No abstract

The development of analytical strategies to fight against food fraud is currently one of the most developing fields in food science as the food value chain becomes increasingly complex and global. Food can be certified by clear labeling but also by objective analytical methods. As shown recently by several groups, the omics technologies such as genomics, proteomics, metabolomics, and isotopolomics are suitable to prove the geographical origin, the production or cultivation process, and the biological and the overall chemical identity of food. This article describes different analytical approaches beginning with non-targeted strategies as well as the further developmental stages of transferring the methods to routine laboratories.

For the first time, a non-targeted metabolomics approach by means of ultraperformance liquid chromatography coupled to electrospray quadruple time-of-flight mass spectrometry was chosen for the discrimination of geographical origins of white asparagus samples (Asparagus officinalis). Over a period of four harvesting periods (4 years), approximately 400 asparagus samples were measured. Initially, four different liquid chromatography–mass spectrometry methods were used to detect as many metabolites as possible and to assess which method is most suitable. The most relevant marker compounds were linked to the influence of different plant stress parameters and climate effects. Some of the samples were also analyzed by isotope-ratio mass spectrometry (IRMS), which is the current gold standard for the discrimination of the geographical origin of asparagus. In summary, the analysis of the metabolome was proven to be quite suitable to determine the geographical origin of asparagus and seems to provide better interpretable results than IRMS studies.

Nontargeted screening methods with ultrahigh-performance liquid chromatography-electrospray ionization/quadrupole-time-of-flight mass spectrometry have been extensively applied to plant metabolomics to very diverse scientific issues in plant metabolomics. In this study, different mobile phase additives were tested in order to improve the electrospray ionization process and to detect as many metabolites as possible with high peak intensities in positive and negative ionization mode. Influences of modifiers were examined for nonpolar and polar compounds, as optimal conditions are not always the same. By combining different additives, metabolite coverage could be significantly increased. The best results for polar metabolites in positive ionization mode were achieved by using 0.1% acetic acid and 0.1% formic acid in negative ionization mode. For measurements of nonpolar metabolites in positive ionization mode, the application of 10 mmol/L ammonium formate led to the best findings, while the use of 0.02% acetic acid was more appropriate in negative ionization mode.

In times of increasing globalization and the resulting complexity of trade flows, securing food quality is an increasing challenge. The development of analytical methods for checking the integrity and, thus, the safety of food is one of the central questions for actors from science, politics, and industry. Targeted methods, for the detection of a few selected analytes, still play the most important role in routine analysis. In the past 5 years, nontargeted methods that do not aim at individual analytes but on analyte profiles that are as comprehensive as possible have increasingly come into focus. Instead of investigating individual chemical structures, data patterns are collected, evaluated and, depending on the problem, fed into databases that can be used for further nontargeted approaches. Alternatively, individual markers can be extracted and transferred to targeted methods. Such an approach requires (i) the availability of authentic reference material, (ii) the corresponding highresolution laboratory infrastructure, and (iii) extensive expertise in processing and storing very large amounts of data. Probably due to the requirements mentioned above, only a few methods have really established themselves in routine analysis. This review article focuses on the establishment of nontargeted methods in routine laboratories. Challenges are summarized and possible solutions are presented.