Institute of Inorganic and Analytical Chemistry, Justus Liebig University Giessen , 35392 Giessen, Germany.
Anal Chem. 2017 Oct 17;89(20):10717-10725. doi: 10.1021/acs.analchem.7b01689. Epub 2017 Sep 25.
Food adulteration is a threat to public health and the economy. In order to determine food adulteration efficiently, rapid and easy-to-use on-site analytical methods are needed. In this study, a miniaturized mass spectrometer in combination with three ambient ionization methods was used for food authentication. The chemical fingerprints of three milk types, five fish species, and two coffee types were measured using electrospray ionization, desorption electrospray ionization, and low temperature plasma ionization. Minimum sample preparation was needed for the analysis of liquid and solid food samples. Mass spectrometric data was processed using the laboratory-built software MS food classifier, which allows for the definition of specific food profiles from reference data sets using multivariate statistical methods and the subsequent classification of unknown data. Applicability of the obtained mass spectrometric fingerprints for food authentication was evaluated using different data processing methods, leave-10%-out cross-validation, and real-time classification of new data. Classification accuracy of 100% was achieved for the differentiation of milk types and fish species, and a classification accuracy of 96.4% was achieved for coffee types in cross-validation experiments. Measurement of two milk mixtures yielded correct classification of >94%. For real-time classification, the accuracies were comparable. Functionality of the software program and its performance is described. Processing time for a reference data set and a newly acquired spectrum was found to be 12 s and 2 s, respectively. These proof-of-principle experiments show that the combination of a miniaturized mass spectrometer, ambient ionization, and statistical analysis is suitable for on-site real-time food authentication.
食品掺假对公众健康和经济构成威胁。为了有效地确定食品掺假,需要快速、易用的现场分析方法。在这项研究中,使用微型质谱仪结合三种大气离子化方法对食品进行了鉴定。使用电喷雾电离、解吸电喷雾电离和低温等离子体电离法测量了三种牛奶类型、五种鱼类和两种咖啡类型的化学指纹图谱。对液体和固体食品样本的分析需要最小的样品制备。使用实验室自制的软件 MS food classifier 处理质谱数据,该软件允许使用多元统计方法从参考数据集定义特定的食品图谱,并随后对未知数据进行分类。通过使用不同的数据处理方法、10%留一交叉验证和实时分类新数据来评估获得的质谱指纹图谱在食品鉴定中的适用性。在交叉验证实验中,牛奶类型和鱼类的区分达到了 100%的分类准确率,咖啡类型的分类准确率达到了 96.4%。两种牛奶混合物的测量结果也得到了正确的分类,准确率超过 94%。对于实时分类,准确率相当。描述了软件程序的功能及其性能。发现参考数据集和新获取的光谱的处理时间分别为 12 秒和 2 秒。这些原理验证实验表明,微型质谱仪、大气离子化和统计分析的组合适用于现场实时食品鉴定。