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Organic Phosphorus Compounds in Aquatic Sediments: Analysis, Abundance and Effects
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för fysikalisk och analytisk kemi, Analytisk kemi.
2006 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

Phosphorus (P) is often the limiting nutrient in lacustrine and brackish eco-systems, and enhanced input of P into an aquatic system might therefore negatively impact the environment. Because modern waste water manage-ment have reduced external P input to surface waters, internal P loading from the sediment has become one of the main P sources to aquatic ecosys-tems, in which relatively unknown organic P compounds seem to be more active in P recycling than previously thought.

This thesis focus is on improving analysis methods for organic P com-pounds in lacustrine and brackish sediments, as well as determining which of these compounds might be degraded, mobilized and subsequently recycled to the water column and on what temporal scale this occur. In both lacustrine and brackish environments, the most labile P compound was pyrophosphate, followed by different phosphate diesters. Phosphate monoesters were the least labile organic P compounds and degraded the slowest with sediment depth. In regulated lakes, it was shown that pyrophosphate and polyphos-phate compound groups were most related to lake trophic status, thus indi-cating their involvement in P cycling. This thesis also indicates faster P turn-over in sediment from the brackish environment compared to sediment from the lacustrine environment.

A comparison of organic P extraction procedures showed that pre-extraction with EDTA, and NaOH as main extractant, was most efficient for total P extraction. Using buffered sodium dithionite (BD) as a pre-extractant and NaOH as main extractant was most efficient for extracting the presuma-bly most labile organic P compound groups, pyrophosphate and polyphos-phate. Furthermore, it was determined that organic P compounds associated with humic substances were more recalcitrant than other P compounds, that the BD step used in traditional P fractionation might extract phosphate monoesters, and that NMR is a statistically valid method for quantification of organic P compounds in sediment extracts.

Ort, förlag, år, upplaga, sidor
Uppsala: Acta Universitatis Upsaliensis , 2006. , s. 57
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 160
Nyckelord [en]
Environmental chemistry, Organic phosphorus, aquatic sediment, eutrophication, NMR, internal loading, sample preparation, extraction, degradation
Nyckelord [sv]
Miljökemi
Nationell ämneskategori
Miljövetenskap
Identifikatorer
URN: urn:nbn:se:uu:diva-6701ISBN: 91-554-6508-0 (tryckt)OAI: oai:DiVA.org:uu-6701DiVA, id: diva2:167993
Disputation
2006-04-21, B41, BMC, Husargatan 3, Uppsala, 10:00
Opponent
Handledare
Tillgänglig från: 2006-03-31 Skapad: 2006-03-31 Senast uppdaterad: 2011-06-10Bibliografiskt granskad
Delarbeten
1. Depth attenuation of biogenic phosphorus compounds in lake sediment measured by 31P NMR
Öppna denna publikation i ny flik eller fönster >>Depth attenuation of biogenic phosphorus compounds in lake sediment measured by 31P NMR
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2005 (Engelska)Ingår i: Environmental Science and Technology, ISSN 0013-936, Vol. 39, nr 3, s. 867-872Artikel i tidskrift (Refereegranskat) Published
Nationell ämneskategori
Naturvetenskap
Identifikatorer
urn:nbn:se:uu:diva-94212 (URN)
Tillgänglig från: 2006-03-31 Skapad: 2006-03-31 Senast uppdaterad: 2017-11-30Bibliografiskt granskad
2. Characterization of phosphorus in sequential extracts from lake sediments using P-31 nuclear magnetic resonance spectroscopy
Öppna denna publikation i ny flik eller fönster >>Characterization of phosphorus in sequential extracts from lake sediments using P-31 nuclear magnetic resonance spectroscopy
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2006 (Engelska)Ingår i: Canadian Journal of Fisheries and Aquatic Sciences, ISSN 0706-652X, E-ISSN 1205-7533, Vol. 63, nr 8, s. 1686-1699Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Phosphorus (P) compounds in three different lake surface sediments were extracted by sequential P extraction and identified by P-31 nuclear magnetic resonance (P-31 NMR) spectroscopy. The extraction procedure primarily discriminates between inorganic P-binding sites but most extraction steps also contained P not reacting (nrP) with the molybdenum complex during P analyses. In all three lakes, the nrP dominated in the NaOH extracts. Nonreactive P from the dystrophic lake was dominated by potentially recalcitrant P groups such as orthophosphate monoesters, while the nrP in the two more productive lakes also contained polyphosphates, pyrophosphate, and organic P groups such as P lipids and DNA-P that may be important in remineralization and recycling to the water column. In addition, polyphosphates showed substantial dynamics in settling seston. The Humic-P pools (P associated with humic acids) showed strong signals of orthophosphate monoesters in all three lakes, which supported the assumption that P-containing humic compounds are indeed recovered in this fraction, although other organic P forms are also present. Thus, in addition to expanding the understanding of which organic P forms that are present in lake sediments, the P-31 NMR technique also demonstrated that the chemical extraction procedure may provide some quantification of recalcitrant versus labile organic P forms.

