深时镁同位素风化指标的验证与新解释

沉积岩碎屑组分镁同位素被广泛应用于恢复深时大陆风化强度.现有深时镁同位素风化指标基于风化残余物镁同位素随化学风化强度提高的一阶段风化模式.但是,近期实验与现代风化剖面研究发现了优先利用轻镁同位素的次生黏土矿物,挑战了深时镁同位素指标的理论基础.本研究测试了华南地区晚古生代沉积岩与中国南海沉积物样品的矿物、元素与镁同位素组成.通过对比深时镁同位素风化指标与化学蚀变指数(CIA)、镁损失量和矿物组成等风化指标来验证深时镁同位素风化指标.结果表明,在较高风化强度下镁同位素随风化强度提高而降低,而在较低风化强度下镁同位素随风化强度的提高而增加.该结果表明在不同风化强度下存在不同的镁同位素行为,以往的一阶段镁同位素风化模式无法准确追踪大陆风化强度的变化.结合深时样品数据、现今风化剖面与实验研究,我们建立了三阶段的镁含量-镁同位素风化模型.在风化初期,原生矿物的溶解与次生黏土矿物的形成造成镁含量的快速降低与镁同位素轻微提高.转换阶段土壤底层绿泥石、蛭石等富镁黏土矿物大量生成造成镁含量和镁同位素的跃升.在进阶风化阶段中,具有较重镁同位素的富镁黏土矿物优先风化,造成镁含量与镁同位素的同步降低.     

陕西洛川黄土化学风化程度的地球化学研究

通过对陕西洛川黄土-古土壤剖面中常量元素、微量元素和REE的分析,采用以Al为标准的变化率参数计算方法对黄土高原化学风化程度进行了初步研究.结果表明在风化成壤过程中,黄土中绝大多数元素都保持稳定,活动性元素仅有Ca,Sr,P,Mg和Na;化学风化处在去Ca,Na风化阶段;化学风化的主要方式是碳酸盐溶解.黄土弱化学风化特征是黄土高原第四纪以来长期受干冷型气候控制的反映.     

CO2浓度升高对浮游藻类元素化学计量值的影响

通过梅梁湾和东太湖的四季原位实验,研究CO_2浓度升高对不同营养水平淡水生态系统中浮游藻类C、N、P元素计量值的影响.实验设置了270、380和750 ppm共3个CO_2浓度,分别代表工业革命前、当前和IPCC预测的21世纪末的CO_2浓度.结果表明梅梁湾水体营养盐浓度在四季均高于东太湖水体营养盐浓度,但梅梁湾原位实验中浮游藻类C、N、P含量却普遍低于东太湖原位实验中浮游藻类营养元素含量,并且前者在季节上变化更大.CO_2浓度升高使梅梁湾原位实验中浮游藻类C∶P比明显增加,N∶P比略有增加,这种增加归因于藻细胞内C、N含量的升高,而东太湖浮游藻类化学计量值对CO_2浓度变化的响应不显著.因此浮游藻类元素化学计量值对CO_2浓度变化的响应程度与水体营养盐的绝对浓度无关,而与浮游藻类的生长是否受营养盐限制有关,只有当藻类生长受到水体营养盐浓度限制时,CO_2浓度升高才会显著改变其元素组成.     

塔吉克斯坦黄土的化学风化历史及古气候意义

对塔吉克斯坦南部Chashmanigar黄土剖面进行了主量元素和部分微量元素的含量测定, 并计算了各层古土壤相对于下伏黄土层的元素淋失状况和样品的风化强度. 根据一些对气候变化较为敏感的元素比值曲线, 我们发现Chashmanigar剖面中的各古土壤层均接受了程度不同的化学风化作用, 且风化强度高于黄土层, 从而表明塔吉克南部同中国黄土一样, 古土壤发育于相对温湿的间冰期. 此外, 塔吉克南部黄土0.9 Ma以前的总体风化强度高于0.9 Ma以后, 这可能意味着0.9 Ma以后的干旱化程度的进一步加强.     

