黄土高原晚中新世—上新世红粘土碳酸盐地球化学研究
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摘要
上新世暖期(5-3Ma)是与当代全球变暖最为相似的类比期。这一时期同工业革命前相比,全球气温高2.5℃,大气二氧化碳浓度高35%,北半球大规模冰川缺失,海平面上升。太平洋地区的表层海水温度上升,在东西和南北两个方向上温度差缩小。由低纬度海洋向中纬度内陆地区输送暖湿气流的信风系统减弱。这些气候特征与当代“厄尔尼诺”现象相似。据现代气象观测,“厄尔尼诺”会给我国北方带来干旱天气。然而上新世暖期的气候是否会长期处于“厄尔尼诺”状态之下,有没有给我国北方地区带来持续性的干旱,目前存有很大争议。
黄土高原的红粘土风成序列为研究这一时期的我国北方的气候特点提供了最佳的材料。为了恢复红粘土发育时期的气候特点,研究人员围绕气候代用指标展开了一系列研究工作,取得了丰硕的成果。这些代用指标包括蜗牛化石记录、植物孢粉记录、磁化率、粒度、铁矿物、碳酸盐矿物含量、碳氧同位素等。然而使用已有的气候代用指标获得的古气候信息之间缺乏一致。上新世的气候特征仍然颇具争议,争议的焦点在于上新世东亚季风是否存在、黄土高原的气候是否更加干燥、黄土高原的植被分布特征与现代是否相似。
为了回答这些问题,本文以气候变化敏感矿物——碳酸盐为切入点,在野外地质考察的基础上,对六盘山以东地区自南向北四条红粘土剖面(段家坡、灵台、巴家嘴和佳县)展开地球化学研究。围绕红粘土碳酸盐矿物已开展的研究工作存在如下问题或不足：1)对于不同的碳酸盐矿物种类未作区分；2)缺少不同种类的碳酸盐矿物的地球化学特征；3)对不同类型的碳酸盐矿物的时空分布特点缺乏了解；4)成壤碳酸盐碳同位素的解释存在争议；5)成壤碳酸盐氧同位素的研究整体上较为薄弱。针对以上问题,本文采用X射线衍射、漫反射红外光谱(FTIR)、场发射扫描电镜(FE-SEM)和稳定同位素质谱仪(MAT)等手段,研究了各剖面中碳酸盐的矿物学特征、成因,建立碳酸盐矿物的定量分析方法,阐明了各剖面中碳酸盐矿物(原白云石、方解石)的含量、碳氧同位素变化规律与分布。在此基础上,进一步探讨了成壤碳酸盐的种类和含量变化与季风的关系；恢复了上新世古生态；揭示了红粘土成壤碳酸盐氧同位素与全球气候变化的联系。
论文的原创性成果包括以下四个方面：
1)发现红粘土存在着次生成因的原白云石(高钙白云石)。本文使用红外光谱方法(FTIR)鉴定和定量了红粘土原白云石和共生方解石,获得了自南向北四条红粘土剖面的原白云石和方解石矿物含量。发现随着地层由老到新,原白云石含量和出现频率在四条红粘土剖面一致呈现出降低的趋势。在空间上,段家坡和巴家嘴红粘土原白云石含量较高,平均值分别达到了6.0%和3.6%；灵台和佳县剖面原白云石含量较低,平均值只有1.6%和1.7%。
2)红粘土原白云石的碳氧同位素偏负,指示了陆相“淡水”成因和大气降水的参与。微形貌观察显示红粘土原白云石由直径为1-20μm的自生微晶体构成,具有菱面体结构,生长在土壤孔隙中与自生方解石共生。这表明原白云石原位生长,是在成壤过程中自生形成的。论文提出较高的Mg2+/Ca2+比值和较为温暖、干旱的气候条件是形成原白云石的必要条件;红粘土原白云石对上新世较温暖和干旱的气候条件具有重要的指示意义。
3)发现红粘土沉积序列存在着碳酸盐淋滤-淀积旋回,基本与深海氧同位素轨道尺度旋回吻合。其中淋滤层碳酸盐含量低,磁化率高,Rb/Sr比值高,Zr/Rb比值低；而淀积层碳酸盐含量高,磁化率低,Rb/Sr比值低,Zr/Rb比值高；与上覆第四纪黄土-古土壤旋回相类似。确立了8-3Ma期间至少存在七次重大环境事件,为青藏高原隆升和全球变化的区域响应研究提供了新的证据。此外,研究发现上新世暖期(5-3Ma B.P.)存在类似于第四纪的季风旋回,结论并不支持上新世暖期“永久性厄尔尼诺”假说。
4)发现了红粘土钙结核碳同位素自南向北逐渐偏正,并揭示了在6.7-6.4Ma和～3.6Ma两次重要的C4植被扩张事件,很可能与干旱化加剧有关。据红粘土钙结核氧同位素时间序列变化特点,确定了晚中新世以来三个重要演化阶段。发现6.1-3.6Ma,钙结核氧同位素逐渐偏正；-3.6Ma之后,偏正的趋势加剧。钙结核氧同位素值逐步偏正与深海氧同位素由轻变重的趋势一致,很可能与全球变冷过程和中国西部内陆干旱化的加强有关。
The Pliocene Warming Period (PWP) is often considered the closest analog of modern global warming. Comparing with the pre-industrial conditions, mean annual temperature was2.5℃higher, with the atmospheric concentration of CO2between300-400ppm. During the PWP, higher latitudes were warmer, the ice cap was largely absent from Northern Hemisphere, and the sea level was higher. The Pacific climate was also quite different. The surface sea temperature (SST) of Pacific increased and the SST gradient between the equatorial Pacific was very small. The Northern Hemisphere atmospheric circulations show a robust response to meridional SST gradient changes. The reduced SST gradient widens the Intertropical Convergence Zone (ITCZ) and decreases precipitation amount at the western coast of Pacific. These Pliocene climate conditions were often called "permanent El Nino". Under modern El Nino-like climate, the landfalls will decrease in North China. However, there is still considerable debate over the characteristics of El Nino/southern oscillation (ENSO) during PWP. The opposing evidence suggests that a La Nina-like state was dominant during PWP. During a modern La Nina event, monsoonal rainfall will be enhanced in North China.
