Advances in Numerical Modelling of Carbon Cycling Processes in Marine Sediments
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摘要: 海洋沉积物不仅是各种不同来源有机碳的重要埋藏场所，也是一个十分活跃的生物地球化学反应器，在全球海洋碳循环中扮演着重要角色.相对传统的地球化学测试和定性描述方法，数值模型可以突破时间和空间的限制，定量获取海洋沉积物中各个碳循环过程的反应速率及其通量，因此日益受到学界的重视.海洋沉积物有机质降解是驱动碳循环最为关键的生物地球化学过程，其释放进入周围孔隙水的溶解无机碳一部分可扩散至沉积物上覆水体，另一部分可与钙、镁等离子沉淀形成自生碳酸盐矿物.首先综述目前主要的3类沉积物有机质降解模型（离散性有机质降解模型、连续性有机质降解模型和Power模型）的建模过程及其在全球海洋沉积物有机质降解过程中的应用；接着从有机质降解相关的初级与次级反应出发，介绍沉积物中与有机质降解相关的地球化学过程反应速率模型的刻画方法，并从碳酸盐平衡体系和同位素质量平衡模式角度，探讨了沉积物有机质降解过程对自生碳酸盐形成及其碳同位素的影响；最后分析了当前阶段数学模型在描述有机质降解过程和自生碳酸盐形成中存在的问题和不足，并在此基础上展望未来亟需加强的研究要点，希企为深入理解海洋碳循环与全球气候变化相互反馈，建立可靠的海洋碳循环和生物地球化学预测系统提供有益的科学支撑.Abstract: Marine sediment is not only a critical burial area of organic carbon from various sources but also a very active biogeochemical reactor, which plays a vital role in the global marine carbon cycle. Compared with the geochemical testing and qualitative description methods, the numerical model can break through the limitations of time and space and quantitatively obtain the reaction rate and flux of each carbon cycle process in marine sediments. Therefore, it has been paid more and more attention by the academic community. The degradation of organic matter in marine sediments is the most critical biogeochemical process driving the carbon cycle. Part of the dissolved inorganic carbon released into the surrounding pore water can diffuse to the overlying water column. The other part can form authigenic carbonate minerals with calcium and magnesium plasma precipitation. In this paper it firstly reviews the modeling process of three main types of sediment organic matter degradation models (discrete model, reactive continuum model, and Power model) and their applications in the global marine sediment organic matter degradation process. Then, starting from the primary and secondary reactions related to the degradation of organic matter, the description method of the reaction rate model of geochemical processes related to the degradation of organic matter in sediments is introduced, and the influence of the degradation of organic matter on the formation of authigenic carbonates and their carbon isotopes is discussed from the perspective of carbonate equilibrium system and isotope mass balance model. Finally, the problems and shortcomings of the current mathematical model in describing the degradation process of organic matter and the formation of authigenic carbonate are analyzed, and on this basis, the research points that need to be strengthened in the future are prospected. It is hoped that in this paper it will provide useful scientific support for understanding the mutual feedback between the ocean carbon cycle and global climate change and establishing a reliable prediction system for ocean carbon cycle and biogeochemistry.
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图 1 多-G模型中有机质降解过程示意图
Fig. 1. Schematic diagram of organic matter degradation process in the multi-G models
图 2 多-G模型中有机质活性及其组分的分布示意图
Fig. 2. Schematic diagram of the distribution of organic matter reactivity and its fraction in the G models
图 3 连续性有机质降解模型中有机质活性分布的示意图
Fig. 3. Schematic representation of organic matter reactivity distribution in RCM
图 5 不同有机质降解模型在全球海洋沉积物中有机质降解过程的应用
Fig. 5. Application of different organic matter degradation models to organic matter degradation processes in global marine sediments
图 6 全球海洋可能发生自生碳酸盐沉淀的区域(a)；全球海洋沉积物中水合物分布及其埋藏量(b)
图a引自Bradbury et al.（2019），图b引自Kretschmer et al.（2015）. 图a中，红色圆点表示机器学习处理的站点，红色区域和绿色区域分别表示AOM主导和硫酸根还原主要的自生碳酸盐形成的区域
Fig. 6. Regions of the global ocean where authigenic carbonate precipitation is likely to occur (a); global hydrate distribution in marine sediments and its burial volume (b)
图 7 Gamma分布函数在参数v < 1和v > 1时的分布特征
Fig. 7. Distribution characteristics of the Gamma distribution function for parameters v < 1 and v > 1
图 8 G模型、γ-RCM和Power模型参数与沉降速率、有机质通量之间的关系
Fig. 8. Relationship between G model, γ-RCM and Power model parameters and sedimentation rate and organic matter flux
表 1 沉积物中有机质相关的初级与次级反应，及其反应速率
Table 1. Primary and secondary redox reactions related to organic matter in sediments, and their reaction rates
地球化学反应 反应速率 初级反应 R1 CH2O+O2 → CO2+H2O -ROM R2 CH2O+4NO3- → 2N2+4HCO3-+CO2+3H2O -4·ROM R3 CH2O+2MnO2+3CO2+H2O → 2Mn2++4HCO3- 2·ROM R4 CH2O+4Fe(OH)3+7CO2 → 4Fe2++8HCO3-+3H2O 4·ROM R5 2CH2O+SO42- → H2S+2HCO3- 0.5·ROM R6 2CH2O+H2O → CH4+HCO3-+H+ 0.5·ROM 次级反应 R7 Fe2++HS-+HCO3- → FeS+CO2+H2O kFeHx·[Fe2+]·[HS-] R8 4Fe2++O2+8HCO3-+2H2O → 4Fe(OH)3+8CO2 kFeOx·[Fe2+]·[O2] R9 2Mn2++O2+4HCO3- → 2MnO2+4CO2+2H2O kMnOx·[Mn2+]·[O2] R10 H2S+2O2+2HCO3- → SO42-+2CO2+2H2O kSOx·[H2S]·[O2] R11 NH4++2O2+2HCO3- → NO3-+2CO2+3H2O kNHOx·[NH4+]·[O2] R12 CH4+O2 → CO2+2H2O kCHOx·[CH4]·[O2] R13 MnO2+2Fe2++3HCO3-+2H2O → 2Fe(OH)3+Mn2++4CO2 kMnFe·[MnO2]·[Fe2+] R14 MnO2+H2S+2CO2 → Mn2++S0+2HCO3- kMnHs·[MnO2]·[H2S] R15 H2S+2Fe(OH)3+4CO2 → 2Fe2++S0+4HCO3-+2H2O kFeHS·[Fe(OH)3]·[H2S] R16 FeS+2Fe(OH)3+6CO2 → 3Fe2++S0+6HCO3- kFeSFe·[Fe(OH)3]·[FeS] R17 FeS+4MnO2+8CO2+4H2O → 4Mn2++4Fe2++SO42-+8HCO3- kFeMnO·[FeS]·[MnO2] R18 FeS+2O2 → Fe2++SO42- kFeSOx·[FeS]·[O2] R19 CH4+SO42- → HCO3-+HS-+H2O kAOM·[CH4]·[SO42-] 注：[]表示括号中物质或元素的含量或浓度，ki表示动力学反应系数. 
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