宁晋泊晚更新世以来气候变化的正构烷烃分子记录

华北地区晚更新世以来气候变化研究具有重要的意义.选择宁晋泊地区开展河湖相沉积物的分子化石研究.结果表明,沉积物中正构烷烃碳数分布范围为C₁₅~C₃₃,高碳数奇碳优势明显,多以C₂₉和C₃₁为主峰的单峰分布,少量样品出现以C₁₇为次主峰的双峰分布,表明有机质以陆生植物和大型水生植物为主.结合正构烷烃参数,分析了宁晋泊地区晚更新世以来的气候演变过程,展现了"83~68 ka气候较为温和,湖泊水位较低;68~30 ka气候暖湿,湖泊扩张;30~22 ka气候冷干,湖泊萎缩;22~10 ka气候好转,湖泊水位上升;全新世气候温和适度,湖泊水位略有降低"的特征.区域对比分析表明,末次冰期以来宁晋泊地区与延庆盆地等地的气候变化基本一致,具有冰期-间冰期旋回特征,说明其主要受太阳辐射的控制.      

内蒙古磴口河湖相沉积物正构烷烃分布特征及其环境意义

为了探讨季风边缘区气候变化特征,对内蒙古磴口一个深15m 的钻孔沉积物中的正构烷烃进行了分析.结果显示,正 构烷烃总体呈现出以高碳数为主的分布特征,表明其主要来源于陆生高等植物,多数样品以nC27、nC29为主峰,奇碳优势明 显,局部样品以nC25为主峰,显示了流域植被类型为木本植物和少量水生植物.但在钻孔上部短链正构烷烃相对丰度较高,主 要以nC18为主峰,无明显的奇偶优势,反映了低等藻类生物增加.正构烷烃的分布特征在沉积钻孔中表现出的多阶段变化,与 岩性、有机碳同位素等变化相吻合,反映出研究区寒暖交替的气候条件.      

低纬度淡水湖沉积物中正构烷烃氢同位素组成特征及其有机质源和环境指示意义

为认识低纬度亚热带地区湖泊沉积物中正构烷烃氢同位素组成特征及其与母源输入和生态环境的关系,本文利用气相色谱-高温热转变-同位素比值质谱议(GC-TC-IRMS),对系统采集的抚仙湖沉积物样品中正构烷烃氢同位素进行了测定。抚仙湖沉积正构烷烃δD值分布在-219.3‰~-142.5‰之间,样品中平均值为-208.1‰~-154.5‰,并且奇碳数正构烷烃δD值明显地将样品划分为两种类型。类型Ⅰ样品中正构烷烃平均δD值明显地高于类型Ⅱ样品,反映了它们生物源存在明显差别。沉积物与水生植物和陆生植物中正构烷烃氢同位素组成对比结果指示了沉积C_(17)、C_(21)~C_(25)奇碳数正构烷烃来自水生植物,C_(27)和C_(29)奇碳数正构烷烃主要来自木本植物,C31和C33正构烷烃来自水生和陆生草本植物的混合。对比研究结果表明,湖泊地区生态环境是控制湖泊沉积正构烷烃氢同位素组成的重要因素之一,在利用沉积正构烷烃氢同位素研究古水文学特征时,还要考虑研究区古生态环境对沉积正构烷烃氢同位素的影响,并且结合沉积正构烷烃ACL值和Qw值,才能对沉积有机质中正构烷烃氢同位素组成及变化作出合理的解释。     

察尔汗盐湖正构烷烃和单体碳同位素分布特征及其古植被意义

对察尔汗盐湖ISL1A钻孔沉积物样品进行了有机分子地球化学分析, 检测出了丰富的类脂物, 包括正构烷烃、一元正脂肪酸、一元正脂肪醇等, 本文主要讨论正构烷烃类脂物的分布特征。正构烷烃的分布型式表明其来源于低等菌藻类生物和陆生高等植物, 正构烷烃的高碳数部分均有显著的奇偶优势, 高碳数正构烷烃全部以C31 为主峰碳。正构烷烃分布特征表明在110.1~50.1 ka B.P.期间, 察尔汗盐湖地区为草原植被景观。对C27、C29、C31 长链正构烷烃进行了单体碳同位素测定, 利用二元模式估算了C3 和 C4 植物的相对输入贡献, 结果表明, 以C3 植物为主。     