The Red Clay Formation, which underlies the well-known Quaternary loess sequence, extends the eolian deposits from2.6Ma through the late Miocene making it a good archive to reconstruct Pliocene climate in North China. Paleoecological analysis of terrestrial snail communities from the Red Clay and pollen assemblages indicates the existence of monsoonal precipitation. However, the temporal sampling resolution in these studies is low and detailed information of EAM variability remains poorly understood. The Pliocene climate pattern was rather controversial and focused on the state of East Asian monsoon (EAM).
The goal of this study is to explore the evolution of EAM during the Pliocene. To accomplish this goal, we studied the carbonate minerals formed in the warmer Pliocene epoch, as carbonate minerals have been suggested as potential paleoclimate proxies in Pleistocene loess-paleosol sequence. However, little work has been done on the carbonates from the underlying Red Clay. Few attempts have been made to determine Red Clay carbonate genesis or distinguish differences between carbonate species. As a result, the lack of information about the relative abundance of different carbonate mineral species in the Red Clay is a potential hindrance to paleoclimate reconstructions. We studied four continuous sections (Duanjiapo, Lingtai, Bajiazui and Jiaxian) of the Red Clay Formation on the Chinese Loess Plateau (CLP) by X-ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM) and Stable Isotope Mass Spectrometry. The fundermantal objective of these studies is to clarify Pliocene paleoclimate state by relative abundances, micro-morphology, stable isotope compositions of primary pedogenic protodolomite and calcite from four typical Red Clay sequences.
The summary of innovations in this study was listed as follows including four aspects.
1) Red Clay on CLP shows diagnostic FTIR absorption features of calcite and protodolomite, which allowed the two carbonate minerals to be identified and quantified using the FTIR method. Linear regression of the713cm-1and728cm-1absorption band area versus calcite and dolomite concentration, respectively, produces regression equations with R2's of0.92and0.96. The protodolomite and calcite minerals contents were acquired for the four studies Red Clay sections. In all the four sections, protodolomite concentrations and the frequency of occurrence increase downward.
