大气CO2汇:硅酸盐风化还是碳酸盐风化的贡献?

至今人们仍普遍认为:是硅酸盐的化学风化碳汇作用在控制着长时间尺度的气候变化,而碳酸盐的化学风化作用不具有这一功能,因为碳酸盐溶解过程中消耗的所有CO<,2>又通过海洋中相对快速的碳酸盐沉积而返回大气.本研究发现,碳酸盐溶解的快速动力学特性(比硅酸盐快100倍以上)以及硅酸盐流域中少量碳酸盐矿物在控制流域溶解无机碳(DI...     

中国岩石风化作用所致的碳汇能力估算

岩石的风化作用同时参与了短时间尺度和长时间尺度的全球碳循环 ,对碳酸盐岩而言 ,它的风化作用在短时间尺度上对大气二氧化碳循环具有重要影响 ,但在长时间尺度上不产生净碳汇 ;而硅酸盐岩等其他类型岩石的风化过程由于反应速率较慢 ,在短时间尺度上对全球碳循环及其变化反应不灵敏 ,但它所产生的净碳汇是遗漏汇的组成之一 .为了准确估计我国岩石风化所致的碳汇能力 ,简要评价了现有的各种模型和方法 ,并基于GEM -CO2 模型进行了计算 .计算结果表明 ,我国岩石每年因溶蚀、风化作用共消耗的CO2 约为 4 .72× 10 7t,折合成C为 1.4 1× 10 7t,其中由碳酸盐类岩石风化消耗的碳量最多 ,约为 0 .74× 10 7t/a ,占总量的 5 2 .6 5 % .硅酸盐岩及其他类型岩石风化消耗的碳量约为 0 .6 7× 10 7t/a ,占总量的 4 7.35 % .岩石风化所致碳汇能力的空间分布首先取决于岩石类型 ,其次受地区的气候条件控制 .     

北江河水溶解无机碳同位素的季节变化

在有碳酸盐岩分布的河流流域, 河水地球化学主要反映的是风化速率较高的碳酸盐矿物风化的信息, 而硅酸盐矿物风化的信息往往被掩盖掉.北江流域碳酸盐岩和硅酸岩分布广泛, 为追踪其中的硅酸盐矿物风化的信息, 分析了北江河水中溶解无机碳同位素的时空变化.河水样品按4个季节自北江的上游到下游采集6个样点, 分析结果显示, 除上游武江的采样点同位素值季节变化不大外, 中下游采样点的同位素值有明显季节变化, 主要表现在6月份的δ13C_DIC显著变轻(-16‰~-19‰).在详细剖析矿物风化过程对碳同位素的影响后, 指出除了显著的碳酸盐矿物风化过程外, 北江流域在夏季还存在明显的硅酸盐矿物风化过程, 大大提高了流域的碳汇作用.      

岩石风化碳汇研究进展:基于IPCC第五次气候变化评估报告的分析

岩石风化碳汇特别是碳酸盐岩风化碳汇积极参与了全球碳循环过程。最新的IPCC第五次气候变化评估报告(AR5)指出全球岩石风化碳汇约为0.4 Pg C/a,占不平衡碳通量的1/2~1/3,并改进和区分了岩石风化碳汇的时间尺度,将硅酸盐岩风化碳汇时间尺度视为104~106年,碳酸盐岩风化碳汇时间尺度视为103~104年。AR5报告将岩石风化碳汇列为CO2移除的4种方法之一,其碳酸盐岩风化碳汇时间尺度属于百年至千年级。虽然AR5报告提出了前述新认识,但仍认为岩石风化碳汇速率太慢,未纳入全球碳收支核算。结合近年来的研究进展,讨论了AR5报告目前对岩石风化碳汇在通量、时间尺度和风化碳汇效应等方面认识的不足,提出了加强岩石风化碳汇速率、稳定性、影响因素和尺度转换方面的研究建议,以期进一步加强岩石风化碳汇研究工作,为平衡全球碳收支做出科学贡献。     

