Estimation of daily aluminum intake in Japan based on food consumption inspection results: impact of food additives.

Dietary aluminum (Al) intake by young children, children, youths, and adults in Japan was estimated using the market basket method. The Al content of food category (I-VII) samples for each age group was determined by inductively coupled plasma-atomic emission spectrometry (ICP-AES). The Al content in processed foods and unprocessed foods ranged from 0.40 to 21.7 mg/kg and from 0.32 to 0.54 mg/kg, respectively. For processed foods in all age groups, the Al content in food category VI samples, sugar and confections/savories, was the highest, followed by those in category II, cereals. The daily dietary Al intake from processed foods was much larger than that from unprocessed foods. The mean weekly percentages of the provisional tolerable weekly intake (PTWI, established by the joint FAO/WHO Expert Committee on Food Additives in 2011) from processed foods for all age groups are 43.1, 22.4, 17.6 and 15.1%, respectively. Only the highest consumer Al exposure value (>P 95) of the young children group exceeded the PTWI.

[Development of identification method for isopropyl citrate].

In Japan's Specification and Standards for Food Additive, 8th edition, two identification tests involving isopropyl citrate for detecting isopropyl alcohol and citrate are stipulated. However, these identification tests use mercury compound, which is toxic, or require a time-consuming pretreatment process. To solve these problems, an identification test method using GC-FID for detecting isopropyl alcohol was developed. In this test, a good linearity was observed in the range of 0.1-40 mg/mL of isopropyl alcohol. While investigating the pretreatment process, we found that isopropyl alcohol could be detected using GC-FID in the distillation step only, without involving any reflux step. The study also showed that the citrate moiety of isopropyl citrate was identified using the solution remaining after conducting the distillation of isopropyl alcohol. The developed identification tests for isopropyl citrate are simple and use no toxic materials.

Absolute quantification of dehydroacetic acid in processed foods using quantitative ¹H NMR.

An absolute quantification method for the determination of dehydroacetic acid in processed foods using quantitative (1)H NMR was developed and validated. The level of dehydroacetic acid was determined using the proton signals of dehydroacetic acid referenced to 1,4-bis (trimethylsilyl) benzene-d4 after simple solvent extraction from processed foods. All the recoveries from three processed foods spiked at two different concentrations were larger than 85%. The proposed method also proved to be precise, with inter-day precision and excellent linearity. The limit of quantification was confirmed as 0.13g/kg in processed foods, which is sufficiently low for the purposes of monitoring dehydroacetic acid. Furthermore, the method is rapid and easy to apply, and provides International System of Units traceability without the need for authentic analyte reference materials. Therefore, the proposed method is a useful and practical tool for determining the level of dehydroacetic acid in processed foods.

[Improved methodology for quantitative determination of thiabendazole].

The method prescribed in the 8th edition of Japan's Specifications and Standards for Food Additives (JSSFA) for the quantitative analysis of thiabendazole was improved by eliminating the use of toxic reagents such as mercuric acetate and chromium trioxide. For exclusion of mercuric acetate, a nonaqueous titration was performed using four types of solvent systems, including acetic acid:acetic anhydride (1:5), acetic acid:acetic anhydride (3:7), acetic acid alone, and formic acid:acetic acid (1:10), that did not contain mercuric compounds. Because precipitates were formed in titrations using acetic acid alone and formic acid:acetic acid (1:10), we considered that it was difficult to determine the purity using these solvent systems. However, it was confirmed that the purity of thiabendazole dissolved in the two acetic acid:acetic anhydride solvent systems can be determined using either a visual indicator or potentiometry. Specifically, the purity of thiabendazole was determined to be 99.9% (relative standard deviation (RSD) = 0.07%) for acetic acid:acetic anhydride (1:5) and 99.7% (RSD = 0.13%) for acetic acid:acetic anhydride (3:7) With respect to chromium trioxide, it was determined that chromium trioxide can be excluded using acetic acid, which conforms to the JIS K8001 standard for nonaqueous titrations. Therefore, in this study, an improved method for the quantitative determination of thiabendazole was developed without the use of toxic reagents.

[Study of purity tests for silicone resins].