8.0 kaBP以来长江中下游南漪湖沉积记录的正构烷烃及其单体碳同位素组成特征和古气候意义

通过分析长江中下游南漪湖柱状沉积物中正构烷烃分布特征及其单体碳同位素组成,重建了该地区8.0 ka BP以来的植被变化,进而反演古气候变迁;同时与其他地质记录的相关指标进行对比,探讨了长江中下游地区中全新世以来东亚夏季风的变化。8.0~4.8 ka BP,长链正构烷烃nC_(27)–nC_(33)含量占绝对优势,Paq值偏低,正构烷烃以陆生高等植物输入为主;相对较低的nC_(27)/nC_(31)比值及较高的ACL27–33值表明这一阶段以草本植物相对发育;长链正构烷烃δ~(13)C整体偏负(–34.7‰~–32.9‰),C_3植物为主;这一时期气候温暖湿润,是东亚夏季风最强盛时期。4.8~2.4 ka BP,长链正构烷烃nC_(27)–nC_(33)含量降低,Paq值偏高,陆生高等植物对正构烷烃的贡献相对减少;nC_(27)/nC_(31)比值升高,ACL27–33值降低,木本植物占优势,草本植物减少;长链正构烷烃δ13C相对正偏(–33.5‰~–29.1‰),C_4植物有一定的增加,但依然以C_3植物为主;这一时期东亚夏季风减弱,气候朝冷干转变。2.4 ka BP以来,长链正构烷烃nC_(27)–nC33含量升高,Paq值逐渐降低,陆源高等植物的贡献逐渐增加;逐渐降低的nC_(27)/nC_(31)比值以及逐渐升高的ACL27–33值表明草本植物重新占相对发育,木本植物含量逐渐减少;长链正构烷烃δ~(13)C波动剧烈,呈现逐渐偏负的趋势,C_3植物继续占据绝对优势,C_4植物呈现逐渐减少的变化趋势;气候由寒冷干燥逐渐向温暖湿润过度。同时,这一时期各指标呈现剧烈波动的变化趋势,推测可能与长江流域人类活动逐渐增加,显著影响了自然植被变化的过程。这些指标记录的东亚夏季风随着北半球夏季太阳辐射量的减少而持续减弱,同时记录了多次冷暖/干湿交替事件,存在6次冷干事件(夏季风减弱事件),其中5次与Bond et al.提出的北大西洋冰筏漂流事件一一对应。     

银川盆地35.0ka以来古植被演化的类脂分子记录

为了更好地了解干旱-半干旱区的植被类型及其演化规律,利用气相色谱仪对银川盆地冰沟剖面河湖相沉积物中的正构烷烃进行了检测,结果显示其正构烷烃碳数分布范围为C_(15)～C_(34),奇碳优势明显,以C_(29)或C_(31)为主峰的单峰型为主,但少量样品也出现双峰型分布模式。通过对冰沟剖面正构烷烃分布特征、碳优势指数CPI和L/H(∑C_(21-)/∑C_(22+))指标的详细分析,得知其有机质来源以陆生高等植物占主导优势。结合年代数据、有机碳同位素、长链正构烷烃平均链长ACL和C_(33)/(C_(33+)C_(27))值,重建出35. 0ka以来银川盆地植被类型以C_3植物为主,并且C_3和C_4植物的相对比例变化主导受温度制约,而木本和草本植被的演化主要受控于水分条件。     

茶卡盐湖沉积物和周围地区植物中正构烷烃及其氢同位素组成特征

为了认识盐湖典型沉积环境中沉积和生物中正构烷烃及其氢同位素特征,应用GC-MS和GC-TC-IRMS同位素分析技术,首次对茶卡盐湖沉积物和周围地区陆生植物中正构烷烃及其氢同位素进行了测定,研究了正构烷烃及其氢同位素组成.结果表明,茶卡盐湖周围地区植物中正构烷烃呈单峰型分布,主峰碳数为C25和C27;存在强的奇偶优势,并...     

