 column. The results of methanol-water and acetonitrile-water were enthusiastic with a C18 column. Later, based on the peak shape and area, acetonitrile and water combination were selected as mobile phases. However, still there is a chance of improvement in shape and sensitivity. To achieve this, combination of the acetonitrile and water was tried in different ratios. The equi-volume ratio of the two, resulted in broad peak shape which later turned good at each combination of increasing the organic solvent contribution. Finally, the best peak in terms of both the peak shape and sensitivity was achieved at acetonitrile: water (80:20).

The method development process of the tartrazine starts with the selection of the proper MS condition for the detec-tion of tartrazine. The method optimization process starts with the monitoring of the precursor ion of tartrazine. For this mass, charged ratio range of 0-575 was selected for monitoring precursor ion. In addition, the trail was also per-formed to select the ionization mode, where the positive ion-ization and negative ionization mode were applied alterna-tively to acquire the most abundant value of m/z. Although the intact molecular mass of the tartrazine is 534.36, yet us-ing the negative ionization mode, the 233 was precursor ions of the tartrazine, the same was reported for tartrazine deter-mination by UPLC-MS [17]. The further determination pro-cess was carried out using the same m/z. The full ion spectra of the tartrazine and possible breaking of the tartrazine mole-cule into possible daughter ions are mentioned in Fig. (1).

3.2. Preparation and Optimization of the Solid Phase Ex-traction (SPE) Conditions and Adsorbent Characteriza-tion

Waste corncob was selected as the extracting adsorbent. In the initial step, corncob was cut into small pieces and grounded. Three different adsorbent particle sizes were se-lected by passing them through different mesh sizes. All three particle-sized corncob adsorbents were washed, grounded and subjected to preliminary studies to check the adsorption capabilities of tartrazine. It was observed that the smallest mesh sized adsorbent has been the best adsorbent owing to its larger surface area. Depending upon the initial

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Page 4: in Carbonated Drinks and Analytical Method using Ultra ...

Corncob Waste Based Adsorbent for Solid Phase Extraction of Tartrazine Current Analytical Chemistry, 2020, Vol. 16, No. 7 927

Fig. (1). Full ion spectra of tartrazine using standard solution of 5 µgml-1. (A higher resolution/colour version of this figure is available in the electronic copy of the article).

adsorption trails, the adsorbent passing through the 0.212 mm mesh size was selected for the solid phase extraction studies. To check the appropriate amount of the adsorbent, different amount of adsorbent was tried in SPE and it was found that the adsorption efficiency increased with the in-crease in the amount of sorbent from 0.05 to 0.1 g proving the strong adsorption capabilities of the corncob solid-phase sorbent. The extraction time has a great role in the perfect extraction of tartrazine. It has been observed that extraction efficiency increased when the dye solution or the real sample solution remains in contact with the sorbent for a longer du-ration. For 3 mL of the dye, the extraction efficiency in-creased from 1 min to 4 min and the best recovery was ob-tained at 4 min and thereafter. Thus, 3 mL of the standard sample was made to pass through the SPE cartridge with a contact time of 5 min. The pre and post-extraction sorbent was subjected to SEM analysis (Fig. 2). The figure illustrates the morphological images of corncob sorbent pre (a) and post (b) tartrazine extraction. Fig. (2a) shows the heteroge-neous surface structure of corncob which was favorable for the elimination of tartrazine. Fig. (2b) illustrates the surface changes after the adsorption process which appeared to be more protuberances, which could be due to the coverage of surface with tartrazine molecule. SEM images indicated that the surface of tartarzine adsorbed corncob is rather heteroge-neous and denser than the surface of corncob. Variations in

surface morphology of adsorbents after adsorption could be attributed to the presence of tartrazine molecule in corncob.

The characterization of the prepared sorbent was also performed using the FTIR technique, and the spectra of sorbent before and after tartrazine adsorption is illustrated in Fig. (3). A peak at 3410 cm−1 corresponds to O-H stretching vibrations, indicating the presence of phenolic group due to cellulose and lignin content in the biomass. A peak at 2905 cm−1 illustrates C-H stretching, corresponds to the presence of aliphatic groups [24, 25]. A specific band at 1050 cm−1 was associated with C-O-C stretching vibration [26], while a peak around 600 cm−1 is the characteristics of C-H bending. After adsorption of tartrazine on corncob waste biomass shifting in spectral peak positions was noticed, these changes were ascribed to the electrostatic interactions between the positively charged functional groups of the sorbent (oxygen being protonated under acidic environments) and the nega-tively charged functionalities (SO3

-, COO-) of the anionic dye [27]. Additionally, there is a possibility that C-O-C sur-face functionalities of corncob biomass bind anionic dye through electrostatic interaction, as confirmed from the ap-pearance of a sharp peak with redshift from 1050 to 1060 cm-1. Also, a band at 1640 cm-1, possibly due to the interac-tion between negatively charged O2 of dye and the sp2-hybridized carbon atom (C=C) of the sorbent. Moreover, a new peak at 2380 cm-1, characteristic of C=O stretching

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928 Current Analytical Chemistry, 2020, Vol. 16, No. 7 Shamari et al.