In the 8th edition of Japan's Specifications and Standards for Food Additives, the purity test for silicone resins requires the determination of the refractive index and kinetic viscosity of the extracted silicone oil, and allows for only a limited amount of silicon dioxide. In the purity test, carbon tetrachloride is used to separate the silicone oil and silicon dioxide. To exclude carbon tetrachloride, methods were developed for separating the silicone oil and silicon dioxide from silicone resin, which use hexane and 10% n-dodecylbenzenesulfonic acid in hexane. For silicone oil, the measured refractive index and kinetic viscosity of the silicone oil obtained from the hexane extract were shown to be equivalent to those of the intact silicone oil. In regard to silicon dioxide, it was confirmed that, following the separation with 10% n-dodecylbenzenesulfonic acid in hexane, the level of silicon dioxide in silicone resin can be accurately determined. Therefore, in this study, we developed a method for testing the purity of silicone resins without the use of carbon tetrachloride, which is a harmful reagent.

[Analytical method for natamycin in wine using high-performance liquid chromatography].

An analytical method was developed for determining amount of natamycin in wine using a C18 minicartridge column and high-performance liquid chromatography (HPLC) with photodiode array (PDA) detection. Natamycin purified from wine was identified in accordance with the retention time and UV spectrum obtained from PDA detection. The limit of quantification of natamycin in wine was estimated as 0.05 microg/ml. Recovery of natamycin in wine was acceptable at 91.0% with low relative standard deviation (2.3%).

[Analysis of hexachlorobenzene in Food Red Nos. 104 (phloxine) and 105 (rose Bengal) by GC-ECD].

A simple and rapid method using electron capture detector gas chromatography (GC-ECD) was developed for the determination of hexachlorobenzene (HCB) in Food Red Nos. 104 and 105. The sample was dissolved in water and HCB was extracted with hexane. The GC-ECD operating conditions were as follows: column, InertCap 5 MS/NP (30 m x 0.25 mm i. d. with 0.25 microm film thickness); oven temperature, 60 degrees C(1 min)-->20 degrees C/min-->150 degrees C(10 min)-->20 degrees C/min-->280 degrees C(5 min); inlet temperature, 260 degrees C; detector temperature, 300 degrees C; carrier gas, nitrogen (constant press 25 psi); inlet mode, splitless. For the evaluation of the method, HCB spiked into R104 and R105 at the levels of 2 microg/g and 5 microg/g was determined in replicate in five laboratories. Mean recoveries of HCB from R104 and R105 were 98.2-103.7%. Repeatability relative standard deviation values were 2.9-6.0% and reproducibility relative standard deviation values were 4.2-9.3%. HORRAT value was less than one. From these results, the validity of this method was confirmed.

Quantitative nuclear magnetic resonance spectroscopic determination of the oxyethylene group content of polysorbates.

Guidelines for the oxyethylene group (EO) content of polysorbates are set by the Food and Agriculture Organization/World Health Organization Joint Expert Committee on Food Additives. However, the classical titration method for EO determination is difficult and time-consuming. Here, we show that quantitative (1)H-nuclear magnetic resonance spectroscopy can determine the EO contents of polysorbates rapidly and simply. The EO signals were identified through comparisons with sorbitan monolaurate and poly(ethylene glycol) distearate. Potassium hydrogen phthalate was used as an internal standard. The EO contents were estimated from the ratio of the signal intensities of EO to the internal standard. Two nuclear magnetic resonance systems were used to validate the proposed method. The EO content of commercial polysorbates 20, 60, 65, and 80 was determined to be within the recommended limits using this technique. Our approach thus represents an additional or alternative method of determining the EO contents of polysorbates.

Application of liquid chromatography-nuclear magnetic resonance spectroscopy for the identification of ethyldimethylpyrazine, a food flavouring agent.

The application of liquid chromatography-nuclear magnetic resonance spectroscopy (LC-NMR) for the direct identification of ethyldimethylpyrazine, a food flavouring agent, has been studied. The commercial product is a mixture of two regio-isomers, 2-ethyl-3,5-dimethylpyrazine (1) and 2-ethyl-3,6-dimethylpyrazine (2); however, the exact composition of the mixture is unknown. Structural characterization by LC-MS and GC-MS was not possible because both regio-isomers yield the same molecular related ion and ion fragmentation. To rapidly identify the two regio-isomers, the product was analyzed by LC-NMR with on-flow and fraction loop modes. From the results, the structure elucidations of the two regio-isomers could be carried out without the need to isolate the isomers by the usual procedures.