武汉东西湖区第四系钻孔的沉积环境及古气候变化

以武汉市东西湖区第四系沉积物ZK25钻孔为例,通过AMS14C年代测定及其粒度与正构烷烃等环境代用指标分析,初步揭示了该孔第四纪沉积环境及晚更新世以来的古气候变化特征.结果显示,该区早更新世为河流沉积,至晚更新世出现河湖相交替沉积,较为干旱;进入全新世由于降雨增多而沉积了较厚的冲积层,随后变得冷干;全新世中期则变成稳定...     

不同纬度地区植物中正构烷烃及其同位素组成

本文应用GC-MS和GC-TC-IRMS同位素分析技术,对我国北部柴达木盆地花土沟至南部广西南宁5个地区草、芦苇和树叶3类植物中正构烷烃及其碳氢同位素进行了分析.结果显示了不同纬度地区植物中正构烷烃碳数分布在C15～C30之间,呈单峰型分布,主峰碳数为C27、C29和C31;CPI值分布在3.49～17.25之间,平均值是草＜芦苇＜树叶;ACL值为26.24～30.26,平均值是草＞芦苇＞树叶.研究发现,随着植物生长地区纬度的增高和年平均气温的降低,植物中正构烷烃主峰碳数、CPI值、ACL值都降低,并且纬度每增加1.,草、芦苇和树叶中ACL值分别减少0.08、0.22和0.36;气温每增加1℃,草、芦苇和树叶中ACL值分别增加0.04、0.24和0.20.研究样品中C27和C29正构烷烃的δ13C值分布在-25.3‰～-35.5‰之间,草具有相对轻的碳同位素组成;C27和C29正构烷烃碳同位素组成与环境因子(如纬度和温度)之间的相关性,在这次研究中没有观察到.样品中C27和C29正构烷烃δD值分布在-132.1‰～-192.6‰之间,草具有相对轻的氢同位素组成.随着纬度增加和气温降低,草和树叶中C27和C29正构烷烃富集轻同位素.因此,可以应用草、芦苇和树叶中正构烷烃主峰碳数、CPI值和ACL值以及草、树叶中C27、C29正构烷烃δD值指示环境特征.     

青藏高原东北部尕海湖沉积物中正构烷烃及其氢同位素组成与有机质源指示意义

系统采集了位于青藏高原东北部的尕海湖淡水湖泊沉积物,对沉积物中正构烷烃及其氢同位素进行了分析,研究了沉积物中正构烷烃及其氢同位素组成,探讨了它们的来源。研究结果表明,尕海湖沉积物中正构烷烃分布反映了它们来自水生和陆生植物。尕海湖沉积正构烷烃氢同位素组成平均值为-221.9‰~-190.5‰。C_(21)~C_(33)奇碳数正构烷烃δD值明显地将样品划分为两种类型。类型Ⅰ样品的C_(21)~C_(33)奇碳数正构烷烃平均δD值明显地高于类型Ⅱ样品。类型Ⅰ沉积正构烷烃δD值分布特征反映了它们主要来自尕海湖水生植物;类型Ⅱ沉积物中正构烷烃δD值特征指示了它们主要来自研究区陆生草本植物。提出了具有δD值低、丰度高和CPI值低的中等链长正构烷烃起源于改造陆源草本植物的细菌。研究成果证实了沉积正构烷烃δD值可以作为指示有机质源的地球化学指标。     

n-alkane distribution coupled with organic carbon isotope composition in the shell bar section, Qarhan paleolake, Qaidam basin, NE Tibetan Plateau