Fig. (2). SEM image of the A) corncob sorbent prior to SPE B) Post SPE. (A higher resolution/colour version of this figure is available in the electronic copy of the article).

Fig. (3). Comparative FTIR spectra of corncob and tartrazine adsorbed onto corncob sorbent. (A higher resolution/colour version of this fig-ure is available in the electronic copy of the article).

vibration of a carbonyl or carboxyl groups appeared after tartrazine adsorption on corncob biomass.

3.3. Method Validation

Method validation is much-required study that should be performed intensively to make sure that the quantitative as-sessment of the target analyte, tartrazine, in this case, is ac-curate. Different parameters, as required by the regulatory authorities were studied to get the developed method validat-ed. The parameters include system suitability, linearity, spec-

ificity, accuracy and precision, the limit of detection and quantitation.

3.3.1. System Suitability

Prior to the start of the experiment, it is required to con-firm the proper functioning of the instruments and the opera-tional parameters. For this, six replicates of 2.0 mgL-1 stand-ard tartrazine, were injected and the peak area stability, re-tention time were established, both the peak area and the retention time were stable. The RSD of the peak area was

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Corncob Waste Based Adsorbent for Solid Phase Extraction of Tartrazine Current Analytical Chemistry, 2020, Vol. 16, No. 7 929

calculated and found to be 1.35% and that the retention time was found to be 1.54%.

3.3.2. Specificity

For the evaluation of the specificity, blank, standard and the dyes spiked into the blank were used. Six runs each of blank, standard and the tartrazine spiked into the blank were injected in the same sequence as mentioned. The retention time each of the standards and the spiked samples was rec-orded. No interferences or any other peaks were found at the retention time of the tartrazine. The standard chromatogram of tartrazine is mentioned in Fig. (4). Regarding the selectivi-ty of the adsorbent, other colorants such as methylene blue, malachite green and Rhodamine B were tried. At the work-ing pH of tartrazine, the recoveries of the above three color-ants were found to be insignificant for the determination studies. However, Allura red was found to adsorb considera-bly at lower pH.

3.3.3. Linearity and Range

To check the concentration range for accurate analysis, studies were conducted to check the range which obeys the beer’s law. Different tartrazine samples in the concentration range of 0.05 mg L-1 to 15 mg L-1 were subjected to analysis using the developed LC-MS method. The evaluation of the area with respect to the concentration revealed that the cur-rent method is linear and follows beer’s law in the range of 0.1 mgL-1 - 10 mgL-1. The statistical treatment of the data

produced intercept, slope and the correlation coefficient. From the resulting data, linear regression equation was de-rived to be A= 417.44+2698.4×C with a correlation coeffi-cient of 0.9994.

3.3.4. Accuracy and Precision

Accuracy and precision studies are equally important as the other validation parameters. Three-point precision studies were conducted where the results were evaluated on the basis of the RSD and % recovery for precision and accuracy, re-spectively. The studies were conducted at 1.3 mg L-1, 4.0 mg L-1 and 10.0 mg L-1. At the specified concentration points, the precision studies were conducted for one day and three consecutive days, the former being the intra-day precision and the latter is inter-day precision. The result of the studies at all the concentration points is mentioned in Table 2. The precision data was analyzed statistically and it was found that the mean recovery of the sample analyzed at three con-centration points was found to be in the range of 99.0-100.87 in intraday precision, which is the same as the interday preci-sion was found to be in the range of 98.54-101.28. The RSD for the same studies was found to be in the range of 0.076-1.30 for intraday precision and 1.34-1.83 for the interday precision. The standard analytical error was also calculated and found to be 0.04,0.017 and 0.05 for intraday assay and 0.007, 0.030 and 0.066 for intra day assay. The confidence limit at 95% confidence level and 5 degrees of freedom was found to be 0.008, 0.033 and 0.11 for intraday assay and 0.014, 0.061 and 0.0134 for interday precision.

Fig. (4). Standard chromatogram of tartrazine with respect to the most abundant m/z. (A higher resolution/colour version of this figure is available in the electronic copy of the article).