河流水-气界面CO2脱气时间尺度变化研究进展

河流作为连接陆地和海洋碳库之间的通道,是全球内陆水体碳排放最主要的载体,在全球碳循环中发挥着至关重要的作用。全球河流水-气界面二氧化碳（CO₂）脱气显著的时间异质性特征研究有助于深入理解其碳循环过程与机制,也为准确评估碳通量以及完善碳循环模型提供了科学支撑。本文系统梳理了国内外的相关研究成果,总结了目前河流CO₂脱气通量在昼夜、季节以及多年尺度上的动态变化及其影响因素,指出其昼夜变化与季节变化存在一定的周期性,并对不同空间尺度上CO₂脱气通量的时间差异进行讨论。同时分析当前研究中的不足,认为缺乏河流二氧化碳分压（pCO₂）与CO₂脱气系数（k）高分辨率且长期连续的直接测量,限制了河流CO₂脱气通量时间尺度变化的周期性及相互之间关系的厘定,使得气候变化与人类活动对河流CO₂脱气时间动态的影响仍然难以量化与预测。最后,根据目前存在的问题,展望了未来的研究重点,为全球河流水-气界面碳循环过程与机制、模型研究提供新的思路与方向,以及可以更准确地评估和预测未来河流碳排放的变化趋势。     

亚热带城市湖泊与河流CO2气体通量特征及其影响因素

湖泊、河流等内陆水体是连接陆地生态系统和海洋的“长程碳环路”的重要节点,也是温室气体二氧化碳(CO₂)排放源,在调节陆地、海洋间的碳迁移转换中发挥着重要作用。相对于自然水体,城市水体因面积小、水深浅且受监测方法限制,水-气界面碳通量经常被忽略。为探讨我国亚热带城市水体温室气体排放特征,本研究以湖南省长沙市典型城市水体,包括洋湖、西湖、松雅湖、月湖4个湖泊和湘江长沙段为研究对象,分别于2022年4和10月采用光化学反馈-腔增强吸收光谱法(OF-CEAS)和扩散模型法对水-气界面CO₂通量进行对比测定。结果表明,长沙城市湖泊与河流春季为CO₂排放源,秋季为吸收汇,河流水-气界面CO₂通量呈显著季节差异。河湖之间CO₂通量在春季表现为显著差异,秋季差异不显著。CO₂通量与水体溶解氧、水体总氮浓度等呈显著正相关。2种方法的CO₂通量对比测定在湖泊上显著相关,但对河流而言相关性不显著。研究揭示的城市湖泊与河流CO₂气体的排放特征有利于深入探究城市水体碳的迁移转化,可对全面了解全球气候变化过程和河湖湿地温室气体减排和调控提供科学支撑。     

地震滑坡在活跃造山带侵蚀和风化中的作用:进展与展望

以地震为代表的构造运动在地球地貌演化中起着根本性的作用,其过程包括同震抬升或沉降和地震滑坡侵蚀.地震诱发的滑坡向河流输送大量的松散物质,可造成流域物质输移通量成倍增加,且持续时间可达几十年或更久.在暴露新鲜岩石的同时,地震滑坡还剥蚀植被和土壤,这些作用都极大地影响着区域的碳输移.越来越多的研究尝试量化地震对地表过程影响...     

马来半岛和婆罗洲北部的化学风化作用:来自河流表层沉积物的黏土矿物和元素地球化学记录

硅酸盐岩的风化产物通常可以有效地用于研究陆地表面发生的化学风化作用及其控制因素.选择位于东南亚热带地区的马来半岛和婆罗洲北部,通过分析其主要流域表层沉积物的黏土矿物和主要元素地球化学组成,开展热带地区化学风化及其控制因素的现代过程研究.结果显示,马来半岛的黏土矿物组合以高岭石(平均80%)为主,其次为伊利石(17%),...     

