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浙江南部近海沉积物柱状样中脂类生物标志物的组成及形态分布
引用本文:尚文郁, 孙静轶, 谢曼曼, 岑况, 蔡泽, 战楠, 凌媛, 孙青. 基于Py-GC/MS的沙漠湖泊直链脂肪族化合物分析及古气候应用初探[J]. 岩矿测试, 2022, 41(5): 836-848. DOI: 10.15898/j.cnki.11-2131/td.202201120009
作者姓名:尚文郁  孙静轶  谢曼曼  岑况  蔡泽  战楠  凌媛  孙青
作者单位:1.自然资源部生态地球化学重点实验室,国家地质实验测试中心,北京 100037;2.中国地质大学(北京)地球科学与资源学院,北京 100083;3.淮南师范学院,安徽 淮南 232038;4.中国地质科学院地质研究所,北京 100037
基金项目:国家自然科学基金面上项目“末次冰盛期以来中—缅热带玛珥湖古温度重建”(41877301);国家自然科学基金项目青年基金项目“基于红外光谱的金川泥炭中有机碳、腐殖酸、木质素等古气候替代指标快速分析方法及在古气候研究中的应用”(41402325);中国地质科学院基本科研业务费项目“湖泊沉积物中记录区域健康风险评价的生态环境指标ACL的研究”(CSJ-2021-09)
摘    要:

湖泊沉积物中直链脂肪族化合物(MCCs)对气候变化响应敏感,环境条件的变化可促使MCCs在游离态和结合态间发生转化,是古气候重建的重要生物标志物。以往研究中对样品前处理通常采用混合溶剂提取法得到MCCs游离态组分,而以化学键合、物理吸附等形式赋存的结合态组分无法通过溶剂提取,不能获取结合态组分特征对气候环境变化的指示信息。本文将热裂解这一有机质高效分解技术与气相色谱-质谱(GC-MS)联用,实现了对内蒙古伊和沙日乌苏湖泊沉积物有机质组成的精细刻画,并识别、分析了共计3类、71项结合态MCCs化合物。结果表明:热解温度是影响热裂解-气相色谱-质谱(Py-GC/MS)分析沉积物样品中结合态MCCs分布特征的主要因素,450℃以下热解能量较低导致结合态MCCs解析不充分,550℃和650℃下各类结合态MCCs(含正构烷烃、正构烯烃及α-正构脂肪酮)充分解析,可经GC-MS实现在线分离、识别;随着热解温度升高,裂解产物中MCCs平均链长趋于降低,过高的裂解能量影响了产物中MCCs化合物链长特征对气候变化指示的敏感性。经研究各类MCCs分布特征发现,550℃下正构烷烃平均链长特征与传统气候替代指标游离态正构烷烃单体碳同位素δ13C27~33具有较好的相关性(R=0.83)。结合态正构烷烃ACL25~31指标响应了区域有效降水变化特征,识别了区域内5.6ka、3.9ka前后的干旱期,反映了东亚夏季风强度变化,对应了北半球中纬度有效降水变化。



关 键 词:热裂解-气相色谱-质谱法(Py-GC/MS)  伊和沙日乌苏湖  结合态直链脂肪族化合物  古气候
收稿时间:2022-01-12
修稿时间:2022-04-29

The potential of biomarker proxies to trace climate,vegetation, and biogeochemical processes in peat: A review
SHANG Wenyu, SUN Jingyi, XIE Manman, CEN Kuang, CAI Ze, ZHAN Nan, LING Yuan, SUN Qing. Py-GC/MS Analysis Method for Aliphatic Biomarker in Desert Lake Sediment and Its Application in Paleoclimatic Study[J]. Rock and Mineral Analysis, 2022, 41(5): 836-848. DOI: 10.15898/j.cnki.11-2131/td.202201120009
Authors:SHANG Wenyu  SUN Jingyi  XIE Manman  CEN Kuang  CAI Ze  ZHAN Nan  LING Yuan  SUN Qing
Affiliation:1.Key Laboratory of Eco-Geochemistry, Ministry of Natural Resources; National Research Center for Geoanalysis, Beijing 100037, China;2.School of Earth Sciences and Resources, China University of Geosciences (Beijing), Beijing 100083, China;3.Huainan Normal University, Huainan 232038, China;4.Institute of Geology, Chinese Academy of Geological Sciences, Beijing 100037, China
Abstract:BACKGROUNDMethylene chain backbone compounds (MCCs) in lake sediments are sensitive to climate change, and changes in environmental conditions could promote the transformation of MCCs lipids between free and bound states, hence providing a series of biomarkers for paleoclimate reconstruction. In previous studies, free MCCs lipids were typically extracted by mixed solvents, bound MCCs lipids with chemical bonding or physical adsorption could not be obtained by organic solvent extraction, and the indicator information of the characteristics of bound components on paleoclimate change was missing.OBJECTIVESTo study the suitable analytical conditions for bound MCCs lipids, and establish proxy based on bound MCCs lipids to provide an effective tool for paleoclimate reconstruction of terrestrial ecosystems.METHODSOptimized analytical method of pyrolysis gas chromatography-mass spectrometry (Py-GC/MS) was established and used to evaluate the bound MCCs in typical Desert Lake sediment.RESULTSTotal of 71 bound MCCs compounds were identified and analyzed based on fine characterization of organic matter composition in the sediments of the Yiheshariwusu Lake in Inner Mongolia. Pyrolysis temperature was the main factor affecting the distribution characteristics of bound MCCs in sediment. Low pyrolysis energy under 450℃ led to insufficient resolution of bound MCCs. At 550℃ and 650℃, total bound n-alkanes, n-alkenes, and n-alkan-2-ones were on-line separated, identified and analyzed. The average chain length characteristics of bound n-alkanes at 550℃ and the carbon isotope of free n-alkanes as a traditional climate substitute index δ13C27-33 had the best correlation (R=0.83, n=11, p < 0.01).CONCLUSIONSProxy ACL25-31 of bound n-alkanes respond to the change characteristics of regional effective precipitation, identify the drought periods around 5.6ka and 3.9ka in the region, reflect the intensity change of East Asian summer monsoon, and correspond to the change of effective precipitation in the mid-latitude of the northern hemisphere.
Keywords:pyrolysis gas chromatography-mass spectrometry (Py-GC/MS)  Yiheshariwusu Lake  bound methylene chain backbone compounds lipid  paleoclimate
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