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Online HPLC-ESI-HRMS Method for the Analysis and Comparison of Different Dissolved Organic Matter Samples
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.ORCID iD: 0000-0002-4301-3923
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.ORCID iD: 0000-0002-4597-041x
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Biology, Department of Ecology and Genetics, Limnology.ORCID iD: 0000-0003-3509-8266
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2018 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 52, no 4, p. 2091-2099Article in journal (Refereed) Published
Abstract [en]

Natural dissolved organic matter (DOM) is an ultracomplex mixture that is essential to global carbon cycling but is poorly understood because of its complexity. The most powerful tool for the DOM characterization is high-resolution mass spectrometry (HRMS) generally combined to direct infusion (DI) as sample introduction. Liquid chromatography (LC) represents a compelling alternative to DI; however, state-of-the-art techniques involve only offline LC-HRMS approaches, which have important logistical drawbacks that make DOM analysis more challenging. This study introduces a new method based on online coupling of liquid chromatography to high resolution mass spectrometry, able to overcome the disadvantages of usual approaches. It is characterized by high reproducibility (% Bray–Curtis dissimilarity among replicates ≈ 2.5%), and it reduces transient complexity and contaminant interferences, thus increasing the signal-to-noise ratio (S/N), leading to the identification of an overall larger number of formulas in the mixture. Moreover, the application of an in silico fractionation prior to the statistical analysis allows an easy, flexible, fast, and detailed comparison of DOM samples from a variety of sources with a single chromatographic run.

Place, publisher, year, edition, pages
2018. Vol. 52, no 4, p. 2091-2099
National Category
Analytical Chemistry
Research subject
Chemistry with specialization in Analytical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-341015DOI: 10.1021/acs.est.7b04508ISI: 000426143300045OAI: oai:DiVA.org:uu-341015DiVA, id: diva2:1180574
Funder
Knut and Alice Wallenberg Foundation, 2013.0091Swedish Research Council, SRC 2015-4870Swedish Research Council, SRC 2014-04264Available from: 2018-02-06 Created: 2018-02-06 Last updated: 2018-04-19Bibliographically approved
In thesis
1. Characterization of dissolved organic matter: An analytical challenge
Open this publication in new window or tab >>Characterization of dissolved organic matter: An analytical challenge
2018 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Dissolved organic matter (DOM) is the prevalent form of organic carbon in most aquatic environments. It is an ultra-complex mixture that plays a crucial role in global carbon cycling. Despite its importance it is still poorly understood due to its extreme heterogeneity and intricacy. Major advances in chemical characterization of DOM were possible with the introduction of high-resolution mass spectrometry (HRMS). This technique, in combination with direct infusion (DI) as sample introduction, is the most powerful tool for the DOM analysis to date. A compelling alternative to DI is represented by upfront separation with liquid chromatography (LC); however, current techniques involve only offline LC-HRMS approaches, which exhibit important logistical drawbacks, making DOM analysis more challenging.

The aim of the presented studies was to develop new methods able to enhance the analysis of the dissolved organic matter and enable a wider range of researchers to participate in the advancement of this field.

In the first study, the application of the Orbitrap mass spectrometer for resolving complex DOM mixtures was investigated and the results were compared to the more established state-of-the-art technique, Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). The Orbitrap was capable of excellent reproducibility and detection of the majority of ionizable organic molecules in typical aquatic mixtures. The main disadvantage of the technique is that fewer molecular formulas can be resolved and detected because of lower resolution and sensitivity. This means that many sulfur peaks and all phosphorous containing peaks are not determined. Despite this drawback, our results suggest that the Orbitrap is an appropriate technique for the investigation of very subtle biogeochemical processing of bulk DOM. The lower costs (purchase and maintenance) and wider availability of Orbitrap mass spectrometers allow a greater number of laboratories to participate in the characterization of DOM.

In the second study, the first online method involving reverse phase chromatography and ultrahigh resolution mass spectrometry for the analysis of DOM was developed. This method overcomes the disadvantages of typical offline approaches. It enhances enormously the amount of information achievable in a single run, maintaining high resolution data, reducing analysis time and potential contamination. The introduction of in silico fractionation makes the method extremely flexible, allowing an easy, fast, and detailed comparison of DOM samples from a variety of sources.

Place, publisher, year, edition, pages
Uppsala: Department of Chemistry, 2018. p. 46
National Category
Analytical Chemistry
Research subject
Chemistry with specialization in Analytical Chemistry
Identifiers
urn:nbn:se:uu:diva-341690 (URN)
Presentation
2018-03-09, B7:101a, BMC, Husargatan 3, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2018-03-02 Created: 2018-02-12 Last updated: 2018-03-02Bibliographically approved

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Patriarca, ClaudiaBergquist, JonasSjöberg, Per JRTranvik, LarsHawkes, Jeffrey A.

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