Lipids extracted from lacustrine deposits in the paleolake Qarhan of the Qaidam basin in the northeastern Tibetan Plateau were determined by conventional gas chromatography-mass spectrometry. Several series of biomarkers were identified, mainly including n-alkanes, n-alkan-2-ones, n-alkanoic acids, branched alkanes, triterpenoids and steroids, indicative of various biogenic contributions. On the basis of cluster analysis, the n-C₁₅, n-C₁₇, n-C₁₉ alkanes were proposed to be derived from algae and/or photosynthetic bacteria, the n-C₂₁, n-C₂₃, n-C₂₅ homologues from aquatic plants, and the n-C₂₉, n-C₃₁ homologues from vascular plants. In contrast, the n-C₂₇ alkane is not categorized in the n-C₂₉ and n-C₃₁ group of alkanes, probably due to more complex origins including both aquatic and vascular plants, and/or differential biodegradation. Stratigraphically, layers-2, 4 and 5 were found to show a close relationship in n-alkane distribution, associated with a positive shift in carbon isotope composition of bulk organic matter (δ¹³C_org), inferring a cold/dry period. Layers-1 and 6 were clustered together in association with a negative δ¹³C_org, excursion, probably indicating a relatively warm/humid climate. The potential coupling between the n-alkane distributions and δ¹³C_org, suggests a consequence of vegetation change in response to climate change, with the late MIS3 being shown to be unstable, thought to be the climatic optimum in the Tibetan Plateau. Our results suggest that the cluster analysis used in this study probably provides an effective and authentic method to investigate the n-alkane distribution in paleolake sediments.     

Carbon isotopic composition of individual n-alkanes in asphaltene pyrolysates of biodegraded crude oils from the Liaohe Basin, China

Biodegraded oils are widely distributed in the Liaohe basin, China. In order to develop effective oil-source correlation tools specifically for the biodegraded oils, carbon isotopic compositions of individual n-alkanes from crude oils and their asphaltene pyrolysates have been determined using the gas chromatography–isotope ratio mass spectrometry technique. No significant fractionation in the stable carbon isotopic ratios of n-alkanes in the pyrolysates of oil asphaltenes was found for anhydrous pyrolysis carried out at temperatures below 340°C. This suggests that the stable carbon isotopic distribution of n-alkanes (particularly in the C₁₆–C₂₉ range) in the asphaltene pyrolysates can be used as a correlation tool for severely biodegraded oils from the Liaohe Basin. Comparison of the n-alkane isotopic compositions of the oils with those of asphaltene pyrolysates shows that this is a viable method for the differentiation of organic facies variation and post-generation alterations.     

Fractionation of hydrogen,oxygen and carbon isotopes in n-alkanes and cellulose of three Sphagnum species

Compound-specific isotope measurements of organic compounds are increasingly important in palaeoclimate reconstruction. Searching for more accurate peat-based palaeoenvironmental proxies, compound-specific fractionation of stable C, H and O isotopes of organic compounds synthesized by Sphagnum were determined in a greenhouse study. Three Sphagnum species were grown under controlled climate conditions. Stable isotope ratios of cellulose, bulk organic matter (OM) and C₂₁–C₂₅ n-alkanes were measured to explore whether fractionation in Sphagnum is species-specific, as a result of either environmental conditions or genetic variation. The oxygen isotopic composition (δ¹⁸O) of cellulose was equal for all species and all treatments. The hydrogen isotopic composition (δD) of the n-alkanes displayed an unexpected variation among the species, with values between −154‰ for Sphagnum rubellum and −184‰ for Sphagnum fallax for the C₂₃ n-alkane, irrespective of groundwater level. The stable carbon isotopic composition (δ¹³C) of the latter also showed a species-specific pattern. The pattern was similar for the carbon isotope fractionation of bulk OM, although the C₂₃ n-alkane was >10‰ more depleted than the bulk OM. The variation in H fractionation may originate in the lipid biosynthesis, whereas C fractionation is also related to humidity conditions. Our findings clearly emphasize the importance of species identification in palaeoclimate studies based on stable isotopes from peat cores.     

Production of n-alkyl lipids in living plants and implications for the geologic past