土地利用对岩溶作用碳汇的影响研究综述

耦合水生光合作用的岩溶作用碳汇新模式的提出使得碳酸盐岩的风化过程成为寻找“陆地剩余碳汇”(residual land sink) 的新方向。传统意义上,碳酸盐岩风化在全球碳循环模型中被认为是未快速响应地表环境变化的地质过程,然而最新一系列研究表明人类土地利用显著改变了这一地质循环过程。文章总结了岩溶作用碳汇对不同土地利用/覆被变化的具体响应,并对其机理进行了系统分析。发现土地利用与覆被变化影响岩溶作用碳循环过程主要源自土壤CO2浓度和径流量变化以及外源酸（硝酸和硫酸）的介入。证据显示在土地利用对岩溶作用碳汇的调控中土壤CO2浓度与径流量是复杂且相互制约的两个机制,人类活动产生的外源酸干扰在不同层面上的影响也不同。由于地表水生生态系统所产生的内源有机碳（AOC）的巨大稳碳能力(水生碳泵效应)在以往的研究中并没有与碳酸盐岩风化过程相联系,因而其对土地利用变化的响应过程和机理是岩溶碳循环研究的最新方向。基于土地利用调控碳酸盐岩风化过程的复杂性和多样性特点,综合考虑岩溶作用产生的DIC(溶解无机碳)与AOC在不同土地利用情况下的相互关系以及定量分析各环境因素的具体效应成为了合理制定人为土地利用调控策略的必要前提,也是岩溶作用碳汇研究的未来发展方向。      

外源水和外源酸对万华岩地下河系统岩溶碳汇效应的影响

流域的岩石化学风化过程是全球碳循环中的重要环节。近年来流域水化学碳汇通量估算已越来越多地关注到外源水(硅酸盐风化)及外源酸对全球碳循环的影响。文章选取万华岩地下河流域为研究区,流域硅酸盐岩和碳酸盐岩分布面积占比为64%和36%,于2017年对洞口进行为期一年的取样监测,并分别于4月和9月对万华岩地下河系统内13个水点的离子组成进行监测,利用水化学平衡法和Galy模型,对流域岩石化学风化速率和CO2消耗通量进行了计算,对万华岩地下河系统的岩石风化和碳循环过程进行了分析。结果表明,万华岩地下河系统岩石风化消耗CO2的速率为31.02 t·(km2·a)-1;以碳酸岩风化为主,其风化速率为硅酸盐溶蚀的20倍;流域内碳酸盐岩风化对CO2消耗量占到整个流域的92.16%;不同岩石风化类型对碳通量的贡献率以碳酸溶解碳酸盐岩最大,为87.06%;流域上游的外源水对岩溶碳汇具有巨大的促进作用,外源水汇入后碳酸盐岩碳汇速率可以达到无外源水汇入流域的2倍;硫酸溶解碳酸盐岩次之,为9.24%;碳酸风化硅酸盐岩最小,为3.7%,在计算流域碳汇量的时候应将硫酸参与岩石风化的影响去除。     

岩溶地质碳汇的稳定性——以贵州草海地质碳汇为例

近几年来对岩溶碳汇的争论越来越多, 其关键问题是岩溶作用产生的重碳酸根是否稳定。本文以贵州草海流域为研究区, 基于前人研究基础, 以碳同位素模型计算出岩溶作用产生的DIC((Dissolved Inorganic Carbon溶解无机碳)中58.8%为草海中为水生植物利用, 草海地质碳汇量达588.67 tC/a。以此推算长江中下游湖泊沉水植物每年固碳量370602 tC/a, 长江中下游湖泊中仅沉水植物稳定的地质风化CO2汇量约为75万吨。从而证明岩溶碳汇的相对稳定性和岩溶动力系统新理论的合理性。     

非岩溶水和硫酸参与溶蚀对湘南地区地下河流域岩溶碳汇通量的影响

研究非岩溶水和硫酸参与溶蚀对地下河流域岩溶碳汇通量的影响,有助于提高岩石风化碳汇通量估算精度,对于推进地质作用与全球气候变化研究意义重大。选取湘南北江上游武水河流域内4条典型地下河为对象,通过水化学对比分析,揭示硅酸盐岩风化对流域地下水化学的重要影响。运用Galy方法计算流域非岩溶地层中的硅酸盐岩风化消耗大气/土壤CO_2对岩石风化碳汇的重要贡献,并评价了H_2SO_4参与下碳汇通量的扣除比例。结果显示:(1)流域内有非岩溶地层的L01,L02地下河,Na~+,K~+和SiO_2浓度明显高于纯碳酸盐L03和L04地下河,非岩溶地层中的硅酸盐的风化对地下河水中K~+,Na~+,SiO_2浓度有一定贡献;(2)4条地下河的[Ca~(2+)+Mg~(2+)]/[HCO_3~-]当量比值为1.05~1.15,[Ca~(2+)+Mg~(2+)]/[HCO_3~-+SO_4~(2-)]的当量比值为0.99~1.08,Ca~(2+)+Mg~(2+)相对于HCO_3~-过量,过量的Ca~(2+)+Mg~(2+)与SO_4~(2-)相平衡,证实硫酸参与流域碳酸盐岩的溶蚀;(3)L01和L02地下河岩石风化消耗的CO_2通量中非岩溶地层中的硅酸盐风化消耗所占比例分别为3.36%和2.22%,而L03和L04地下河中硅酸盐风化消耗比例小于0.50%,表明有非岩溶地层存在的地下河流域,其岩石风化消耗的CO_2通量中硅酸盐风化消耗占有一定比例;(4)在考虑硫酸参与碳酸盐岩溶蚀时,4条地下河的碳汇通量分别扣除4.84%,4.52%,6.20%和9.36%。     

