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Online HPLC-ESI-HRMS Method for the Analysis and Comparison of Different Dissolved Organic Matter Samples
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.ORCID-id: 0000-0002-4301-3923
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.ORCID-id: 0000-0002-4597-041x
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC, Analytisk kemi.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Biologiska sektionen, Institutionen för ekologi och genetik, Limnologi.ORCID-id: 0000-0003-3509-8266
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2018 (Engelska)Ingår i: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 52, nr 4, s. 2091-2099Artikel i tidskrift (Refereegranskat) 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.

Ort, förlag, år, upplaga, sidor
2018. Vol. 52, nr 4, s. 2091-2099
Nationell ämneskategori
Analytisk kemi
Forskningsämne
Kemi med inriktning mot analytisk kemi
Identifikatorer
URN: urn:nbn:se:uu:diva-341015DOI: 10.1021/acs.est.7b04508ISI: 000426143300045OAI: oai:DiVA.org:uu-341015DiVA, id: diva2:1180574
Forskningsfinansiär
Knut och Alice Wallenbergs Stiftelse, 2013.0091Vetenskapsrådet, SRC 2015-4870Vetenskapsrådet, SRC 2014-04264Tillgänglig från: 2018-02-06 Skapad: 2018-02-06 Senast uppdaterad: 2018-12-12Bibliografiskt granskad
Ingår i avhandling
1. Characterization of dissolved organic matter: An analytical challenge
Öppna denna publikation i ny flik eller fönster >>Characterization of dissolved organic matter: An analytical challenge
2018 (Engelska)Licentiatavhandling, sammanläggning (Övrigt vetenskapligt)
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.

Ort, förlag, år, upplaga, sidor
Uppsala: Department of Chemistry, 2018. s. 46
Nationell ämneskategori
Analytisk kemi
Forskningsämne
Kemi med inriktning mot analytisk kemi
Identifikatorer
urn:nbn:se:uu:diva-341690 (URN)
Presentation
2018-03-09, B7:101a, BMC, Husargatan 3, Uppsala, 10:15 (Engelska)
Opponent
Handledare
Tillgänglig från: 2018-03-02 Skapad: 2018-02-12 Senast uppdaterad: 2018-03-02Bibliografiskt granskad

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