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930 Current Analytical Chemistry, 2020, Vol. 16, No. 7 Shamari et al.

Table 2. Accuracy and the precision studies for the determination of Tartrazine.

Proposed Procedure Amount of Tartrazine (mgL-1) Recovery

Taken Found ± RSD(%)a (%)

Intra-day

Precision

1.3 1.287 ± 0.76 99.0

4.0 4.008 ± 1.01 100.20

- 10.0 10.087 ± 1.30 100.87

Inter-day

Precision

1.3 1.281± 1.34 98.54

4.0 4.051± 1.83 101.28

10.0 10.06 ± 1.62 100.60 a Mean± RSD for six determination.

Table 3. Standard addition method to check the recovery of tartrazine through the developed method.

Amount Added

(mg L-1)

Amount Recovered

(mg L-1)

RSD

(%)

Recovery

(%)

0.1 0.0978 4.86 97.78

2.0 1.965 1.83 98.30

7.5 7.35 2.99 98.13

10 9.84 4.4 98.40

Table 4. Amount of tartrazine present in the real soft drink samples, determine by the developed method.

Sample Number Concentration Found RSD

01 20.39 1.74

02 25.92 2.03

03 37.67 1.89

04 83.26 1.56

3.3.5. Limits of Detection and Quantitation

The standard tartrazine sample was used for the assess-ment of the limit of detection and quantitation, which repre-sents a minimum concentration that gives S/N of 3 for LOD and 10 for LOQ. The results of six replicate analyses of low concentration tartrazine samples show that the LOD and LOQ of the developed method were found to be 0.0165 mg L-1 and 0.055 mg L-1.

3.4. Recovery of Tartrazine

Tartrazine recovery studies were performed by spiking the known amount of tartrazine into the colorless carbonated drink and extracting the dye through the recommended pro-cedure. In the current analysis 0.1, 2, 7.5 and 10 (mg L-1), tartrazine drink solution was prepared by spiking tartrazine in the carbonated colorless drink. Recovery studies were performed using the recommended procedure. The recovery studies of the four spiked solutions were performed via solid-

phase extraction prior to the chromatographic analysis and the recovery was found in the range of 97.78% to 98.40%. The results of the standard addition studies are mentioned in Table 3.

3.5. Application of the Developed Method

The developed method was applied to the determination of the dye tartrazine in soft drinks. The drinks considered in this study were carbonated drinks. Table 4 summarizes the results of the tartrazine found in different samples where the dye was found in the range of 20.39 mgL-1 - 83.26 mgL-1.

CONCLUSION

In this study, we have developed a new method for the determination of tartrazine, a food dye in carbonated bever-ages. The complete study involves two steps; first step in-volves the method development phase for the determination of dyes and the second step involves the solid-phase extrac-

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Page 8: in Carbonated Drinks and Analytical Method using Ultra ...

Corncob Waste Based Adsorbent for Solid Phase Extraction of Tartrazine Current Analytical Chemistry, 2020, Vol. 16, No. 7 931

tion process prior to the application stage. The developed method was found to be linear in the range of 0.1 mgL-1 to 10 mgL-1. The LOD and LOQ of the developed method were found to be 0.0165 mgL-1 and 0.055 mgL-1, respectively. Tartrazine found in the carbonated drinks were in the range of 20.39 mgL-1 - 83.26 mgL-1. The solid-phase extraction step involves the use of waste corncob as sorbent while the dye was eluted after adsorption with basic methanol.

ETHICS APPROVAL AND CONSENT TO PARTICI-PATE

Not applicable.

HUMAN AND ANIMAL RIGHTS

No animals/humans were used for studies that are base of this research.

CONSENT FOR PUBLICATION

Not applicable.

AVAILABILITY OF DATA AND MATERIALS

The authors confirm that the data supporting the findings of this study are available within the article.

FUNDING

The authors would like to extend their sincere apprecia-tion to the Deanship of Scientific Research at King Saud University for funding this work through Research Group No. RG-1437-031.

CONFLICT OF INTEREST

The authors declare no conflict of interest, financial or otherwise.

ACKNOWLEDGEMENTS

Declared none.