岩溶系统中土壤氮肥施用对岩溶碳汇的影响

有资料显示陆地碳酸盐岩风化消耗大气CO2的碳通量与世界森林碳汇通量量级相当。但农业地区过量施用氮肥形成的硝酸对碳酸盐岩的溶解会减弱岩溶碳汇效应,其量可达到7%~38%,而适量施用氮肥在增加农作物产量的同时,能降低土壤C/N比,增加土壤微生物活性,促进有机物料分解,从而提高土壤CO2浓度,提高土下碳酸盐岩的溶解速率。因此,要从两方面分析岩溶系统中土壤氮肥施用对岩溶碳汇效应的影响。同时,岩溶区碳酸盐岩风化形成的土壤具有较高的pH值及盐基饱和度,对H+有较强的缓冲作用,可能是导致自然条件下,河流中溶解无机碳(DIC)与水体中钙、镁等离子并不守恒的原因之一,因此,运用端元法可能过高估算了硝酸对碳酸盐岩的溶解量。岩溶区土壤环境中硝化作用产生的硝酸到底多少能对碳酸盐岩产生溶蚀,并影响到岩溶碳汇效应还有待研究。应结合土壤本身的特性及河流生物地球化学过程,综合研究不同施氮水平、土壤硝化产酸及其影响下的土下碳酸盐岩溶解及碳汇效应过程,客观评价岩溶区土壤氮肥施用对岩溶碳汇的影响,并寻求适宜氮肥施用量及促进岩溶碳循环,提高岩溶碳汇效应的技术方法。      

微藻无机碳利用在岩石风化及碳循环过程中的作用

岩溶碳汇呈现两种不同观点:(1)岩溶碳汇巨大,其机理在于岩溶区藻类及光合细菌利用碳酸氢根离子(HCO₃^-)实现光合作用,从动力学上加速了岩溶风化过程,促进大气CO₂的溶解。(2)岩溶区碳酸盐岩的风化作用,产生HCO₃^-,随后产生等量的阳离子在海洋中进行碳酸盐岩的沉积作用,这仅仅体现的是碳酸盐岩的搬运作用,不能体现碳汇,在长期尺度上仅仅有硅酸盐岩风化产生净碳汇。文章抓住岩石风化产生HCO₃^-与微藻光合作用利用HCO₃^-的耦合点,分析了典型代表性水生生物——微藻在无机碳利用上对岩石风化及碳汇的影响。从微藻光合无机碳利用机制以及光合作用关键性酶-碳酸酐酶(CA)作用两方面,论证了微藻生长对岩石风化及其碳汇的的促进作用;同时论述高pH、高HCO₃^-的风化环境对微藻生长影响。获得以下新认识:(1)微藻通过胞外碳酸酐酶(CAex)利用了大量HCO_3<...     

硅酸盐风化与全球碳循 环研究回顾及新进展

硅酸盐风化是大气CO2 的一个主要汇,直接影响到全球碳循环进而影响全球气候。自Walker 等（1981）进行的开创 工作以来,有关“硅酸盐风化- 碳循环- 气候变化”方面的研究大量涌现。从计算机模型到河流水化学研究,从流域面积 超过百万平方公里的大河到数十数百平方公里的单岩性小河流,取得了很多重要的进展。从全球尺度上看,硅酸盐风化每 年所消耗的大气CO2 量为0.138~0.169 Gt,相比现在大气碳库中碳的含量（约800 Gt）,乍看似乎是微不足道的,然而硅酸盐 风化消耗CO2 并将其作为碳酸盐矿物埋藏在海洋,它的存留时间超过了百万年。因此,在地质时间尺度上,硅酸盐风化是 调节全球碳循环的一个重要机制。对小流域进行的研究发现,热带地区流经玄武岩/蛇绿岩的小流域有着最高的硅酸盐风化 和大气CO2 消耗速率,热带区域火山岩化学风化消耗的大气CO2 占全球硅酸盐风化所消耗量的10%,而流域面积不到1%。     

