An Automated Methodology for Non-targeted Compositional Analysis of Small Molecules in High Complexity Environmental Matrices Using Coupled Ultra Performance Liquid Chromatography Orbitrap Mass Spectrometry (original) (raw)
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Journal of Chromatography A, 2009
The European Reach legislation will possibly drive producers to develop newly designed chemicals that will be less persistent, bioaccumulative or toxic. If this innovation leads to an increased use of more hydrophilic chemicals it may result in higher mobilities of chemicals in the aqueous environment. As a result, the drinking water companies may face stronger demands on removal processes as the hydrophilic compounds inherently are more difficult to remove. Monitoring efforts will also experience a shift in focus to more water-soluble compounds. Screening source waters on the presence of (emerging) contaminants is an essential step in the control of the water cycle from source to tap water. In this article, some of our experiences are presented with the hybrid linear ion trap (LTQ) FT Orbitrap mass spectrometer, in the area of chemical water analysis. A two-pronged strategy in mass spectrometric research was employed: (i) exploring effluent, surface, ground-and drinking-water samples searching for accurate masses corresponding to target compounds (and their product ions) known from, e.g. priority lists or the scientific literature and (ii) full-scan screening of water samples in search of 'unknown' or unexpected masses, followed by MS n experiments to elucidate the structure of the unknowns. Applications of both approaches to emerging water contaminants are presented and discussed. Results are presented for target analysis search for pharmaceuticals, benzotriazoles, illicit drugs and for the identification of unknown compounds in a groundwater sample and in a polar extract of a landfill soil sample (a toxicity identification evaluation bioassay sample). The applications of accurate mass screening and identification described in this article demonstrate that the LC-LTQ FT Orbitrap MS is well equipped to meet the challenges posed by newly emerging polar contaminants.
Scientific Data, 2021
Non-target analysis (NTA) employing high-resolution mass spectrometry is a commonly applied approach for the detection of novel chemicals of emerging concern in complex environmental samples. NTA typically results in large and information-rich datasets that require computer aided (ideally automated) strategies for their processing and interpretation. Such strategies do however raise the challenge of reproducibility between and within different processing workflows. An effective strategy to mitigate such problems is the implementation of inter-laboratory studies (ILS) with the aim to evaluate different workflows and agree on harmonized/standardized quality control procedures. Here we present the data generated during such an ILS. This study was organized through the Norman Network and included 21 participants from 11 countries. A set of samples based on the passive sampling of drinking water pre and post treatment was shipped to all the participating laboratories for analysis, using ...
Environmental Mass Spectrometry
Analytical Chemistry, 2000
Environmental mass spectrometry is an important branch of science because it provides many of the data that underlie policy decisions that can directly influence the health of people and ecosystems. Environmental mass spectrometry is currently undergoing rapid development. Among the most relevant directions are a significant broadening of the lists of formally targeted compounds; a parallel interest in nontarget chemicals; an increase in the reliability of analyses involving accurate mass measurements, tandem mass spectrometry, and isotopically labeled standards; and a shift toward faster high-throughput analysis, with minimal sample preparation, involving various approaches, including ambient ionization techniques and miniature instruments. A real revolution in analytical chemistry could be triggered with the appearance of robust, simple, and sensitive portable mass spectrometers that can utilize ambient ionization techniques. If the cost of such instruments is reduced to a reasonable level, mass spectrometers could become valuable household devices.
Analytical and bioanalytical chemistry, 2015
In this article, a dataset from a collaborative non-target screening trial organised by the NORMAN Association is used to review the state-of-the-art and discuss future perspectives of non-target screening using high-resolution mass spectrometry in water analysis. A total of 18 institutes from 12 European countries analysed an extract of the same water sample collected from the River Danube with either one or both of liquid and gas chromatography coupled with mass spectrometry detection. This article focuses mainly on the use of high resolution screening techniques with target, suspect, and non-target workflows to identify substances in environmental samples. Specific examples are given to emphasise major challenges including isobaric and co-eluting substances, dependence on target and suspect lists, formula assignment, the use of retention information, and the confidence of identification. Approaches and methods applicable to unit resolution data are also discussed. Although most s...