Nationell ämneskategori
Biologiska vetenskaper
Identifikatorer
urn:nbn:se:uu:diva-94213 (URN)10.1139/F06-070 (DOI)000239655100003 ()
Tillgänglig från: 2006-03-31 Skapad: 2006-03-31 Senast uppdaterad: 2017-12-14Bibliografiskt granskad
3. Degradation of organic phosphorus compounds in anoxic Baltic Sea sediments: A P-31 nuclear magnetic resonance study
Öppna denna publikation i ny flik eller fönster >>Degradation of organic phosphorus compounds in anoxic Baltic Sea sediments: A P-31 nuclear magnetic resonance study
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2006 (Engelska)Ingår i: Limnology and Oceanography, ISSN 0024-3590, E-ISSN 1939-5590, Vol. 51, nr 5, s. 2341-2348Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

The composition and abundance of phosphorus extracted by NaOH-ethylenediaminetetraacetic acid from anoxic Northwest Baltic Sea sediment was characterized and quantified using solution P-31 nuclear magnetic resonance. Extracts from sediment depths down to 55 cm, representing 85 yr of deposition, contained 18.5 g m(-2) orthophosphate. Orthophosphate monoesters, teichoic acid P, microbial P lipids, DNA P, and pyrophosphate corresponded to 6.7, 0.3, 1.1, 3.0, and 0.03 g P m(-2), respectively. The degradability of these compound groups was estimated by their decline in concentration with sediment depth. Pyrophosphate had the shortest half-life (3 yr), followed by microbial P lipids with a half-life of 5 yr, DNA P (8 yr), and orthophosphate monoesters (16 yr). No decline in concentration with sediment depth was observed for orthophosphate or teichoic acid P.

Nationell ämneskategori
Biologiska vetenskaper
Identifikatorer
urn:nbn:se:uu:diva-94214 (URN)000240673800036 ()
Tillgänglig från: 2006-03-31 Skapad: 2006-03-31 Senast uppdaterad: 2017-12-14Bibliografiskt granskad
4. Biogenic phosphorus in oligotrophic mountain lake sediments: Differences in composition measured with NMR spectroscopy
Öppna denna publikation i ny flik eller fönster >>Biogenic phosphorus in oligotrophic mountain lake sediments: Differences in composition measured with NMR spectroscopy
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2006 (Engelska)Ingår i: Water Research, ISSN 0043-1354, E-ISSN 1879-2448, Vol. 40, nr 20, s. 3705-3712Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Phosphorus (P) composition in alkaline sediment extracts from three Swedish oligotrophic mountain lakes was investigated using P-31-NMR spectroscopy. Surface sediments from one natural lake and two mature reservoirs, one of which has received nutrient additions over the last 3 years, were compared with respect to biogenic P composition. The results show significant differences in the occurrence of labile and biogenic P species in the sediments of the different systems. The P compound groups that varied most between these three systems were pyrophosphate and polyphosphates, compound groups known to play an important role in sediment P recycling. The content of these compound groups was lowest in the reservoirs and may indicate a coupling between anthropogenic disturbances (i.e., impoundment) to a water system and the availability of labile P species in the sediment. A statistical study was also conducted to determine the accuracy and reliability of using P-31-NMR spectroscopy for quantification of sediment P forms.