三峡水库CO2、CH4通量监测分析研究

自成库以来,三峡水库CO₂、CH₄等温室气体通量较蓄水前发生明显改变。如何科学认识和客观评估三峡水库修建及运行对其CO₂、CH₄等温室气体通量的影响备受关注。本文简要回顾了自2009年以来在三峡水库开展CO₂、CH₄等温室气体通量监测与分析工作,综述认为,现阶段三峡水库温室气体排放以水-气界面扩散释放为主要途径。陆源输入的有机碳是主导三峡水库CO₂、CH₄产生的主要碳源,但在局部区段或时段自源性有机碳的贡献亦十分显著。同蓄水前相比,三峡水库碳排放量呈现为净增加,淹没效应约占水库C净增量的20%,库区内点面源污染负荷并未对CO₂排放的净增量产生显著贡献,阻隔效应和生态系统重建效应对三峡水库碳排放的净增量产生显著贡献。近10年来,监测方法比对、监测点位优化等工作在一定程度上完善了三峡水库温室气体通量监测体系。新方法、新技术的引入也为三峡水库温室气体通量监测分析提供了有利支撑和保障,但复杂水文环境...     

蓄水初期三峡水库草堂河水-气界面CO2和CH4通量日变化特征及其影响因素

为查明三峡水库蓄水初期典型支流水-气界面CO_2和CH_4通量的日变化特征,采用LGR在线分析仪-通量箱法,于2015年9月初在库腹一级支流草堂河回水区开展连续24 h的定位观测.结果表明,24 h监测期内,支流库湾水-气界面CO_2通量变幅为-81.642~180.991 mg/(m~2·h),呈"昼吸夜放"特征,均值为17.346 mg/(m~2·h),总体为释放特征;CH_4全天均表现为释放状态,释放通量均值为0.064 mg/(m~2·h),呈"昼弱夜强"变化.相关分析结果表明,CH_4和CO_2释放通量与风速呈正相关,与表层水温、溶解氧浓度、叶绿素a浓度呈负相关,说明风速物理扰动、浮游植物光合作用是控制草堂河水-气界面气体通量最重要的环境因素.同时,干-支流相互作用形成的特殊水环境(如异重流、水温分层)也与水-气界面温室气体通量过程密切相关,但是其作用机制更为复杂,应开展进一步系统观测和深入研究.     

Chemical weathering and CO2 consumption in the glaciated Karuxung River catchment,Tibetan Plateau

Climate factors play critical roles in controlling chemical weathering, while chemically weathered surface material can regulate climate change. To estimate global chemical weathering fluxes and CO₂ balance, it is important to identify the characteristics and driving factors of chemical weathering and CO₂ consumption on the Tibetan Plateau, especially in glaciated catchments. The analysis of the hydro-geochemical data indicated that silicate weathering in this area was inhibited by low temperatures, while carbonate weathering was promoted by the abundant clastic rocks with fresh surfaces produced by glacial action. Carbonate weathering dominated the riverine solute generation (with a contribution of 58%, 51%, and 43% at the QiangYong Glacier (QYG), the WengGuo Hydrological Station (WGHS), and the lake estuary (LE), respectively). The oxidation of pyrite contributed to 35%, 42%, and 30% of the riverine solutes, while silicate weathering contributed to 5%, 6%, and 26% of the riverine solutes at the QYG, WGHS, and LE, respectively. The alluvial deposit of easily weathering fine silicate minerals, the higher air temperature, plant density, and soil thickness at the downstream LE in comparison to upstream and midstream may lead to longer contact time between pore water and mineral materials, thus enhancing the silicate weathering. Because of the involvement of sulfuric acid produced by the oxidation of pyrite, carbonate weathering in the upstream and midstream did not consume atmospheric CO₂, resulting in the high rate of carbonate weathering (73.9 and 75.6 t km⁻² yr⁻¹, respectively, in maximum) and potential net release of CO₂ (with an upper constraint of 35.6 and 35.2 t km⁻² yr⁻¹, respectively) at the QYG and WGHS. The above results indicate the potential of the glaciated area of the Tibetan Plateau with pyrite deposits being a substantial natural carbon source, which deserves further investigation.     