Leaf waxes (i.e., n-alkyl lipids or n-alkanes) are land-plant biomarkers widely used to reconstruct changes in climate and the carbon isotopic composition of the atmosphere. There is little information available, however, on how the production of leaf waxes by different kinds of plants might influence the abundance and isotopic composition of n-alkanes in sedimentary archives. This lack of information increases uncertainty in interpreting n-alkyl lipid abundance and δ¹³C signals in ancient settings. We provide here n-alkyl abundance distributions and carbon isotope fractionation data for deciduous and evergreen angiosperm and gymnosperm leaves from 46 tree species, representing 24 families. n-Alkane abundances are significantly higher in angiosperms than gymnosperms; many of the gymnosperm species investigated did not produce any n-alkanes. On average, deciduous angiosperms produce 200 times more n-alkanes than deciduous gymnosperms. Although differences between angiosperms and gymnosperms dominate the variance in n-alkane abundance, leaf life-span is also important, with higher n-alkane abundances in longer-lived leaves. n-Alkanol abundances covary with n-alkanes, but n-alkanoic acids have similar abundances across all plant groups. Isotopic fractionation between leaf tissue and individual alkanes (ε_lipid) varies by as much as 10‰ among different chain lengths. Overall, ε_lipid values are slightly lower (−4.5‰) for angiosperm than for gymnosperm (−2.5‰) n-alkanes. Angiosperms commonly express slightly higher Δ_leaf (photosynthetic discrimination) relative to gymnosperms under similar growth conditions. As a result, angiosperm n-alkanes are expected to be generally 3-5‰ more depleted in ¹³C relative to gymnosperm alkanes for the same locality. Differences in n-alkane production indicate the biomarker record will largely (but not exclusively) reflect angiosperms if both groups were present, and also that evergreen plants will likely be overrepresented compared with deciduous ones. We apply our modern lipid abundance patterns and ε_lipid results to constrain the magnitude of the carbon isotope excursion (CIE) at the onset of the Paleocene-Eocene Thermal Maximum (55.8 Ma). When Bighorn Basin (WY) sediment n-alkanes are interpreted in context of floral changes and modern n-alkane production estimates for angiosperms and gymnosperms, the CIE is greater in magnitude (−5.6‰) by ∼1‰ compared to previous estimates that do not take into account n-alkane production.     

Experimental investigation of the compositional variation of acyclic paraffins during expulsion from source rocks

Anhydrous non-isothermal heating experiments were conducted under controlled compressive stress on cylindrical plugs of six oil shales from Permian through Eocene age. The objective of this study was to compare the distribution of acyclic paraffins in initial, residual and expelled organic matter and to highlight causes of compositional differences resulting from expulsion. Pristane generation from kerogen is highest in the Eocene Messel shale and affects the pristane / phytane (pr / ph) ratio commonly used as a redox proxy. The isoprenoid to n-alkane ratios (pr / n-C₁₇, ph / n-C₁₈) decrease during generation and are lowest in the residual bitumen due to preferential generation and retention of n-alkanes. The n-alkane distribution shows that only lacustrine shales produce high wax oils. Evaporative fractionation leads to loss of n-alkanes up to n-C₂₀ with boiling points below 350 °C. This demonstrates that lacustrine and marine shales may lead to accumulation of low wax oils due to evaporative fractionation after expulsion.     

Abundance and distribution of leaf wax n-alkanes in leaves of Acacia and Eucalyptus trees along a strong humidity gradient in northern Australia

Environmental parameters such as rainfall, temperature and relative humidity can affect the composition of higher plant leaf wax. The abundance and distribution of leaf wax biomarkers, such as long chain n-alkanes, in sedimentary archives have therefore been proposed as proxies reflecting climate change. However, a robust palaeoclimatic interpretation requires a thorough understanding of how environmental changes affect leaf wax n-alkane distributions in living plants. We have analysed the concentration and chain length distribution of leaf wax n-alkanes in Acacia and Eucalyptus species along a 1500 km climatic gradient in northern Australia that ranges from subtropical to arid. We show that aridity affected the concentration and distribution of n-alkanes for plants in both genera. For both Acacia and Eucalyptus n-alkane concentration increased by a factor of ten to the dry centre of Australia, reflecting the purpose of the wax in preventing water loss from the leaf. Furthermore, Acacian-alkanes decreased in average chain length (ACL) towards the arid centre of Australia, whereas Eucalyptus ACL increased under arid conditions. Our observations demonstrate that n-alkane concentration and distribution in leaf wax are sensitive to hydroclimatic conditions. These parameters could therefore potentially be employed in palaeorecords to estimate past environmental change. However, our finding of a distinct response of n-alkane ACL values to hydrological changes in different taxa also implies that the often assumed increase in ACL under drier conditions is not a robust feature for all plant species and genera and as such additional information about the prevalent vegetation are required when ACL values are used as a palaeoclimate proxy.     