2) SEM observations indicate that Red Clay protodolomite is composed of euhedral rhombic crystals coexisting with calcite and palygorskite. The crystals vary from1-20μm and grow into the soil voids, implying that the protodolomite is authigenic. The depletion of δ18O further indicates that this protodolomite formed in a fresh water environment. The above results demonstrate that the protodolomite originated from pedogenesis. Dolomitization in the Red Clay sequence appears to be the result of overcoming kinetic barriers. A high pore water Mg/Ca ratio is the critical kinetic factor controlling Red Clay dolomitization. Warm and seasonal dry conditions lead to the formation of protodolomite. Protodolomite is indicative for the warm and dry climate during Pliocene.
3) Red Clay Formation contains the leached and calcareous horizons. Their carbonate content varies with high frequency and large amplitude. High MS values, Rb/Sr ratios and lower Zr/Rb ratios are found in the leached horizons, whereas low MS values, Rb/Sr ratios and higher Zr/Rb ratios are found in the calcareous horizons. These variations are comparable with those observed in the overlying paleosol-loess sequence. Seven highly leached horizons, whose carbonate content is near zero, reflect climate intervals dominated by large climate events. They were in phase with the deep sea δ18O isotope fluctuations, indicating a close connection with global climate change. At least two strong leaching/carbonate accumulation cycles occurred during the PWP (5-3Ma). The dramatic differences in the precipitation suggested by these cycles do not appear to support the hypothesis that past and future warmer climate would lead to a permanent El Nino-like climate.
4) The carbon isotopes of carbonate nodules in Red Clay show a northward positive gradient on CLP, revealing that the abundance of C4plants was in proportion with aridity. C4plants greatly expanded in two intervals from6.7-6.4Ma and at～3.6Ma on CLP. The second C4expansion interval is in phase with the increasing dust deposition rate in North Pacific, suggesting that the drying of Asian interior may have triggered the C4plants expansion. Three important climate evolution stages were revealed from the oxygen isotopes of carbonate nodules in Red Clay. Between6.1-3.6Ma, oxygen isotopes of carbonate nodules gradually increased and after～3.6Ma, the increasing trend was even more evident. The enhancement of oxygen isotopes from carbonate nodules correlated with deep sea oxygen isotopes, indicating a close dependence on global temperatures.
