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Screening for Organic Phosphorus Compounds in Aquatic Sediments by Liquid Chromatography Coupled to ICP-AES and ESI-MS/MS
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Physical and Analytical Chemistry, Analytical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Physical and Analytical Chemistry, Analytical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Physical and Analytical Chemistry, Analytical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Physical and Analytical Chemistry, Analytical Chemistry.
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2008 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 80, no 17, 6689-6697 p.Article in journal (Refereed) Published
Abstract [en]

The structures of organic phosphorous (P) compounds in aquatic sediments are to a large extent unknown although these compounds are considered to play an important role in regulating lake trophic status. To enhance identification of these compounds, a liquid chromatography (LC) method for their separation was developed. The stationary phase was porous graphitic carbon (PGC), and the mobile phases used in the gradient elution were compatible with both inductive coupled plasma atomic emission spectroscopy (ICP-AES) and electrospray ionization tandem mass spectrometry (ESI-MS/MS). With LC-ICP-AES, eight different P containing peaks could be observed in the P chromatogram indicating that at least eight different P compounds were separated. With the setup of an information dependent acquisition (IDA) with ESI-MS/MS, the mass over charge (m/z) of compounds containing a phosphate group (H2PO3, m/z 97) could be measured and further fragmentation experiments gave additional information on the structure of almost 40 separated P compounds, several were verified to be nucleotides. ICP-AES was very suitable in the development of the LC method and allowed screening and quantification of P compounds. The presented LC-ESI-MS/MS technique was able to identify several sediment organic P compounds.

Place, publisher, year, edition, pages
2008. Vol. 80, no 17, 6689-6697 p.
National Category
Analytical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-97626DOI: 10.1021/ac8006335ISI: 000258865300034OAI: oai:DiVA.org:uu-97626DiVA: diva2:172644
Available from: 2008-10-15 Created: 2008-10-15 Last updated: 2017-12-14Bibliographically approved
In thesis
1. Inductively Coupled Plasma Spectrometry for Speciation Analysis: Development and Applications
Open this publication in new window or tab >>Inductively Coupled Plasma Spectrometry for Speciation Analysis: Development and Applications
2007 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In analytical chemistry the main goal is normally to determine the identity and/or concentration of one or more species in a sample. The samples analyzed are often natural samples, containing numerous different species in a complex matrix and the choice of technique for multi-elemental detection is in general inductively coupled plasma spectrometry. The chemical forms of an element can affect many of its characteristics e.g. toxicity, which makes speciation analysis important. Therefore, determination of the identity and quantity of an element is still important, but for many applications measurements of total element concentration provides insufficient information. To be able to perform speciation analysis, separation, identification and/or characterization of the various forms of elements in the sample has to be accomplished. Speciation analysis has been employed in a wide range of disciplines, including for example environmental science, biology and clinical chemistry.

This thesis describes work to improve and understand the elemental speciation analysis with liquid chromatography coupled to plasma spectrometry and also highlights the importance and potential of the synergy between atomic spectrometry and molecular mass spectrometry. The combination of the matrix tolerant, robust and very sensitive plasma spectrometry used together with molecular mass spectrometry, which provides structural information and the possibility to identify unknown species, is demonstrated to be a very powerful tool for speciation analysis. In this thesis methods are developed for on-line sample clean-up and pre-concentration coupled to liquid chromatography and plasma spectrometry, which makes handling of small sample volumes easier and also decreases the risk of contamination. The problems associated with organic modifiers in plasma spectrometry are also addressed. Applications of speciation analysis are exemplified by analysis of aluminium-chelated siderophores in field-soil solutions and organic phosphorous species in aquatic sediments. The possibility to analyze un-dissolved samples as slurries with minimal sample preparation is also discussed.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2007. 56 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 327
Keyword
Analytical chemistry, Speciation analysis, Atomic emission spectrometry (AES), Mass spectrometry (MS), Inductively coupled plasma (ICP), Liquid Chromatography (LC), on-line sample pre-treatment, Organic phosphour, Siderophores, Slurry nebulization, matrix effects, Analytisk kemi
Identifiers
urn:nbn:se:uu:diva-8169 (URN)978-91-554-6945-0 (ISBN)
Public defence
2007-09-25, B41, BMC, Uppsala, 13:15 (English)
Opponent
Supervisors
Available from: 2007-09-04 Created: 2007-09-04 Last updated: 2011-05-10Bibliographically approved
2. Organic Phosphorus Compounds in Aquatic Sediments: Towards Molecular Identification with Mass Spectrometry
Open this publication in new window or tab >>Organic Phosphorus Compounds in Aquatic Sediments: Towards Molecular Identification with Mass Spectrometry
2008 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Phosphorus (P) regulates trophic status in most aquatic systems. However, only bioavailable P contributes to primary production. In most lakes and shallow seas, mineralisation of sediment P into its bioavailable form and its release to the water column is important for maintaining primary production. Sediment organic P forms a substantial proportion of this P to be mineralised and can originate from different sources on land (farmland, forests, etc.) or from primary production in the lake. These organic P forms can thus be expected to have differing composition, degradability and recyclable P content.

Knowledge of the chemical structure of sediment organic P compounds is scarce, mainly due to lack of appropriate analytical techniques. The commonly used 31P-nuclear magnetic resonance (31P-NMR) technique, only identifies P binding groups, so a mass spectrometric (MS) analysis method was developed that allows individual sediment organic P compounds to be identified.

EDTA as pre-extractant resulted in the highest P yield in subsequent NaOH extraction. Extracted organic P compound groups were identified using 31P-NMR. For identification of specific P compounds with MS, a sample preparation method prior to electrospray tandem mass spectrometry (ESI-MS/MS) analysis was developed. Liquid chromatography (LC) with porous graphitic carbon prior to ESI-MS/MS enhanced sensitivity and selectivity, enabling several of the ions detected to be identified as nucleotides. 31P-NMR analysis showed P monoesters to be the most stabile P compounds throughout a lake sediment profile. The developed LC-ESI-MS/MS analysis method revealed that some monoester-P (nucleotides) were labile, while other P compounds increased in concentration with Baltic Sea sediment depth and were therefore considered stabile. Differences in patterns of P compounds detected were also shown depending on catchment characteristics in relation to Baltic Sea sediment age.

For cost-effective management of eutrophication, knowledge of the sources of degradable organic P forms, contributing to internal loading, is needed. This thesis showed the developed LC-ESI-MS/MS analysis method to be a powerful analytical tool for this purpose.

Place, publisher, year, edition, pages
Uppsala: Universitetsbiblioteket, 2008. 58 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 560
Keyword
electrospray ionisation, mass spectrometry, liquid chromatography, organic phosphorus, aquatic sediment, eutrophication, sample preparation, extraction
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:uu:diva-9319 (URN)978-91-554-7306-8 (ISBN)
Public defence
2008-11-07, B42, BMC, Husargatan 3, Uppsala, Sweden, 10:15
Opponent
Supervisors
Available from: 2008-10-15 Created: 2008-10-15 Last updated: 2010-08-16Bibliographically approved

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Sjöberg, Per J. R.

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