三峡水库澎溪河CO2、CH4气泡释放通量初探

气泡释放是天然水体中水-气交换的重要途径之一.采用改进的倒置漏斗型气泡通量监测装置于2012年3-8月期间对三峡支流澎溪河高阳平湖库湾水域进行气泡释放通量的监测研究.研究期间,研究水域CH4气泡释放通量变化范围为0.01 ～ 23288.64 μmol/(m2·d);CO2气泡释放通量变化范围为0～799.89 μmol/(m2·d).不同常规采样点CH4、CO2气泡释放通量均呈现出高度的时空异质性特征.但CH4气泡释放通量显著高于CO2气泡释放通量,且二者释放过程具有同步性.同国外已有水库监测结果相比,澎溪河回水区高阳平湖库湾水域CH4、CO2气泡释放通量位于中等水平.CH4气泡释放通量约为同期CH4扩散通量的0～ 1893.90％,超量释放下CH4气泡释放通量可达同水域CH4扩散通量的6270.5％±390.0％.CO2气泡释放通量仅占同期扩散通量绝对值的0～ 21.74‰,超量释放下,CO2气泡释放通量亦仅为同期扩散通量绝对值的40.33‰ ±0.93‰.CH4气泡释放通量在支流库湾水域对总通量的贡献不可忽视.     

三峡水库澎溪河水-气界面CO2、CH4扩散通量昼夜动态初探

三峡水库温室气体效应近年来备受关注.为揭示三峡水库典型支流澎溪河水-气界面CO₂和CH₄通量的昼夜动态规律,明晰短时间尺度下该水域温室气体释放的影响因素,在2010年6月至2011年5月的一个完整水文周年内,选择4个具有代表性的时段(2010年8、11月和2011年2、5月)对澎溪河高阳平湖水域开展昼夜跟踪观测.结果表明:2010年8、11月和2011年2、5月4次采样的CO₂日总通量值分别为-8.34、73.94、28.13和-20.12 mmol/(m²·d),相应的CH₄日总通量值分别为2.22、0.11、0.32和7.16 mmol/(m²·d),不同时期昼夜变化明显.研究水域CO₂和CH₄通量过程不具同步性:CO₂昼夜通量变化可能更显著地受到水柱光合/呼吸过程的影响,但瞬时气象过程(水汽温差、瞬时风速等)在高水位时期亦可对CO₂通量产生显著影响;CH₄昼夜通量变化与水温条件改变更为密切.     

夏季金沙江下游水-气界面CO2、CH4通量特征初探

河流是连接大陆和海洋两大碳库的桥梁,在全球碳循环中的作用举足轻重.金沙江作为长江的上游段,对区域碳循环及区域化学风化的影响非常重要.于2015年8月8-18日对金沙江下游水-气界面CO_2与CH_4通量特征进行监测与分析.采用顶空平衡法结合薄边界层模型估算法计算表层水体CO_2与CH_4的分压以及水-气界面的交换通量,并分析环境变量与其之间的相关性.研究发现,金沙江下游表层水体p(CO_2)平均值为2724.84±477.18μatm,表层水体p(CH_4)平均值为59.96±6.74μatm;水-气界面CO_2通量平均值为2.24±0.50 mmol/(m2·h),CH_4通量平均值为0.000163±0.00009 mmol/(m2·h),通量与分压趋势基本保持一致.表层水体p(CO_2)与溶解性无机碳浓度、碱度均呈显著正相关,而p(CH_4)与水温、叶绿素a浓度均呈显著正相关,CO_2通量与p(CO_2)、溶解性无机碳浓度、碱度均呈正相关,CH_4通量与p(CH_4)、风速均呈正相关,其他环境因素对通量的影响不明显,仍需进一步研究.金沙江下游水-气界面CH_4扩散通量较低,而CO_2扩散通量在世界主要河流中属于中等水平.     

