Organic Geochemistry最新文献

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Identification of novel sulfur-containing petroporphyrins in a natural bitumen: Potential biomarkers for aerobic organisms
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-04-04 DOI: 10.1016/j.orggeochem.2025.104987
Fang Zheng , Weisheng Yang , Yanbin Wang , Mi An , Da Huo , Chunyan Wang , Qing Cao , Jing He , Quan Shi , Yongge Sun
{"title":"Identification of novel sulfur-containing petroporphyrins in a natural bitumen: Potential biomarkers for aerobic organisms","authors":"Fang Zheng ,&nbsp;Weisheng Yang ,&nbsp;Yanbin Wang ,&nbsp;Mi An ,&nbsp;Da Huo ,&nbsp;Chunyan Wang ,&nbsp;Qing Cao ,&nbsp;Jing He ,&nbsp;Quan Shi ,&nbsp;Yongge Sun","doi":"10.1016/j.orggeochem.2025.104987","DOIUrl":"10.1016/j.orggeochem.2025.104987","url":null,"abstract":"<div><div>In this study, a serial of novel sulfur-containing petroporphyrins were identified in a natural bitumen by chemical derivatization and solvent extraction. In contrast to previously reported sulfur-containing petroporphyrins, the new petroporphyrins exhibit reduced unsaturation and are characterized by a reduced number of double-bond equivalences (number of rings plus double bonds). Molecular structures of these sulfur-containing petroporphyrins were further elucidated by multiple collision-induced dissociation in Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). The results indicate that sulfur atoms are present as cyclic thioether on the side chain of porphyrin, suggesting that these compounds may have evolved from <em>heme</em> <strong><em>a</em></strong> or <em>heme</em> <strong><em>o</em></strong> in aerobic organisms. We thereby propose a potentially diagenetic pathway of these compounds. Due to the relative stability of cyclic thioethers in the porphyrin structure, potential geochemical information could be carried by these compounds, which warrants further investigation.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104987"},"PeriodicalIF":2.6,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nanometer-scale relationships between sedimentary organic matter molecular composition, fluorescence, cathodoluminescence, and reflectance: The importance of oxygen content at low thermal maturities
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-04-04 DOI: 10.1016/j.orggeochem.2025.104990
Aaron M. Jubb , Paul C. Hackley , Ryan J. McAleer , Jing Qu
{"title":"Nanometer-scale relationships between sedimentary organic matter molecular composition, fluorescence, cathodoluminescence, and reflectance: The importance of oxygen content at low thermal maturities","authors":"Aaron M. Jubb ,&nbsp;Paul C. Hackley ,&nbsp;Ryan J. McAleer ,&nbsp;Jing Qu","doi":"10.1016/j.orggeochem.2025.104990","DOIUrl":"10.1016/j.orggeochem.2025.104990","url":null,"abstract":"<div><div>Molecular characterization of sedimentary organic matter (SOM), termed macerals, is a common goal when seeking to understand petroleum generation as well as other geologic processes in deep time. However, unambiguous measurement of discrete macerals is challenging due to the small size of organic particles in sedimentary rocks, the proximity of different organic matter types to one another, mineral-organic matter interactions, and maceral mixing that occurs during SOM isolation prior to ex situ analysis. The recent advent of infrared spectrometers capable of nanometer-scale resolution and the application of these technologies to geologic samples has enabled advances in rapid, in situ molecular characterization of SOM allowing for insights into paleoenvironmental processes, such as organic matter productivity and preservation, among others. Here we employ one such technology, optical photothermal infrared (OPTIR) spectroscopy, to map SOM functional group distributions at 500-nm resolution in a sample from the Lower Cretaceous Sunniland Limestone of the South Florida Basin. Examined fields of view include occurrences of amorphous organic matter (AOM), inertinite, micrinite, solid bitumen, telalginite, and vitrinite. OPTIR data from these macerals are compared against traditional organic petrographic data from the same organic grains including fluorescence intensity and white light reflectance as well as against cathodoluminescence response, an emerging organic petrographic approach. Maceral oxygen content (using carbonyl functional group abundance as a proxy) is observed to vary widely between maceral types but correlates strongly with fluorescence and cathodoluminescence intensity as well as against reflectance. These findings highlight the important role that oxygen content plays in determining the optical properties of SOM and further demonstrate the ability of OPTIR to discriminate subtle molecular differences between SOM types.