Ecosystem-driven karst carbon cycle and carbon sink effects

It is recognized that karst processes are actively involved in the current global carbon cycle based on twenty years research, and the carbon sink occurred in karst processes is possibly an important part of “missing sink” in global carbon cycle. In this paper, an overview is given on karst carbon cycle research, and influence factors, formed carbon pools (background carbon sink) and sink increase potentials of current karst carbon cycle are analyzed. Carbonate weathering could contribute to the imbalance item (B_IM) and land use change item (E_LUC) in the global carbon cycle model, owing to its uptake of both atmospheric CO₂ (carbon sink effect) and CO₂ produced by soil respiration (carbon source reduction effect). Karst carbon sink includes inorganic carbon sink resulted from hydrogeochemical process and organic carbon sink generated by aquatic photosynthetic DIC conversion, forming relatively stable river (reservoir) water body or sediment carbon sink. The sizes of both sinks are controlled by terrestrial ecosystems and aquatic ecosystems, respectively. Desertification rehabilitation and carbon sequestration by aquatic plants are two effective ways to increase the carbon sink in karst area. It is estimated that the rate of carbon sink is at least 381 000 t CO₂/a with vegetation restoration and afforestation in southwest China karst area, while the annual organic carbon sink generated by aquatic photosynthesis is about 84 200 t C in the Pearl River Basin. The development of a soil CO₂ based model for assessment of regional dissolution intensity will help to improve the estimation accuracy of carbon sink increase and potential, thus provide a more clear and efficient karst sink increase scheme and pathway to achieve the goals of “double carbon”. With the deep investigation on karst carbon cycle, mechanism and carbon sink effect, and the improvement of watershed carbon sink measurement methods and regional sink increase evaluation approaches. Karst carbon sink is expected to be included in the list of atmospheric CO₂ sources/sinks of the global carbon budget in the near future.     

微型生物在岩溶碳循环中的作用研究回顾与展望

全球气候变化问题使岩溶系统碳循环的研究倍受关注,有关微型生物及其碳酸酐酶在岩溶系统碳循环中的作用的认识也在不断深入。文章回顾了微型生物及其碳酸酐酶在碳酸盐岩风化以及碳酸盐岩沉积过程中的作用过程及作用机制,指出未来的研究需结合不同岩溶生态环境,量化微型生物及其碳酸酐酶对岩溶生态系统碳增汇的影响,为深入研究微型生物及其碳酸酐酶对岩溶碳汇的贡献、增加岩溶生态系统碳汇的能力、助力实现碳中和提供参考。      

Atmospheric CO2 sink: Silicate weathering or carbonate weathering?

It is widely accepted that chemical weathering of Ca–silicate rocks could potentially control long-term climate change by providing feedback interaction with atmospheric CO₂ drawdown by means of precipitation of carbonate, and that in contrast weathering of carbonate rocks has not an equivalent impact because all of the CO₂ consumed in the weathering process is returned to the atmosphere by the comparatively rapid precipitation of carbonates in the oceans. Here, it is shown that the rapid kinetics of carbonate dissolution and the importance of small amounts of carbonate minerals in controlling the dissolved inorganic C (DIC) of silicate watersheds, coupled with aquatic photosynthetic uptake of the weathering-related DIC and burial of some of the resulting organic C, suggest that the atmospheric CO₂ sink from carbonate weathering may previously have been underestimated by a factor of about 3, amounting to 0.477 Pg C/a. This indicates that the contribution of silicate weathering to the atmospheric CO₂ sink may be only 6%, while the other 94% is by carbonate weathering. Therefore, the atmospheric CO₂ sink by carbonate weathering might be significant in controlling both the short-term and long-term climate changes. This questions the traditional point of view that only chemical weathering of Ca–silicate rocks potentially controls long-term climate change.     

