Isoprenoid glycerol dialkanol diethers: A series of novel archaeal lipids in marine sediments

Liu, Xiao Lei; Lipp, Julius S.; Schröder, Jan M.; Summons, Roger E.; Hinrichs, Kai‐Uwe

doi:10.1016/j.orggeochem.2011.11.002

Cited by 54 publications

(50 citation statements)

References 27 publications

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“…S4). The offset between both methods, with LDI-based MI values being consistently higher than the LC-based counterparts, is possibly due to overestimation of GDGT-1 with the LDI approach due to codetection of unsaturated GDGT-0, which may be formed by dehydration of hydroxylated GDGT-0 (27).…”

Section: Resultsmentioning

confidence: 90%

Ultra-high-resolution paleoenvironmental records via direct laser-based analysis of lipid biomarkers in sediment core samples

Wörmer

Elvert

Fuchser

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

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Marine microorganisms adapt to their habitat by structural modification of their membrane lipids. This concept is the basis of numerous molecular proxies used for paleoenvironmental reconstruction. Archaeal tetraether lipids from ubiquitous marine planktonic archaea are particularly abundant, well preserved in the sedimentary record and used in several molecular proxies. We here introduce the direct, extraction-free analysis of these compounds in intact sediment core sections using laser desorption ionization (LDI) coupled to Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). LDI FTICR-MS can detect the target lipids in single submillimeter-sized spots on sediment sections, equivalent to a sample mass in the nanogram range, and could thus pave the way for biomarker-based reconstruction of past environments and ecosystems at subannual to decadal resolution. We demonstrate that ratios of selected archaeal tetraethers acquired by LDI FTICR-MS are highly correlated with values obtained by conventional liquid chromatography/MS protocols. The ratio of the major archaeal lipids, caldarchaeol and crenarchaeol, analyzed in a 6.2-cm intact section of Mediterranean sapropel S1 at 250-μm resolution (∼4-y temporal resolution), provides an unprecedented view of the fine-scale patchiness of sedimentary biomarker distributions and the processes involved in proxy signal formation. Temporal variations of this lipid ratio indicate a strong influence of the ∼200-y de Vries solar cycle on reconstructed sea surface temperatures with possible amplitudes of several degrees, and suggest signal amplification by a complex interplay of ecological and environmental factors. Laser-based biomarker analysis of geological samples has the potential to revolutionize molecular stratigraphic studies of paleoenvironments. molecular stratigraphy | solar cycle | laser desorption ionization | FTICR-MS | archaeal tetraether lipids M icrobial lipids in aquatic sediments reflect phylogeny, environmental conditions, and biogeochemistry of the water column in which they were produced. After sedimentation and because of the persistence of lipid structures in the sedimentary record, the information archived in these lipids remains available on geological time scales. Retrieval of this information from sediments and rocks has increasingly contributed to our understanding of past environments, microbial communities, and biogeochemical processes (e.g., refs. 1-5). Merged with the concept of molecular stratigraphy (2, 6), i.e., the analysis of selected biomarkers in solvent extracts of sediment samples in a stratigraphic framework, unique information can be gleaned regarding the temporal changes of past ecological and environmental conditions in aquatic systems. Because of analytical requirements, the temporal resolution is typically limited by centimeter-scale-sized samples, which, dependent on the depositional setting, tend to integrate time periods of decades to millennia, even in high-sedimentation settings such as the Santa Barbara Basin...

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Section: Resultsmentioning

confidence: 90%

Ultra-high-resolution paleoenvironmental records via direct laser-based analysis of lipid biomarkers in sediment core samples

Wörmer

Elvert

Fuchser

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

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“…Recently, a range of new glycerol ether lipids have been detected (Liu et al, 2012a), including glycerol dialkanol diethers (GDDs) which resemble GDGTs, in that the alkyl chains are attached to a glycerol at one end and to hydroxyl groups at the other end (Fig. 1).…”

Section: Introductionmentioning

confidence: 99%

“…Yet, neither their source, function or association with GDGTs have been clearly determined. Two hypotheses were proposed (Liu et al, 2012a;Meador et al, 2014;Yang et al, 2014): GDDs could be (i) degradation products of GDGTs or (ii) biosynthetic compounds, either as structural membrane compounds or as GDGT intermediates. Meador et al (2014) characterised a series of iso GDD IPLs with a glycosidic head group in estuarine and hot spring sediments as well as in a pure archaeal culture (Nitrosopumilus maritimus).…”