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104990"},"PeriodicalIF":2.6,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767532","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Analytical inconsistencies in the measurement and reporting of IP25, IPSO25 and related biomarkers for paleo sea ice reconstruction
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-03-22 DOI: 10.1016/j.orggeochem.2025.104989
Simon T. Belt , Lukas Smik
{"title":"Analytical inconsistencies in the measurement and reporting of IP25, IPSO25 and related biomarkers for paleo sea ice reconstruction","authors":"Simon T. Belt ,&nbsp;Lukas Smik","doi":"10.1016/j.orggeochem.2025.104989","DOIUrl":"10.1016/j.orggeochem.2025.104989","url":null,"abstract":"<div><div>IP<sub>25</sub> and related biomarkers are commonly used for Arctic and Antarctic sea ice reconstruction. With a growing number of laboratories performing their measurement, we reviewed many publications spanning the period 2007–2024 in order to assess analytical rigour. We found a number of common shortfalls in analytical protocols, or at least how they are reported, which may have important implications for future synthesis studies and meta-data analyses. Here, we outline some of these shortcomings and provide suggestions of how to improve both data acquisition and reporting.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104989"},"PeriodicalIF":2.6,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143724185","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unraveling the origin and charge of Halahatang oils, Tarim Basin
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-03-16 DOI: 10.1016/j.orggeochem.2025.104962
Peng Sun , Chunfang Cai , Daowei Wang , Yu Qi , Chenlu Xu , Paul F. Greenwood
{"title":"Unraveling the origin and charge of Halahatang oils, Tarim Basin","authors":"Peng Sun ,&nbsp;Chunfang Cai ,&nbsp;Daowei Wang ,&nbsp;Yu Qi ,&nbsp;Chenlu Xu ,&nbsp;Paul F. Greenwood","doi":"10.1016/j.orggeochem.2025.104962","DOIUrl":"10.1016/j.orggeochem.2025.104962","url":null,"abstract":"<div><div>Uncertainty about the source of the oils from the Halahatang region of the Tabei Uplift, Tarim Basin (NW China) presents an ongoing challenge to exploration. Previous analyses of several Halahatang oils showed isotopic (δ<sup>13</sup>C &lt; –32 ‰) and aliphatic hydrocarbon distributions (e.g., V-shaped C<sub>27</sub>-C<sub>29</sub> steranes) more typical of regional Ordovician source rocks than the Cambrian rocks that are the predominant source of petroleum of the Tarim Basin, supporting prospects for a second major regional oil source. In pursuit of a more definitive source assignment of Halahatang oils and further insight into their depositional environment and charge history, a detailed molecular appraisal of the aromatic hydrocarbon composition of 27 marine oils and complementary stable sulfur and carbon isotopic analyses were conducted. The oils were from different Halahatang wells resolved into three separate block groups, with variations to the extent molecular and isotopic data was influenced by secondary alteration (i.e., thermal maturity, biodegradation and, possibly, minor thermochemical sulfate reduction) evident among the groups. The major aromatic products of all oils were alkylated naphthalenes, phenanthrenes, dibenzothiophenes and trace levels of thiadiamondoids were detected in a few Group II and III oils. Aryl isoprenoids, typical biomarkers of an euxinic depositional environment, were also conspicuous in lower maturity Group I and II oils (Rc &lt; 0.9 %), but absent in higher maturity oils (Rc up to 1.02 %). Molecular evidence of severe biodegradation (e.g., unresolved complex matter, 25-norterpenoids) was evident in some Group I oils, although some of these also showed coincident non-biodegradation molecular features (e.g., low MW <em>n</em>-alkanes) implying a mixing of biodegraded and non-biodegraded charges. The δ<sup>34</sup>S values of the bulk oil and their dibenzothiophene and alkyldibenzothiophene products were generally in the range +17 to +23 ‰,although some oils impacted by biodegradation showed slightly heavier δ<sup>34</sup>S values (&gt;+26 ‰). The Group II oils were not significantly impacted by secondary processes and their aromatic signature (e.g., aryl isoprenoids), δ<sup>34</sup>S data and whole oil δ<sup>13</sup>C values were closely correlated with regional Lower Cambrian source rocks and are atypical of Upper Ordovician source rocks. These results identify the Halahatang oils as a further representation of Lower Cambrian-derived oils of the Tabei Uplift.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104962"},"PeriodicalIF":2.6,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143631874","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Clumped 13C–13C isotopes of ethane from laboratory pyrolysis of kerogen: Implications for intramolecular 13C distributions
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-03-15 DOI: 10.1016/j.orggeochem.2025.104951
Koudai Taguchi , Yuichiro Ueno , Alexis Gilbert , Xiaoqiang Li , Juske Horita
{"title":"Clumped 13C–13C isotopes of ethane from laboratory pyrolysis of kerogen: Implications for intramolecular 13C distributions","authors":"Koudai Taguchi ,&nbsp;Yuichiro Ueno ,&nbsp;Alexis Gilbert ,&nbsp;Xiaoqiang Li ,&nbsp;Juske Horita","doi":"10.1016/j.orggeochem.2025.104951","DOIUrl":"10.1016/j.orggeochem.2025.104951","url":null,"abstract":"<div><div>The clumped isotope geochemistry of <sup>13</sup>C–<sup>13</sup>C bonding offers a valuable tool for distinguishing the formation processes of ethane (C<sub>2</sub>H<sub>6</sub>) and its thermogenic and abiotic origins. Thermogenic ethane is characterized by isotope distributions that are nearly in thermodynamic equilibrium, whereas abiotic ethane is governed by kinetic isotope effects during C–C bond synthesis. <sup>13</sup>C–<sup>13</sup>C ordering in thermogenic ethane varies with the source organic material, but limited studies on ethane clumped isotopes from natural gases restrict our understanding of these signatures. To address this, we performed pyrolysis experiments at 310–470 °C on various immature kerogens from the Eocene Green River Formation (Type I), Upper Devonian–Lower Mississippian Woodford Shale (Type II), and Pennsylvanian Springfield Coal Member (Type III). The ethane-clumped isotope compositions aligned with those of natural gas samples and varied based on the starting kerogen’s isotope composition. We propose a thermogenic model that describes isotopic systematics, including <sup>13</sup>C–<sup>13</sup>C variations in the pyrolysis product ethane, driven by (i) combinatorial isotope effect during C–C bond breaking and (ii) intramolecular isotopic heterogeneity in the starting kerogen. Isotopic and clumped isotope variations suggest a zigzag isotopic pattern in kerogen alkyl chains, similar to that seen in biological fatty acids. We could extend the model to position-specific (PS) isotope signatures in propane, showing that intramolecular isotopic heterogeneity in kerogens also affect PS isotopes, alongside structural heterogeneity, such as isoprenoid versus alkyl. Overall, our findings demonstrate that <sup>13</sup>C–<sup>13</sup>C clumping is a ubiquitous signature for thermogenic ethane, with variations reflecting isotopic information of the original organic matter.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104951"},"PeriodicalIF":2.6,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143631872","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mid- to Late-Holocene branched GDGT-based air temperatures from a crater lake in Cameroon (Central Africa)
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-03-14 DOI: 10.1016/j.orggeochem.2025.104982
Guillemette Ménot , Salomé Ansanay-Alex , Valérie F. Schwab , Gilbert Todou , Olivier Séné , Jean-Michel Onana , Gerd Gleixner , Dirk Sachse , Yannick Garcin