Origin and source of CO2 in natural gas from the eastern Sichuan Basin

The CO2 contents of natural gas from the eastern Sichuan Basin were mainly less than 2%,and they were generally large when the H2S contents were over 5%.The natural gas in the eastern Sichuan Basin showed high δ13C1 values uncorrelated with H2S contents,and the oil-associated gas generally displayed carbon isotopic reversal between methane and ethane,whereas the coal-derived gas samples displayed positive series.The δ13C values of CO2 in the natural gas could be divided into two types,one with low values(-24‰--12‰)and the other with high values(-8‰-4‰).The natural gas had low R/Ra values and broad CO2/3He values distinct from the mantle-derived gas,and the CO2 was typical of crustal origin.Natural gas with high δ13CCO2 values is distributed in the north region of the eastern Sichuan Basin,and CO2 in H2S-poor and H2S-free reservoirs was mainly derived from the thermal decomposition of carbonate rocks under Permian magmatism and high heat flow,whereas CO2 in the gas reservoirs with high TSR extent was derived mainly from the dedolomitization of carbonate reservoirs under acidic formation water,and the CO2 of TSR origin generally entered into the secondary calcite.The CO2 in natural gas in the south-central region of the eastern Sichuan Basin,which had been rarely affected by the Emeishan mantle plume,displayed low δ13C values and was of organic origin.Though the natural gas in Wolonghe gas field had experienced TSR,the low reaction extent and weak acidity of formation water could hardly have resulted in the dedolomitization,and therefore CO2 in the natural gas was mainly of TSR origin with low δ13C values.     

三峡水库澎溪河消落区土-气界面CO2和CH4通量初探

水库近岸湿地(消落区)温室气体(CO₂、CH₄)产汇是水库温室气体效应问题的重要组成部分.本文以三峡水库支流澎溪河的白家溪、养鹿两处大面积消落区为研究对象,于2010年6 9月水库低水位运行期间,对近岸消落区土-气界面CO₂、CH₄通量进行监测.白家溪消落区土-气界面CO₂通量均值为12.38±2.42 mmol/(m²·h);CH₄通量均值为0.0112±0.0064 mmol/(m²·h).养鹿消落区CO₂、CH₄通量均值分别为10.54±5.17、0.14±0.16 mmol/(m²·h).总体上,6 9月土-气界面CO₂通量呈增加趋势,而CH₄通量水平呈现显著的递减趋势.消落区土地出露后植被恢复,在一定程度上促进了土壤有机质含量的增加,使得6 9月CO₂释放通量的总体趋势有所增加.消落区退耕后,其甲烷氧化菌的活性得到恢复,加之在土地出露曝晒过程中土壤透气性增强,使得消落区土壤对大气中CH₄吸收氧化潜势增强.尽管如此,仍需进一步的研究以明晰消落区土-气界面CO₂、CH₄产汇的主要影响因素.     

Stability of forsterite + CO2 and its bearing on the role of CO2 in the mantle

An experimental determination of the reaction MgCO₃ + MgSiO₃ = Mg₂SiO₄ + CO₂ between 20 and 40 kbars and in the range 1000–1500°C yields an average pressure effect on the equilibrium of 44 bars/°C. This result shows that the assemblage forsterite and carbon dioxide is not stable under most pressure and temperature conditions expected in the upper mantle. Hypotheses requiring the presence of free CO₂ in the low-velocity zone, CO₂ as a drive mechanism for kimberlite emplacement, or action of a free CO₂ phase in ultramafic rocks may need considerable revision.     