柴达木盆地第四纪古气候变化在物理测井自然伽玛曲线上的记录

利用物理测井曲线分析古气候变化，是近年发展起来的新领域。本文在对取芯井涩中6井多种气候指标分析的基础上，建立了涩中6井GR曲线古气候反演模式，将该模式引进到盆地东部唯一贯穿第四纪的钻孔---达参1井，利用该井高分辨率自然伽玛曲线建立了盆地东部地区2.85Ma以来的时间标尺，据此讨论盆地东部地区2.85Ma以来的古气候变化，表明盆地气候变化在大阶段上明显受到天文轨道周期的控制，但也具有明显的区域性特征。此外还与盆地西部大浪滩ZK-336孔进行了对比。表明柴达木盆地同时包含了高原隆升与全球性气候变化的信息，是古环境变迁的良好的信息载体。也证明了自然伽玛曲线是反映内陆干旱盆地气候与环境变化良好的代用指标。     

Possible ecological and environmental significance of the predominance of even-carbon number C20-C30n-alkanes

Even-carbon number C₂₂-C₂₈n-alkanes, are present in higher concentrations than their C₂₁-C₂₉ odd-carbon number homologs in an organic-rich rock of Mississippian (ca. 310 × 10⁶-yr-old) age, which contains algae-like remnants. Environmental indicators associated with this organic-rich rock permitted environmental comparison with ancient and modern environments that contain n-alkanes which exhibit similar distributions. The results of these comparisons suggest that even-carbon number n-alkanes are preferentially produced in highly saline, carbonate environments where aerobic and anaerobic bacteria have subsisted on the remains of blue-green algae.     

Distribution of n-alkanes in lacustrine sediments from subtropical lake in Brazil

The geochemical composition of lake bed sediments of a tropical reservoir in Brazil have been investigated. The C, N, P composition showed almost no variation between the different sampling points. All samples contained inorganic phosphorus (IP) ranging from 52 to 70%. The Redfield ratios show that the lake is without significant anthropogenic inputs. Most of the organic matter is composed by higher plants decomposition revealed in the total organic carbon (TOC):nitrogen (N) ratio ranging from 15.4 to 57.2. Also, TOC:organic phosphorus (OP) ranged from 265.3 to 933.6, suggesting that most of the organic matter has terrestrial origin from wood plants. The ratios suggest that most organic matter is influenced by the terrestrial characteristics of the watershed. Furthermore, the relative abundance of n-alkane homologues in the sediments was investigated. All samples have been analyzed for the n-alkanes C₈ to C₄₀. The sediments were dominated by n-alkanes C₂₅–C₃₈. It is concluded that n-alkane in sediments mainly come from terrestrial plants, however there is a contribution of submerged aquatic plants, especially in those sites in deeper areas of the lake. On the basis of P_aq index the n-alkanes in sediments comes from terrestrial plants, however there is a contribution from emerged/floating plants.The investigated lake seems to be considered as meso to eutrophic. Because of the relatively high primary productivity in the lakes, there is a substantial organic-matter flux to the sediments, which rapidly becomes anoxic. According to the pristine/phytane ratio the sediments represent an anoxic environment with values found between 0.38 and 1.72.     

Composition of organic matter in subducted and unsubducted sediments off the Nicoya peninsula, Costa Rica (ODP Leg 170, Sites 1039 and 1040)

Investigation of sediment samples from Sites 1039 and 1040 (ODP Leg 170) drilled off the Nicoya peninsula (Costa Rica) by organic geochemical and organic petrological methods has revealed that subduction has only little influence on the composition of the sedimentary organic matter. Organic carbon contents reached 1.5% in the Pleistocene samples but Miocene and Pliocene sediments had an average organic carbon content of less than 0.5%. Organic carbon/sulfur ratios are generally below 2.8, reflecting an intense sulfate reduction in the uppermost sediments which was enhanced by sulfate supply both from sea water and deeper strata. Microscopical examinations indicate that the organic matter is mainly derived from marine sources. A small amount of terrigenous organic matter is, however, present as well according to n-alkane and fatty acid distributions. The alkenone unsaturation index U₃₇^k′ shows only a slight decrease during the Miocene and Pliocene, and stronger variations in the Pleistocene, probably indicating more stable sea surface temperatures during the Miocene and Pliocene. Variations in the Pleistocene can possibly be related to glacial/interglacial changes.