黄土高原的红粘土风成序列为研究这一时期的我国北方的气候特点提供了最佳的材料。为了恢复红粘土发育时期的气候特点,研究人员围绕气候代用指标展开了一系列研究工作,取得了丰硕的成果。这些代用指标包括蜗牛化石记录、植物孢粉记录、磁化率、粒度、铁矿物、碳酸盐矿物含量、碳氧同位素等。然而使用已有的气候代用指标获得的古气候信息之间缺乏一致。上新世的气候特征仍然颇具争议,争议的焦点在于上新世东亚季风是否存在、黄土高原的气候是否更加干燥、黄土高原的植被分布特征与现代是否相似。
为了回答这些问题,本文以气候变化敏感矿物——碳酸盐为切入点,在野外地质考察的基础上,对六盘山以东地区自南向北四条红粘土剖面(段家坡、灵台、巴家嘴和佳县)展开地球化学研究。围绕红粘土碳酸盐矿物已开展的研究工作存在如下问题或不足：1)对于不同的碳酸盐矿物种类未作区分；2)缺少不同种类的碳酸盐矿物的地球化学特征；3)对不同类型的碳酸盐矿物的时空分布特点缺乏了解；4)成壤碳酸盐碳同位素的解释存在争议；5)成壤碳酸盐氧同位素的研究整体上较为薄弱。针对以上问题,本文采用X射线衍射、漫反射红外光谱(FTIR)、场发射扫描电镜(FE-SEM)和稳定同位素质谱仪(MAT)等手段,研究了各剖面中碳酸盐的矿物学特征、成因,建立碳酸盐矿物的定量分析方法,阐明了各剖面中碳酸盐矿物(原白云石、方解石)的含量、碳氧同位素变化规律与分布。在此基础上,进一步探讨了成壤碳酸盐的种类和含量变化与季风的关系；恢复了上新世古生态；揭示了红粘土成壤碳酸盐氧同位素与全球气候变化的联系。
论文的原创性成果包括以下四个方面：
1)发现红粘土存在着次生成因的原白云石(高钙白云石)。本文使用红外光谱方法(FTIR)鉴定和定量了红粘土原白云石和共生方解石,获得了自南向北四条红粘土剖面的原白云石和方解石矿物含量。发现随着地层由老到新,原白云石含量和出现频率在四条红粘土剖面一致呈现出降低的趋势。在空间上,段家坡和巴家嘴红粘土原白云石含量较高,平均值分别达到了6.0%和3.6%；灵台和佳县剖面原白云石含量较低,平均值只有1.6%和1.7%。
2)红粘土原白云石的碳氧同位素偏负,指示了陆相“淡水”成因和大气降水的参与。微形貌观察显示红粘土原白云石由直径为1-20μm的自生微晶体构成,具有菱面体结构,生长在土壤孔隙中与自生方解石共生。这表明原白云石原位生长,是在成壤过程中自生形成的。论文提出较高的Mg2+/Ca2+比值和较为温暖、干旱的气候条件是形成原白云石的必要条件;红粘土原白云石对上新世较温暖和干旱的气候条件具有重要的指示意义。
3)发现红粘土沉积序列存在着碳酸盐淋滤-淀积旋回,基本与深海氧同位素轨道尺度旋回吻合。其中淋滤层碳酸盐含量低,磁化率高,Rb/Sr比值高,Zr/Rb比值低；而淀积层碳酸盐含量高,磁化率低,Rb/Sr比值低,Zr/Rb比值高；与上覆第四纪黄土-古土壤旋回相类似。确立了8-3Ma期间至少存在七次重大环境事件,为青藏高原隆升和全球变化的区域响应研究提供了新的证据。此外,研究发现上新世暖期(5-3Ma B.P.)存在类似于第四纪的季风旋回,结论并不支持上新世暖期“永久性厄尔尼诺”假说。
4)发现了红粘土钙结核碳同位素自南向北逐渐偏正,并揭示了在6.7-6.4Ma和～3.6Ma两次重要的C4植被扩张事件,很可能与干旱化加剧有关。据红粘土钙结核氧同位素时间序列变化特点,确定了晚中新世以来三个重要演化阶段。发现6.1-3.6Ma,钙结核氧同位素逐渐偏正；-3.6Ma之后,偏正的趋势加剧。钙结核氧同位素值逐步偏正与深海氧同位素由轻变重的趋势一致,很可能与全球变冷过程和中国西部内陆干旱化的加强有关。
The Pliocene Warming Period (PWP) is often considered the closest analog of modern global warming. Comparing with the pre-industrial conditions, mean annual temperature was2.5℃higher, with the atmospheric concentration of CO2between300-400ppm. During the PWP, higher latitudes were warmer, the ice cap was largely absent from Northern Hemisphere, and the sea level was higher. The Pacific climate was also quite different. The surface sea temperature (SST) of Pacific increased and the SST gradient between the equatorial Pacific was very small. The Northern Hemisphere atmospheric circulations show a robust response to meridional SST gradient changes. The reduced SST gradient widens the Intertropical Convergence Zone (ITCZ) and decreases precipitation amount at the western coast of Pacific. These Pliocene climate conditions were often called "permanent El Nino". Under modern El Nino-like climate, the landfalls will decrease in North China. However, there is still considerable debate over the characteristics of El Nino/southern oscillation (ENSO) during PWP. The opposing evidence suggests that a La Nina-like state was dominant during PWP. During a modern La Nina event, monsoonal rainfall will be enhanced in North China.