Mass‐balance modeling of mineral weathering rates and CO2 consumption in the forested,metabasaltic Hauver Branch watershed,Catoctin Mountain,Maryland, USA

Mineral weathering rates and a forest macronutrient uptake stoichiometry were determined for the forested, metabasaltic Hauver Branch watershed in north‐central Maryland, USA. Previous studies of Hauver Branch have had an insufficient number of analytes to permit determination of rates of all the minerals involved in chemical weathering, including biomass. More equations in the mass‐balance matrix were added using existing mineralogic information. The stoichiometry of a deciduous biomass term was determined using multi‐year weekly to biweekly stream‐water chemistry for a nearby watershed, which drains relatively unreactive quartzite bedrock. At Hauver Branch, calcite hosts ~38 mol% of the calcium ion (Ca²⁺) contained in weathering minerals, but its weathering provides ~90% of the stream water Ca²⁺. This occurs in a landscape with a regolith residence time of more than several Ka (kiloannum). Previous studies indicate that such old regolith does not typically contain dissolving calcite that affects stream Ca²⁺/Na⁺ ratios. The relatively high calcite dissolution rate likely reflects dissolution of calcite in fractures of the deep critical zone. Of the carbon dioxide (CO₂) consumed by mineral weathering, calcite is responsible for approximately 27%, with the silicate weathering consumption rate far exceeding that of the global average. The chemical weathering of mafic terrains in decaying orogens thus may be capable of influencing global geochemical cycles, and therefore, climate, on geological timescales. Based on carbon‐balance calculations, atmospheric‐derived sulfuric acid is responsible for approximately 22% of the mineral weathering occurring in the watershed. Our results suggest that rising air temperatures, driven by global warming and resulting in higher precipitation, will cause the rate of chemical weathering in the Hauver Branch watershed to increase until a threshold temperature is reached. Beyond the threshold temperature, increased recharge would produce a shallower groundwater table and reduced chemical weathering rates. Copyright © 2013 John Wiley & Sons, Ltd.     

Melting relationships in CaO-CO2 and MgO-CO2 to 36 kilobars with comments on CO2 in the mantle

The melting curves of CaCO₃ and MgCO₃ have been extended to pressures of 36 kb by experiments in piston-cylinder apparatus. At 30 kb, the melting temperatures of calcite and magnesite are 1610°C and 1585°C, respectively. New data for the magnesite dissociation reaction permit the location of an invariant point for the assemblage magnesite + periclase + liquid + vapor near 26 kb-1550°C. New data are also presented for the calcite-aragonite transition at 800°C, 950°C and 1100°C. At pressures above 36–50 kb, calcite and magnesite melt at temperatures lower than the solidus of dry mantle peridotite. Natural and experimental evidence suggests that carbon dioxide in the Earth's mantle could be present in a variety of forms: (a) a free vapor phase, (b) vapor dissolved in silicate magma, (c) crystalline carbonate, (d) carbonatite liquid, (e) carbon-bearing silicate analogs, or (f) carbonato-silicates (such as scapolite, spurrite, tilleyite, and related compounds).     

Geochemical features of the geothermal CO2-watercarbonate rock system and analysis on its CO2 sources

Taking Huanglong Ravine and Kangding, Sichuan, and Xiage, Zhongdian, Yunnan, as examples, the authors summarize the hydrogeochemical and carbon stable isotopic features of the geothermal CO₂-water-carbonate rock system and analyze the CO₂ sources of the system. It was found that the hydrogeochemical and carbon stable isotopic features of such a system are different from those of shallow CO₂-water-carbonate rock system, which is strongly influenced by biosphere. The former has higher CO₂ partial pressure, and is rich in heavy carbon stable isotope. In addition, such a geothermal system is also different from that developed in igneous rock. The water in the latter system lacks Ca²⁺, and thus, there are few tufa deposits on ground surface, but it is rich in light carbon stable isotope. Further analysis shows that CO₂ of the geothermal CO₂-water-carbonate rock system is a mixture of metamorphic CO₂ and magmatic CO₂.