REFERENCES [1] Moutinho, I.L.D.; Bertges, L.C.; Assis, R.V.C. Prolonged use of

the food dye tartrazine (FD&C yellow no 5) and its effects on the gastric mucosa of Wistar rats. Braz. J. Biol., 2007, 67(1), 141-145.

http://dx.doi.org/10.1590/S1519-69842007000100019 PMID: 17505761

[2] de Andrade, F.I.; Florindo Guedes, M.I.; Pinto Vieira, Í.G.; Pereira Mendes, F.N.; Salmito Rodrigues, P.A.; Costa Maia, C.S.; Marques Ávila, M.M.; de Matos Ribeiro, L. Determination of synthetic food dyes in commercial soft drinks by TLC and ion-pair HPLC. Food Chem., 2014, 157, 193-198.

http://dx.doi.org/10.1016/j.foodchem.2014.01.100 PMID: 24679770

[3] http://www.ukfoodguide.net/e102.htm [4] Abu Shawish, H.M.; Ghalwa, N.A.; Saadeh, S.M.; El Harazeen, H.

Development of novel potentiometric sensors for determination of tartrazine dye concentration in foodstuff products. Food Chem., 2013, 138(1), 126-132.

http://dx.doi.org/10.1016/j.foodchem.2012.10.048 PMID: 23265466

[5] Shawish, H.M.A.; Ghalwa, N.A.; El Harazeen, H. Assay of tartra-zine dye concentration in foodstuff products by new potentiometric carbon paste electrode. Sens. Lett., 2012, 10, 894-901.

http://dx.doi.org/10.1166/sl.2012.2600 [6] Lipskikh, O.I.; Nikolaeva, A.A.; Korotkova, E.I. Voltammetric

determination of Tartrazine in food. J. Anal. Chem., 2017, 72(4), 396-401.

http://dx.doi.org/10.1134/S1061934817040062 [7] Song, Y.Z.; Xu, J.M.; Lv, J.S.; Zhong, H.; Ye, Y.; Xie, J.M. Elec-

trochemical reduction of tartrazine at multi-walled carbon nano-tube-modified pyrolytic graphite electrode. Indian J. Chem., 2010, 49A(8), 1030-1034.

[8] Ghoreishi, S.M.; Behpour, M.; Golestaneh, M. Simultaneous volt-ammetric determination of Brilliant Blue and Tartrazine in real samples at the surface of a multi-walled carbon nanotube paste electrode Anal. Met., 2011, 3, 2842-2847.

http://dx.doi.org/10.1039/c1ay05327b [9] Ghoreishi, S.M.; Behpour, M.; Golestaneh, M. Selective voltam-

metric determination of tartrazine in the presence of red 10B by nanogold‐modified carbon paste electrode. J. Chin. Chem. Soc. (Taipei), 2013, 60(1), 120-126.

http://dx.doi.org/10.1002/jccs.201200143 [10] Perdomo, Y.; Arancibia, V.; García-Beltrán, O.; Nagles, E. Adsorp-

tive stripping voltammetric determination of amaranth and tartra-zine in drinks and gelatins using a screen-printed carbon electrode. Sensors (Basel), 2017, 17(11), 2665.

http://dx.doi.org/10.3390/s17112665 PMID: 29156561 [11] Karim-Nezhad, G.; Khorablou, Z.; Zamani, M.; Seyed Dorraji, P.;

Alamgholiloo, M. Voltammetric sensor for tartrazine determination in soft drinks using poly (p-aminobenzenesulfonic acid)/zinc oxide nanoparticles in carbon paste electrode. Yao Wu Shi Pin Fen Xi, 2017, 25(2), 293-301.

http://dx.doi.org/10.1016/j.jfda.2016.10.002 PMID: 28911670 [12] Nevado, J.J.B.; Floresa, J.R.; Llerena, M.J.V. Simultaneous spec-

trophotometric determination of Tartrazine, Sunset Yellow and Ponceau 4R in commercial products by partial least squares and principal component regression multivariate calibration methods. Fresenius J. Anal. Chem., 1998, 361(5), 465-472.

http://dx.doi.org/10.1007/s002160050927 [13] Nevado, J.J.B.; Flores, J.R.; Llerena, M.J.V.; Fariñas, N.R. Simul-

taneous spectrophotometric determination of tartrazine, patent blue V, and indigo carmine in commercial products by partial least squares and principal component regression methods. Talanta, 1999, 48(4), 895-903.

http://dx.doi.org/10.1016/S0039-9140(98)00301-4 PMID: 18967532

[14] Antakli, S.; Nejem, L.; Katran, S. Simultaneous determination of tartrazine and brilliant blue in foodstuffs by spectrophotometric method. Int. J. Pharm. Pharm. Sci., 2015, 7(6), 214-218.