The Red Clay Formation, which underlies the well-known Quaternary loess sequence, extends the eolian deposits from2.6Ma through the late Miocene making it a good archive to reconstruct Pliocene climate in North China. Paleoecological analysis of terrestrial snail communities from the Red Clay and pollen assemblages indicates the existence of monsoonal precipitation. However, the temporal sampling resolution in these studies is low and detailed information of EAM variability remains poorly understood. The Pliocene climate pattern was rather controversial and focused on the state of East Asian monsoon (EAM).
The goal of this study is to explore the evolution of EAM during the Pliocene. To accomplish this goal, we studied the carbonate minerals formed in the warmer Pliocene epoch, as carbonate minerals have been suggested as potential paleoclimate proxies in Pleistocene loess-paleosol sequence. However, little work has been done on the carbonates from the underlying Red Clay. Few attempts have been made to determine Red Clay carbonate genesis or distinguish differences between carbonate species. As a result, the lack of information about the relative abundance of different carbonate mineral species in the Red Clay is a potential hindrance to paleoclimate reconstructions. We studied four continuous sections (Duanjiapo, Lingtai, Bajiazui and Jiaxian) of the Red Clay Formation on the Chinese Loess Plateau (CLP) by X-ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM) and Stable Isotope Mass Spectrometry. The fundermantal objective of these studies is to clarify Pliocene paleoclimate state by relative abundances, micro-morphology, stable isotope compositions of primary pedogenic protodolomite and calcite from four typical Red Clay sequences.
The summary of innovations in this study was listed as follows including four aspects.
1) Red Clay on CLP shows diagnostic FTIR absorption features of calcite and protodolomite, which allowed the two carbonate minerals to be identified and quantified using the FTIR method. Linear regression of the713cm-1and728cm-1absorption band area versus calcite and dolomite concentration, respectively, produces regression equations with R2's of0.92and0.96. The protodolomite and calcite minerals contents were acquired for the four studies Red Clay sections. In all the four sections, protodolomite concentrations and the frequency of occurrence increase downward.
2) SEM observations indicate that Red Clay protodolomite is composed of euhedral rhombic crystals coexisting with calcite and palygorskite. The crystals vary from1-20μm and grow into the soil voids, implying that the protodolomite is authigenic. The depletion of δ18O further indicates that this protodolomite formed in a fresh water environment. The above results demonstrate that the protodolomite originated from pedogenesis. Dolomitization in the Red Clay sequence appears to be the result of overcoming kinetic barriers. A high pore water Mg/Ca ratio is the critical kinetic factor controlling Red Clay dolomitization. Warm and seasonal dry conditions lead to the formation of protodolomite. Protodolomite is indicative for the warm and dry climate during Pliocene.
3) Red Clay Formation contains the leached and calcareous horizons. Their carbonate content varies with high frequency and large amplitude. High MS values, Rb/Sr ratios and lower Zr/Rb ratios are found in the leached horizons, whereas low MS values, Rb/Sr ratios and higher Zr/Rb ratios are found in the calcareous horizons. These variations are comparable with those observed in the overlying paleosol-loess sequence. Seven highly leached horizons, whose carbonate content is near zero, reflect climate intervals dominated by large climate events. They were in phase with the deep sea δ18O isotope fluctuations, indicating a close connection with global climate change. At least two strong leaching/carbonate accumulation cycles occurred during the PWP (5-3Ma). The dramatic differences in the precipitation suggested by these cycles do not appear to support the hypothesis that past and future warmer climate would lead to a permanent El Nino-like climate.
4) The carbon isotopes of carbonate nodules in Red Clay show a northward positive gradient on CLP, revealing that the abundance of C4plants was in proportion with aridity. C4plants greatly expanded in two intervals from6.7-6.4Ma and at～3.6Ma on CLP. The second C4expansion interval is in phase with the increasing dust deposition rate in North Pacific, suggesting that the drying of Asian interior may have triggered the C4plants expansion. Three important climate evolution stages were revealed from the oxygen isotopes of carbonate nodules in Red Clay. Between6.1-3.6Ma, oxygen isotopes of carbonate nodules gradually increased and after～3.6Ma, the increasing trend was even more evident. The enhancement of oxygen isotopes from carbonate nodules correlated with deep sea oxygen isotopes, indicating a close dependence on global temperatures.
引文
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