Nyckelord
phosphorus species, P-31-NMR spectroscopy, reservoirs, oligotrophication, method validation, P-31-NMR accuracy
Nationell ämneskategori
Biologiska vetenskaper
Identifikatorer
urn:nbn:se:uu:diva-94215 (URN)10.1016/j.watres.2006.09.006 (DOI)000242988600005 ()17070896 (PubMedID)
Tillgänglig från: 2006-03-31 Skapad: 2006-03-31 Senast uppdaterad: 2017-12-14Bibliografiskt granskad
5. Degradation rates of organic phosphorus in lake sediment
Öppna denna publikation i ny flik eller fönster >>Degradation rates of organic phosphorus in lake sediment
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2007 (Engelska)Ingår i: Biogeochemistry, ISSN 0168-2563, E-ISSN 1573-515X, Vol. 82, nr 1, s. 15-28Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Phosphorus (P) binding groups were identified in phytoplankton, settling particles, and sediment profiles by 31P NMR spectroscopy from the Swedish mesotrophic Lake Erken. The 31P NMR analysis revealed that polyphosphates and pyrophosphates were abundant in the water column, but rapidly mineralized in the sediment. Orthophosphate monoesters and teichoic acids degraded more slowly than DNA-P, polyphosphates, and P lipids. Humic acids and organic acids from phytoplankton were precipitated from the NaOH extract by acidification and identified by 31P NMR spectroscopy. The precipitated P was significantly more recalcitrant than the P compound groups remaining in solution, but does not constitute a major sink of P as it did not reach a stable concentration with depth, which indicates that it may eventually be degraded. Since P also precipitated from phytoplankton, the origin of humic-P can not be related solely to allochthonous P.

Nyckelord
Organic P, 31P NMR, Lake sediment, Degradation rates
Nationell ämneskategori
Biologiska vetenskaper Kemi
Identifikatorer
urn:nbn:se:uu:diva-97627 (URN)10.1007/s10533-006-9049-z (DOI)000244070900002 ()
Tillgänglig från: 2008-10-15 Skapad: 2008-10-15 Senast uppdaterad: 2022-01-28Bibliografiskt granskad
6. Sediment Phosphorus Extractants for Phosphorus-31 Nuclear Magnetic Resonance Analysis: A Quantitative Evaluation
Öppna denna publikation i ny flik eller fönster >>Sediment Phosphorus Extractants for Phosphorus-31 Nuclear Magnetic Resonance Analysis: A Quantitative Evaluation
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2007 (Engelska)Ingår i: Journal of Environmental Quality, ISSN 0047-2425, E-ISSN 1537-2537, Vol. 36, nr 3, s. 892-898Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

The influence of pre-extractant, extractant, and post-extractant on total extracted amounts of P and organic P compound groups measured with 31P nuclear magnetic resonance (31P-NMR) in lacustrine sediment was examined. The main extractants investigated were sodium hydroxide (NaOH) and sodium hydroxide ethylenediaminetetraacetic acid (NaOH-EDTA) with bicarbonate buffered dithionite (BD) or EDTA as pre-extractants. Post extractions were conducted using either NaOH or NaOH-EDTA, depending on the main extractant. Results showed that the most efficient combination of extractants for total P yield was NaOH with EDTA as pre-extractant, yielding almost 50% more than the second best procedure. The P compound groups varying the most between the different extraction procedures were polyphosphates and pyrophosphates. NaOH with BD as pre-extractant was the most efficient combination for these compound groups.

Nationell ämneskategori
Kemi
Identifikatorer
urn:nbn:se:uu:diva-94217 (URN)10.2134/jeq2006.0235 (DOI)000246430500028 ()17485721 (PubMedID)
Tillgänglig från: 2006-03-31 Skapad: 2006-03-31 Senast uppdaterad: 2017-12-14Bibliografiskt granskad

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