全球变暖背景下北美育空河流域化学风化增强

硅酸盐岩风化对气候变化和构造运动的反馈对长尺度气候变化可能起到重要的调节作用,对该反馈过程的定量认识有助于更确切理解地球碳循环的运行规律。通常认为风化类型可分为两种,分别是供应限制和动力学限制。全球变暖可能促进了动力学限制流域的化学风化作用,然而,关于这方面的认识仍很有限。育空河流域是典型的动力学限制风化区域,研究育空河的风化对气候变暖的响应有助于深入认识气候和大陆风化之间的相互作用。正演模型是区分河流风化端元的重要手段,文章利用正演模型对育空河流域从1975年到2019年的主要离子组成的数据集进行分析,并获得了该流域在过去几十年的化学风化速率的变化趋势。结果表明,育空河水化学性质主要受到碳酸盐岩风化和硅酸盐岩风化控制,两者多年平均碳汇通量分别为2.1×10¹¹ mol/yr和4.1×10¹⁰ mol/yr,处于世界主要大河碳汇通量的中间水平。更重要的是,在同一时期,伴随着2.2℃的温度增幅和13.7%的径流量增加,流域内的阳离子总通量增加了35.7%,其中硅酸盐岩和碳酸盐岩风化产生的阳离子通量分别增加了41%和35%,阳离子通量/风化速率对气候的敏感性与冰岛地区的研究结果符合的很好,与风化速率加快相对应的,硅酸盐岩风化碳汇通量相对增加了59.6%。尽管碳汇的增加在绝对通量上相比人类化石燃烧产生的碳排放通量微不足道,但是考虑到构造尺度内全球硅酸盐岩风化速率的增强,尤其是在较为寒冷的高纬度地区,额外的二氧化碳固定量可能对地球历史时期的全球气候产生重要影响。     

Quantifying the carbon source of pedogenic calcite veins in weathered limestone: implications for the terrestrial carbon cycle

The continent is the second largest carbon sink on Earth’s surface. With the diversification of vascular land plants in the late Paleozoic, terrestrial organic carbon burial is represented by massive coal formation, while the development of soil profiles would account for both organic and inorganic carbon burial. As compared with soil organic carbon, inorganic carbon burial, collectively known as the soil carbonate, would have a greater impact on the long-term carbon cycle. Soil carbonate would have multiple carbon sources, including dissolution of host calcareous rocks, dissolved inorganic carbon from freshwater, and oxidation of organic matter, but the host calcareous rock dissolution would not cause atmospheric CO₂ drawdown. Thus, to evaluate the potential effect of soil carbonate formation on the atmospheric pCO₂ level, different carbon sources of soil carbonate should be quantitatively differentiated. In this study, we analyzed the carbon and magnesium isotopes of pedogenic calcite veins developed in a heavily weathered outcrop, consisting of limestone of the early Paleogene Guanzhuang Group in North China. Based on the C and Mg isotope data, we developed a numerical model to quantify the carbon source of calcite veins. The modeling results indicate that 4–37 wt% of carbon in these calcite veins was derived from atmospheric CO₂. The low contribution from atmospheric CO₂ might be attributed to the host limestone that might have diluted the atmospheric CO₂ sink. Nevertheless, taking this value into consideration, it is estimated that soil carbonate formation would lower 1 ppm atmospheric CO₂ within 2000 years, i.e., soil carbonate alone would sequester all atmospheric CO₂ within 1 million years. Finally, our study suggests the C–Mg isotope system might be a better tool in quantifying the carbon source of soil carbonate.

     

Century-scale nitrogen and phosphorus controls of the carbon cycle

In recent decades, humans have become a very important force in the Earth system, demonstrating that emissions (gaseous, liquid, and solid) are the cause of many of our environmental issues. These emissions are responsible for major global reorganizations of the biogeochemical cycles. The oceans are now a net sink of atmospheric CO₂, whereas in their preindustrial state they were a source; the trophic state of the coastal oceans is progressively moving toward increased heterotrophy; and the terrestrial realm is now vacillating between trophic states, whereas in preindustrial times it was autotrophic. In this paper, we present model calculations that underscore the role of human-induced perturbations in changing Earth's climate, specifically the role of anthropogenic nitrogen and phosphorus in controlling processes in the global carbon cycle since the year 1850 with projections to the year 2035. Our studies show that since the late 1940's emissions of nitrogen and phosphorus have been sequestered in the terrestrial living phytomass and groundwater. This nutrient-enhanced fertilization of terrestrial biota, coupled with rising atmospheric CO₂ and global temperature, has induced a sink of anthropogenic CO₂ that roughly balances the emission of CO₂ owing to land use change. In the year 2000, for example, the model-calculated terrestrial biotic sink was 1730 Mtons C/year, while the emission of CO₂ from changes in land use was 1820 Mtons C/year, a net flux of 90 Mtons C/year emitted to the atmosphere. In the global aquatic environment, enhanced terrestrial inputs of biotically reactive phosphorus (about 8.5 Mtons P/year) and inorganic nitrogen (about 54 Mtons N/year), have induced increased new production and burial of organic carbon in marine sediments, which is a small sink of anthropogenic CO₂. It is predicted that the response of the global land reservoirs of C, N, and P to sustained anthropogenic perturbations will be maintained in the same direction of change over the range of projected scenarios of global population increase and temperature change for the next 35 years. The magnitude of change is significantly larger when the global temperature increase is maximum, especially with respect to the processes of remobilization of the biotically important nutrients nitrogen and phosphorus.