{"title":"Mid- to Late-Holocene branched GDGT-based air temperatures from a crater lake in Cameroon (Central Africa)","authors":"Guillemette Ménot ,&nbsp;Salomé Ansanay-Alex ,&nbsp;Valérie F. Schwab ,&nbsp;Gilbert Todou ,&nbsp;Olivier Séné ,&nbsp;Jean-Michel Onana ,&nbsp;Gerd Gleixner ,&nbsp;Dirk Sachse ,&nbsp;Yannick Garcin","doi":"10.1016/j.orggeochem.2025.104982","DOIUrl":"10.1016/j.orggeochem.2025.104982","url":null,"abstract":"<div><div>African low-latitude regions tend to be underrepresented in global continental temperature reconstructions, limiting both our understanding and the reliability of predictions of past and future changes in temperature and precipitation in those parts of the world. The lack of continuous sedimentary archives and quantitative temperature proxies further complicates this issue, especially outside Eastern Africa. Here, we use data collected in Cameroon lakes to assess branched glycerol dialkyl glycerol tetraether (brGDGT)-based temperature proxies and examine potential confounding variables impacting temperature reconstructions. By analyzing GDGT distributions in soil watershed, water column, and surface sediment samples from a total of 11 Cameroon lakes, we could verify that the degree of methylation of brGDGTs (through the MBT′<sub>5Me</sub>) can serve as a reliable indicator for reconstructing mean annual air temperatures. Additionally, we could confirm that surface water conductivity represents a controlling factor for the brGDGT assemblage in surface sediments of crater lakes. Moreover, we provide the first reconstruction of Mid- to Late-Holocene GDGT-based air temperatures for a crater lake in Cameroon (Central Africa), revealing a temperature decrease of 2.5 °C over the last 7000 years, which agrees with recently published records for East Africa but exceeds current model predictions. These discrepancies highlight the need for additional studies to focus on this geographically underrepresented area.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104982"},"PeriodicalIF":2.6,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760936","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Reforestation in northeastern China increased the soil microbial necromass carbon accumulation by influencing glomalin and enzyme activities
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-03-13 DOI: 10.1016/j.orggeochem.2025.104983
Li Pan , Xiuwei Wang
{"title":"Reforestation in northeastern China increased the soil microbial necromass carbon accumulation by influencing glomalin and enzyme activities","authors":"Li Pan ,&nbsp;Xiuwei Wang","doi":"10.1016/j.orggeochem.2025.104983","DOIUrl":"10.1016/j.orggeochem.2025.104983","url":null,"abstract":"<div><div>Farmland reforestation is a common measure aimed at improving soil properties and preventing soil carbon loss, with microbial necromass carbon (MNC) being a crucial component of soil organic carbon. The changes in soil MNC content are closely linked to microbial community structure and microbial metabolites. However, the precise impact of microbial community, enzyme activities, and glomalin-related soil protein (GRSP) on MNC accumulation following the conversion from farmland to forest remains incompletely understood. To address these knowledge gaps, soil samples were collected from a farmland and two adjacent forests in the black soil region of Northeast China, focusing on the 0–30 cm depth. By utilizing the microbial cell wall’s biomarker amino sugars, the study estimated MNC contents and investigated how reforestation influences MNC levels in farmland, along with exploring the underlying mechanisms. The results revealed a significant increase in soil MNC by 139–167% and soil organic carbon by 25–34% post-reforestation. Moreover, the contribution of MNC to the soil organic carbon pool was enhanced following reforestation. It was observed that GRSP content was predominantly influenced by microbial community composition, with β-1,4-N-acetyl-glucosaminidase and GRSP emerging as key indicators affecting soil MNC levels. Notably, compared to microbial community composition alone, GRSP and enzyme activities exerted a more substantial impact on MNC in soil. In conclusion, this study underscores the significance of GRSP and enzyme activities in shaping soil MNC accumulation, thereby enhancing our understanding of the implications of reforestation on soil carbon stocks and the microbial-driven mechanisms at play.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104983"},"PeriodicalIF":2.6,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143687784","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sedimentary geochemical records of the palaeovegetation and palaeoclimate evolution in the Pinghu Formation, Western Slope Belt, Xihu Sag, East China Sea Basin