The benefits of high resolution mass spectrometry in environmental analysis
The Analyst, 2013
The benefits of high resolution mass spectrometry (HRMS) are well known and widely realized in various applications; however, HRMS is very rarely utilized in environmental GC/MS analyses. It is assumed that low resolution GC/MS provides adequate and reliable results in the majority of cases dealing with priority pollutants and other volatile and semivolatile compounds. As environmental issues become more and more important in modern society and new generations of high resolution and high mass accuracy mass spectrometers become available, it is quite reasonable to expect improvements in sensitivity, reliability and quantity of information provided by GC/MS analyses. This article demonstrates the advantages of high resolution GC/MS for qualitative and quantitative environmental analyses including targeted and non-targeted approaches as well as de novo structural elucidation of analytes not present in commercial libraries. Most of the examples presented here involve the GC/MS analysis of snow samples collected in 2012 and 2013 in Moscow, Russia.
Challenges and achievements of LC-MS in environmental analysis: 25 years on
TrAC Trends in Analytical Chemistry, 2007
In this overview article celebrating the 25th anniversary of TrAC, we will discuss the progress of liquid chromatography-mass spectrometry (LC-MS) and LC-tandem MS (LC-MS 2) in environmental analysis. The article will cover challenges and achievements of LC-MS in environmental analysis with emphasis on the developments that occurred over 20 years and the impact caused by the discovery of electrospray and its applications to organic trace analysis. We will also outline the history of TrAC in relation to the publication of papers dealing with LC-MS applied to environmental analysis. The second part of the article will be devoted to LC-MS 2 as the preferred method of choice in environmental analysis. We will report on applications on the use of triple quadupoles and hybrid technologies (e.g., Qq-LIT. Qq-TOF and Orbitrap) for a variety of the so-called emerging contaminants (e.g., pharmaceuticals, pesticides and endocrine disruptors).
Environmental Sciences Europe, 2019
Non-target screening (NTS) including suspect screening with high resolution mass spectrometry has already shown its feasibility in detecting and identifying emerging contaminants, which subsequently triggered exposure mitigating measures. NTS has a large potential for tasks such as effective evaluation of regulations for safe marketing of substances and products, prioritization of substances for monitoring programmes and assessment of environmental quality. To achieve this, a further development of NTS methodology is required, including: (i) harmonized protocols and quality requirements, (ii) infrastructures for efficient data management, data evaluation and data sharing and (iii) sufficient resources and appropriately trained personnel in the research and regulatory communities in Europe. Recommendations for achieving these three requirements are outlined in the following discussion paper. In particular, in order to facilitate compound identification it is recommended that the relevant information for interpretation of mass spectra, as well as about the compounds usage and production tonnages, should be made accessible to the scientific community (via open-access databases). For many purposes, NTS should be implemented in combination with effectbased methods to focus on toxic chemicals.
2018
38 A key challenge in the environmental and exposure sciences is to establish experimental evidence of the 39 role of chemical exposure in human and environmental systems. High resolution and accurate tandem 40 mass spectrometry (HRMS) is increasingly being used for the analysis of environmental samples. One 41 lauded benefit of HRMS is the possibility to retrospectively process data for (previously omitted) 42 compounds that has led to the archiving of HRMS data. Archived HRMS data affords the possibility of 43 exploiting historical data to rapidly and effectively establish the temporal and spatial occurrence of 44 newly identified contaminants through retrospective suspect screening. We propose to establish a 45 global emerging contaminant early warning network to rapidly assess the spatial and temporal 46 distribution of contaminants of emerging concern in environmental samples through performing 47 retrospective analysis on HRMS data. The effectiveness of such a network is demon...
Communications Earth & Environment, 2022
Fine particulate-matter is an important component of air pollution that impacts health and climate, and which delivers anthropogenic contaminants to remote global regions. The complex composition of organic molecules in atmospheric particulates is poorly constrained, but has important implications for understanding pollutant sources, climate-aerosol interactions, and health risks of air pollution exposure. Here, comprehensive nontarget high-resolution mass spectrometry was combined with in silico structural prediction to achieve greater molecular-level insight for fine particulate samples (n = 40) collected at a remote receptor site in the Maldives during January to April 2018. Spectral database matching identified 0.5% of 60,030 molecular features observed, while a conservative computational workflow enabled structural annotation of 17% of organic structures among the remaining molecular dark matter. Compared to clean air from the southern Indian Ocean, molecular structures from hi...