Section: Introductionmentioning

confidence: 99%

“…Our results confirm and extend their finding, as correlation between fractional abundances of both iso and br GDGTs and GDDs were found for the first time in the IPL pool. It strongly suggests that the two groups of compounds are closely related and share common metabolic and/or degradation pathways (Liu et al, 2012a;Meador et al, 2014;Yang et al, 2014), whatever their origin -archaeal or bacterial.…”

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confidence: 99%

“…This pathway involves the potential recycling of biphytane diols derived from the degradation of ancient GDGTs, which would be further linked to newly synthesized glycerol. Liu et al (2012a) and Meador et al (2014) proposed that iso GDDs may be involved in this pathway through glycerol addition or cleavage. Similar pathways are conceivable for br GDGTs.…”

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confidence: 99%

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Occurrence and distribution of glycerol dialkanol diethers and glycerol dialkyl glycerol tetraethers in a peat core from SW Tanzania

Coffinet

Huguet

Williamson

et al. 2015

Organic Geochemistry

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Christelle Anquetil, et al.. Occurrence and distribution of glycerol dialkanol diethers and glycerol dialkyl glycerol tetraethers in a peat core from SW Tanzania. Organic Geochemistry, Elsevier, 2015Elsevier, , 83-84, pp.170-177. 10.1016Elsevier, /j.orggeochem.2015 Their structures strongly resemble those of glycerol dialkyl glycerol tetraethers (GDGTs).Nevertheless, the origin of GDDs and their link to GDGTs remain unclear. Here we examined the concentration and distribution of iso GDDs and br GDDs, together with those of iso GDGTs and br GDGTs along a 4 m peat core from Tanzania. Whereas br GDDs have only been detected to date in their core lipid (CL) form, we report here, for the first time, br GDDs in both CL and intact polar lipid (IPL) forms, suggesting a biosynthetic origin for br GDDs. 2 metabolic pathways, although the hypothesis of GDDs being degradation products of GDGTs cannot be excluded. Concentration of br GDGTs and br GDDs on one hand, and of iso GDGTs and iso

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Structural characterization of ether lipids from the archaeonSulfolobus islandicusby high-resolution shotgun lipidomics

et al. 2015

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The molecular structures, biosynthetic pathways and physiological functions of membrane lipids produced by organisms in the domain Archaea are poorly characterized as compared with that of counterparts in Bacteria and Eukaryota. Here we report on the use of high-resolution shotgun lipidomics to characterize, for the first time, the lipid complement of the archaeon Sulfolobus islandicus. To support the identification of lipids in S. islandicus, we first compiled a database of ether lipid species previously ascribed to Archaea. Next, we analyzed the lipid complement of S. islandicus by high-resolution Fourier transform mass spectrometry using an ion trap-orbitrap mass spectrometer. This analysis identified five clusters of molecular ions that matched ether lipids in the database with sub-ppm mass accuracy. To structurally characterize and validate the identities of the potential lipid species, we performed structural analysis using multistage activation on the ion trap-orbitrap instrument as well as tandem mass analysis using a quadrupole time-of-flight machine. Our analysis identified four ether lipid species previously reported in Archaea, and one ether lipid species that had not been described before. This uncharacterized lipid species features two head group structures composed of a trisaccharide residue carrying an uncommon sulfono group (-SO3) and an inositol phosphate group. Both head groups are linked to a glycerol dialkyl glycerol tetraether core structure having isoprenoid chains with a total of 80 carbon atoms and 4 cyclopentane moieties. The shotgun lipidomics approach deployed here defines a novel workflow for exploratory lipid profiling of Archaea.

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Isoprenoid glycerol dialkanol diethers: A series of novel archaeal lipids in marine sediments

Cited by 54 publications

References 27 publications

Ultra-high-resolution paleoenvironmental records via direct laser-based analysis of lipid biomarkers in sediment core samples

Ultra-high-resolution paleoenvironmental records via direct laser-based analysis of lipid biomarkers in sediment core samples

Occurrence and distribution of glycerol dialkanol diethers and glycerol dialkyl glycerol tetraethers in a peat core from SW Tanzania

Structural characterization of ether lipids from the archaeonSulfolobus islandicusby high-resolution shotgun lipidomics

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