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-03-09 DOI: 10.1016/j.orggeochem.2025.104973
Yanan Wang , Lin Wei , Xiong Cheng , Hui Diao , Wenjun Li , Dujie Hou , Jiansheng Li
{"title":"Sedimentary geochemical records of the palaeovegetation and palaeoclimate evolution in the Pinghu Formation, Western Slope Belt, Xihu Sag, East China Sea Basin","authors":"Yanan Wang ,&nbsp;Lin Wei ,&nbsp;Xiong Cheng ,&nbsp;Hui Diao ,&nbsp;Wenjun Li ,&nbsp;Dujie Hou ,&nbsp;Jiansheng Li","doi":"10.1016/j.orggeochem.2025.104973","DOIUrl":"10.1016/j.orggeochem.2025.104973","url":null,"abstract":"<div><div>The sedimentary development of source rocks in marine-continental transitional facies is controlled mainly by the synergistic evolution of palaeovegetation and palaeoclimate. A set of marine-continental transitional coal seams in Xihu Sag of the East China Sea Basin were discovered at the end of the last century, whose lithology is mainly fine-grained sedimentary, with significant non-homogeneity and complex developmental control factors. Although systematic geochemical evaluations and hydrocarbon potential studies have been carried out on the source rocks in the Xihu Sag, few studies have focused on the fine-grained characterization of the palaeovegetation and palaeoclimate evolution during the depositional period. In this study, the palaeovegetation and palaeoclimate of the Pinghu Formation in Xihu Sag have been reconstructed based on biomarkers, pollen abundance, and trace elements. The organic matter of the Pinghu Formation is mainly input from terrigenous higher plants. The biomarkers reveal that gymnosperms gradually increase from the early to late stages of the Pinghu Formation, whereas pteridophytes exhibit the opposite trend. The contribution of gymnosperms to organic matter in the Wuyunting area is higher than in the Pinghu area. Furthermore, the number of temperate deciduous broad-leaved angiosperms (<em>Alnipollenites</em>, <em>Ulmipollenites</em>, <em>Momipites</em>, and <em>Juglanspollenites</em>) and mountain coniferous gymnosperms (<em>Pinuspollenites</em>) increased from the early to late stages of the Pinghu Formation, while the abundance of tropical/subtropical plants (<em>Quercoidites</em>, <em>Taxodiaceaepollenites</em>, and <em>Salixipollenites</em>) decreased. The vegetation succession<!--> <!-->is characterized by gradually transforming from tall gymnosperms to low-growing pteridophytes from the northern Wuyunting area to the southern Pinghu area. In conclusion, palynological data (including pteridophytes, angiosperms, and gymnosperms) and trace element ratios indicate that from the early to late stages of the Pinghu Formation, the palaeoclimate gradually became colder, with humidity and water depth decreasing.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"203 ","pages":"Article 104973"},"PeriodicalIF":2.6,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143578858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Preservation of archaeal core lipids in siliceous hot spring deposits: An experimental study 硅质温泉沉积中古生物核心脂质的保存:实验研究
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-03-04 DOI: 10.1016/j.orggeochem.2025.104974
L. Weimann , M. Reinhardt , C. Ostertag-Henning , J.-P. Duda , V. Thiel
{"title":"Preservation of archaeal core lipids in siliceous hot spring deposits: An experimental study","authors":"L. Weimann ,&nbsp;M. Reinhardt ,&nbsp;C. Ostertag-Henning ,&nbsp;J.