Identification of novel penta- and hexamethylated branched glycerol dialkyl glycerol tetraethers in peat using HPLC–MS2, GC–MS and GC–SMB-MS

Jonge, Cindy De; Hopmans, Ellen C.; Stadnitskaia, Alina; Rijpstra, W. Irene C.; Hofland, Ron; Tegelaar, Erik; Damsté, Jaap S. Sinninghe

doi:10.1016/j.orggeochem.2012.10.004

Cited by 193 publications

(127 citation statements)

References 12 publications

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“…This additional methylation occurs at one (i.e., 2) or both alkyl chains at C-5, although recently brGDGTs with the methylation at C-6 also have been reported (77). The detection of the 5-methyl iso-diabolic acid (i.e., 4) and MGE 6 in five out of seven species of SD 4 Acidobacteria now, for the first time, reveals that an additionally methylated iso-diabolic acid or its ether derivative is biosynthesized by Acidobacteria.…”

Section: Figmentioning

confidence: 96%

Ether- and Ester-Bound iso -Diabolic Acid and Other Lipids in Members of Acidobacteria Subdivision 4

Damsté

Rijpstra

Hopmans

et al. 2014

Appl Environ Microbiol

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123

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e Recently, iso-diabolic acid (13,16-dimethyl octacosanedioic acid) has been identified as a major membrane-spanning lipid of subdivisions 1 and 3 of the Acidobacteria, a highly diverse phylum within the Bacteria. This finding pointed to the Acidobacteria as a potential source for the bacterial glycerol dialkyl glycerol tetraethers that occur ubiquitously in peat, soil, lakes, and hot springs. Here, we examined the lipid composition of seven phylogenetically divergent strains of subdivision 4 of the Acidobacteria, a bacterial group that is commonly encountered in soil. Acid hydrolysis of total cell material released iso-diabolic acid derivatives in substantial quantities (11 to 48% of all fatty acids). In contrast to subdivisions 1 and 3 of the Acidobacteria, 6 out of the 7 species of subdivision 4 (excepting "Candidatus Chloracidobacterium thermophilum") contained iso-diabolic acid ether bound to a glycerol in larger fractional abundance than iso-diabolic acid itself. This is in agreement with the analysis of intact polar lipids (IPLs) by high-performance liquid chromatography-mass spectrometry (HPLC-MS), which showed the dominance of mixed ether-ester glycerides. iso-Diabolic acid-containing IPLs were not identified, because these IPLs are not released with a Bligh-Dyer extraction, as observed before when studying lipid compositions of subdivisions 1 and 3 of the Acidobacteria. The presence of ether bonds in the membrane lipids does not seem to be an adaptation to temperature, because the five mesophilic isolates contained a larger amount of ether lipids than the thermophile "Ca. Chloracidobacterium thermophilum." Furthermore, experiments with Pyrinomonas methylaliphatogenes did not reveal a major influence of growth temperature over the 50 to 69°C range.

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Section: Figmentioning

confidence: 96%

Ether- and Ester-Bound iso -Diabolic Acid and Other Lipids in Members of Acidobacteria Subdivision 4

Damsté

Rijpstra

Hopmans

et al. 2014

Appl Environ Microbiol

Self Cite

123

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“…A new method that has recently been proposed uses 2 silica columns in tandem, which improves the separation of brGDGTs and any occurring isomers with methyl branches attached on positions 6/6 ′ rather than 5/5 ′ (De Jonge et al, 2013;Hopmans et al, 2016). A subsequent re-investigation of the global surface soil calibration set indicated that 5-methyl brGDGTs relate to MAT, and 6-methyl brGDGTs to soil pH (De Jonge et al, 2014a).…”

Section: Brgdgt Distribution and Sourcementioning

confidence: 99%

Grain Size Associations of Branched Tetraether Lipids in Soils and Riverbank Sediments: Influence of Hydrodynamic Sorting Processes

Peterse

Eglinton

2017

Front. Earth Sci.

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We analyzed the abundance and distribution of branched glycerol dialkyl glycerol tetraethers (brGDGTs) in grain size fractions of 7 globally distributed river flank sediments and catchment soils in order to determine if and how the initial soil-brGDGT signature is influenced by hydrodynamic sorting upon entering a river and during subsequent transport from land to sea. BrGDGTs are hypothesized to form associations with high-surface-area fine-grained minerals in soils. Such associations, if maintained during transport, may impart resistance to degradation and promote downstream transport, reducing potential interferences by aquatic brGDGTs. We find that brGDGTs are indeed primarily associated with organic carbon (OC) bound to the clay-silt fraction (<63 µm) in both soils and river sediments, and that these associations appear to be maintained during river transport. However, the relative distribution of individual brGDGTs among size fractions is relatively uniform, suggesting that brGDGTs are well mixed in river sediments and that OC-mineral associations are continuously renewed. Consequently, the brGDGT signature finally stored in continental margin sediments appears insensitive to differential particle transport processes. Nevertheless, the lower (upstream) temperature signal generally reflected by brGDGTs in river sediments may also be explained by a contribution of in situ produced brGDGTs leading to an underestimation of reconstructed air temperatures.

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“…However, the tetramethylated brGDGTs (brIa to brIc), which contribute ≥80 % of total brGDGTs in all samples presented here (Table 5.S2), exist only as 5-methyl homologues (De Jonge et al, 2013). As such, fractional abundance of 6-methyl compounds only becomes significant at soil pH values greater than ≈6 (De Jonge et al, 2014a), suggesting that these homologues are of minimal importance in the highly acidic soils of the Congo basin.…”

Section: Effect Of 6-methyl Brgdgtsmentioning

confidence: 87%

“…Compounds were ionized using atmospheric-pressure chemical ionization ( . We note that this chromatographic method cannot separate multiple co-eluting compounds such as the six distinct peaks at 1050 m/z observed by Becker et al (2013) and the recently discovered 6-methyl brGDGTs IIa'-IIIc' (see Figure 5.S1 for structures ;De Jonge et al, 2013, 2014a. Such co-elution could potentially alter calculated brGDGT metrics, although this effect is likely negligible in our sample set (see Supplemental Discussion 5.9.1).…”

Section: Gdgt Detection and Analysismentioning

confidence: 88%

“…Updated chromatographic methods not employed here now allow for the separation of previously coeluting 5-methyl and 6-methyl brGDGTs and have led to improved metrics for tracking environmental parameters when calibrated using a global soil dataset (De Jonge et al, 2013, 2014aHopmans et al, 2016). However, the tetramethylated brGDGTs (brIa to brIc), which contribute ≥80 % of total brGDGTs in all samples presented here (Table 5.S2), exist only as 5-methyl homologues (De Jonge et al, 2013).…”

Identification of novel penta- and hexamethylated branched glycerol dialkyl glycerol tetraethers in peat using HPLC–MS2, GC–MS and GC–SMB-MS

Cited by 193 publications

References 12 publications

Ether- and Ester-Bound iso -Diabolic Acid and Other Lipids in Members of Acidobacteria Subdivision 4

Ether- and Ester-Bound iso -Diabolic Acid and Other Lipids in Members of Acidobacteria Subdivision 4

Grain Size Associations of Branched Tetraether Lipids in Soils and Riverbank Sediments: Influence of Hydrodynamic Sorting Processes

Understanding terrestrial organic carbon export : a time-series approach

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