[15] Sha, O.; Zhu, X.; Feng, Y.; Ma, W. Determination of sunset yellow and tartrazine in food samples by combining ionic liquid-based aqueous two-phase system with high performance liquid chroma-tography. J Anal. Met. Chem., 2014, 2014, Article ID 964273.

http://dx.doi.org/10.1155/2014/964273 [16] Vlase, L.; Muntean, D.; Cobzac, S.C.; Filip, L. Development and

validation of an HPLC-UV method for determination of synthetic food colorants. Rev. Roum. Chim., 2014, 59(9), 719-725.

[17] Gao, H-G.; Gong, W-J.; Zhao, Y-G. Rapid method for quantifica-tion of seven synthetic pigments in colored Chinese steamed buns using UFLC-MS/MS without SPE. Anal. Sci., 2015, 31(3), 205-210.

http://dx.doi.org/10.2116/analsci.31.205 PMID: 25765275 [18] Nagappan, K.; Yamjala, K.; Sathyaseelan, M.; Byran, G. Stability

evaluation of tartrazine by liquid chromatography-diode array de-tector and high-resolution electron spray ionization quadrupole time-offlight mass spectrometry/mass spectrometry analysis Asian J. Pharm. Clin. Res., 2017, 10(7), 295-299.

http://dx.doi.org/10.22159/ajpcr.2017.v10i7.17191 [19] Ates, E.; Mittendorf, K.; Senyuva, H. LC/MS method using cloud

point extraction for the determination of permitted and illegal food colors in liquid, semiliquid, and solid food matrixes: single-laboratory validation. J. AOAC Int., 2011, 94(6), 1853-1862.

http://dx.doi.org/10.5740/jaoacint.11-220 PMID: 22320093

For pe

rsona

l priv

ate us

e only

.

Not be

distr

ibuted

or up

loade

d to a

nyon

e or a

nywhe

re.

Page 9: in Carbonated Drinks and Analytical Method using Ultra ...

932 Current Analytical Chemistry, 2020, Vol. 16, No. 7 Shamari et al.

[20] Chen, B.; Wang, W.; Huang, Y. Cigarette filters as adsorbents of solid-phase extraction for determination of fluoroquinolone antibi-otics in environmental water samples coupled with high-performance liquid chromatography. Talanta, 2012, 88, 237-243.

http://dx.doi.org/10.1016/j.talanta.2011.09.066 PMID: 22265493 [21] Chen, B.; Wang, S.; Zhang, Q.; Huang, Y. Highly stable magnetic

multiwalled carbon nanotube composites for solid-phase extraction of linear alkylbenzene sulfonates in environmental water samples prior to high-performance liquid chromatography analysis. Analyst (Lond.), 2012, 137(5), 1232-1240.

http://dx.doi.org/10.1039/c2an16030g PMID: 22262090 [22] Wang, W.; Chen, B.; Huang, Y. Eggshell membrane-based biotem-

plating of mixed hemimicelle/admicelle as a solid-phase extraction adsorbent for carcinogenic polycyclic aromatic hydrocarbons. J. Agric. Food Chem., 2014, 62(32), 8051-8059.

http://dx.doi.org/10.1021/jf501877k PMID: 25025712 [23] Jiménez, S.; Velásquez, C.; Mejía, F.; Hormaza, A. Proceedings of

the international conference of recent trends in environmental sci-

ence and engineering (RTESE'17). Toronto, Canada Paper No. 141, 2017.

http://dx.doi.org/10.11159/rtese17.141. [24] Farnane, M.; Tounsadi, H.; Machrouhi, A.; Elhalil, A.; Mahjoubi,

F.Z.; Sadiq, M.; Abdennouri, M.; Qourzal, S.; Barka, N. Dye re-moval by raw maize corncob and H3PO4 activated maize corncob. J. Water Reuse Desal., 2017, 8(2), 214-224.

[25] Aljeboree, A.M.; Alkaim, A.F. Comparative removal of three tex-tile dyes from aqueous solutions byadsorption: As a model (corn-cob source waste) of plants role in environmental enhancement. Plant Arch., 2019, 19(1), 1613-1620.

[26] Foo, K.Y.; Hameed, B.H. Preparation and characterizationof acti-vated carbon from pistachio nut shells via microwave-induced chemical activation. Biomass Bioener., 2011, 35(7), 3257-3326.

http://dx.doi.org/10.1016/j.biombioe.2011.04.023 [27] Suteu, D.; Malutan, T.; Bilba, D. Agricultural waste corn cob as a

sorbent for removing reactive dye orange 16: equilibrium and ki-netic study cellulose. Chem. Technol., 2011, 45(5-6), 413-420.

For pe

rsona

l priv

ate us

e only

.

Not be

distr

ibuted

or up

loade

d to a

nyon

e or a

nywhe

re.


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