-P. Duda ,&nbsp;V. Thiel","doi":"10.1016/j.orggeochem.2025.104974","DOIUrl":"10.1016/j.orggeochem.2025.104974","url":null,"abstract":"<div><div>Siliceous hot spring systems have been present on our planet since at least 3.5 Ga, often hosting diverse communities of Archaea. Isoprenoid core lipids are important biomarkers for these microorganisms, but these lipids have only been reported from modern and subrecent siliceous sinter settings, perhaps indicating a bias against their long-term preservation in such environments. We conducted closed-system maturation experiments with the archaeal core lipids archaeol and isoprenoid glycerol dialkyl glycerol tetraethers (isoGDGTs) at 250 °C and 300 bar for 14 days. Compounds were heated with artificial sea water, with and without silica, as single compounds, and as part of a lipid mixture from a microbial mat. The products were analyzed using gas chromatography-mass spectrometry, scanning electron microscopy, and X-ray diffraction. This allowed to assess the preservation potential of these biomarkers during simulated siliceous sinter formation and subsequent diagenesis. Amorphous silica gel transformed into small microspheres (∼10 µm) when heated with single organic compounds, but formed more irregularly shaped rounded grains when heated with the lipid mixture. The presence of silica led to an enhanced degradation of archaeol, most likely caused by hydroxyl radicals deriving from silica-fluid interactions. IsoGDGTs, in contrast, were less affected by silica and showed an enhanced stability when heated as part of the lipid mixture. The results indicate that (i) the silica matrix, (ii) the molecular structure, and (iii) the presence of other organic compounds play a critical role for the preservation of archaeal core lipids in siliceous hot spring systems.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"204 ","pages":"Article 104974"},"PeriodicalIF":2.6,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143631873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optimized sample cleanup for compound-specific isotope analysis of polycyclic aromatic hydrocarbons in complex environmental samples
IF 2.6 3区 地球科学
Organic Geochemistry Pub Date : 2025-02-28 DOI: 10.1016/j.orggeochem.2025.104966
Md Samrat Alam , Jason M.E. Ahad , Colin A. Cooke
{"title":"Optimized sample cleanup for compound-specific isotope analysis of polycyclic aromatic hydrocarbons in complex environmental samples","authors":"Md Samrat Alam ,&nbsp;Jason M.E. Ahad ,&nbsp;Colin A. Cooke","doi":"10.1016/j.orggeochem.2025.104966","DOIUrl":"10.1016/j.orggeochem.2025.104966","url":null,"abstract":"<div><div>Compound-specific isotope analysis (CSIA) using gas chromatography – isotope ratio mass spectrometry is a powerful tool to discriminate sources of polycyclic aromatic hydrocarbons (PAHs). However, interferences from co-eluting peaks often prevent accurate isotopic measurements in complex environmental samples. Purification of sample extracts is thus a crucial analytical step. In this study, we report a rapid and effective cleanup method using high-performance liquid chromatography (HPLC) that provides high integrity isolation of PAHs suitable for CSIA. The method reported here was effective at purifying both parent and alkylated PAHs from several highly complex matrices, including river sediments, bitumen, petroleum coke, and wildfire ash. HPLC separation removed much of the interfering aromatic unresolved complex mixture (UCM) and significantly improved chromatography, yielding well-resolved PAH peaks with high intensities and signal-to-noise ratios. Recoveries and purities of target compounds following HPLC separation were 70 ± 13% and 97 ± 5%, respectively. No noticeable differences (± 0.5‰) were observed in the carbon isotope values (δ<sup>13</sup>C) of standards subjected to extraction and HPLC purification steps, indicating negligible isotopic fractionation associated with the protocol. The δ<sup>13</sup>C values for individual PAHs in samples were comparable to those previously reported for the same sample types, further demonstrating this method’s high level of accuracy and precision. Additionally, this technique allows for isotopic characterisation of a larger number of 4- to 5-ring PAHs compared to many previous studies due to removal of much of the later-eluting UCM, potentially providing greater insight into source discrimination and understanding of PAH deposition and transformation processes. While the focus of this investigation was on PAHs, this technique could be adapted to other problematic compounds targeted for CSIA.</div></div>","PeriodicalId":400,"journal":{"name":"Organic Geochemistry","volume":"203 ","pages":"Article 104966"},"PeriodicalIF":2.6,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143511397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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