橄榄岩蛇纹石化和碳酸盐化反应动力学、反馈机制及固碳-产氢效应

doi:10.3799/dqkx.2025.301

橄榄岩蛇纹石化和碳酸盐化反应动力学、反馈机制及固碳-产氢效应

doi: 10.3799/dqkx.2025.301

张宓^1,2,
李玟玟^1,2,
黄瑞芳^1,2, ,

1. 中国科学院南海海洋研究所, 热带海洋环境与岛礁生态全国重点实验室, 广东广州 510301
2. 中国科学院大学, 北京 100049

基金项目:

科技部重点研发专项 (2023YFF0807101), 广州市南沙区重点科技计划 (2023ZD018).

详细信息

作者简介:
张宓 (2003-), 硕士研究生, 从事蛇纹石化过程中碳的地球化学行为实验研究. ORCID: 0009-0003-2896-3044. E-mail: zhangmi200307@163.com

通讯作者:
黄瑞芳(1986-),博士,研究员,从事蛇纹石化反应机制及其地球宜居性效应研究.ORCID:0000-0002-3052-5890.E-mail:rfhuang@scsio.ac.cn

中图分类号: P588.323
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出版历程
- 收稿日期: 2025-08-11
- 网络出版日期: 2026-01-05

Kinetics of Serpentinization and Carbonation of Peridotite and Their Feedback Mechanisms: Implications for Carbon Sequestration Coupled with Hydrogen Production

Zhang Mi^1,2,
Li Wenwen^1,2,
Huang Ruifang^{1,2
, ,}

1. State Key Laboratory of Tropical Oceanography, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China
2. University of Chinese Academy of Sciences, Beijing 100049, China

摘要

摘要: 蛇纹石化通常是指超基性岩 (如橄榄岩和科马提岩)的热液蚀变，岩石中的橄榄石和斜方辉石与富水流体反应，生成蛇纹石、(±)滑石和 (±)磁铁矿等矿物。橄榄岩作为地幔中最具代表性的超镁铁质岩石，其蛇纹石化过程在地壳-地幔水循环和岩石圈演化中扮演关键角色，并且在天然氢生成和固碳方面具有重要潜力。本研究系统探究了影响橄榄岩蛇纹石化与碳酸盐化反应动力学的关键因素，重点分析了二者之间能量与物质传递的反馈机制，以评估其在碳封存与制氢领域的应用前景。温度、压力、盐度、pH及溶液组分 (如NaCl和NaHCO₃浓度)是影响蛇纹石化与碳酸盐化反应动力学的核心参数。特定温压条件能够显著加快反应速率，而流体化学成分的变化也对反应整体进程具有关键调控作用。此外，反应的自热特征、自限性以及生成的富硅层共同构成了复杂的动力学反馈机制。蛇纹石化与碳酸盐化本质上均为放热反应，释放的热量能够有效提高体系温度，从而促进反应动力学过程。尽管橄榄石蛇纹石化与碳酸盐化反应速率均高度依赖温度，但两者存在不同的最佳反应温度区间。同时，蛇纹石化与碳酸盐化反应通常伴随着体积膨胀和孔隙度的变化。反应初期，孔隙发育有利于流体渗入与矿物接触，但随着碳酸盐矿物持续沉淀，孔隙率与渗透率显著降低，对流体运移形成负反馈。由于二者沉淀动力学的差异，最终产物在高流速区与低流速区呈现明显的分异分布。此外，固液界面形成的钝化层会抑制矿物溶解和碳酸盐沉淀，严重制约蛇纹石化与碳酸盐化反应的持续进行。未来的研究可通过优化反应条件，提升固碳效率与产氢速率，并针对协同反应中的离子迁移行为展开深入探索，从而有效缓解溶解点位附近因沉淀导致的孔隙堵塞与钝化层问题。同时，推动原位固碳-产氢技术的实际应用，有望为应对气候变化与满足能源需求提供兼具“固碳”与“产氢”双重效益的解决方案。
- 橄榄岩 /
- 蛇纹石化 /
- 产氢 /
- 碳封存 /
- 反馈机制
Abstract: Serpentinization generally refers to the hydrothermal alteration of ultramafic rocks (e.g., peridotite and komatiite), where olivine and orthopyroxene react with water-rich fluids to form secondary minerals including serpentine, (±) talc, and (±) magnetite. Peridotite is the most representative ultramafic rock of the Earth's mantle, and its serpentinization is central to crust-mantle water cycling and lithospheric evolution. Concurrently, this process holds significant potential for natural hydrogen generation and carbon sequestration. This study systematically investigates the key reaction kinetic factors of peridotite serpentinization and carbonation, and elaborates in depth on the feedback mechanism of energy and material transfer between the two reactions, aiming to assess their application prospects in carbon sequestration and hydrogen production. In the reactions of peridotite serpentinization and carbonation, temperature, pressure, salinity, pH, and solution components (such as NaCl and NaHCO₃ concentrations) are the core controlling factors influencing the reaction kinetics of both. Specific temperature and pressure conditions can significantly accelerate the reaction rate, and changes in fluid chemical composition also play a crucial role in altering the overall reaction process. Additionally, the self-heating feature, self-limiting nature, and the formation of a silica-rich layer during the reaction constitute a complex kinetic feedback mechanism. Both serpentinization and carbonation are exothermic reactions, and the heat they release can effectively increase the system temperature and promote the reaction kinetics. Although the reaction rates of olivine serpentinization and carbonation are highly dependent on temperature, they have different optimal temperature ranges. Moreover, serpentinization and carbonation reactions are usually accompanied by volume expansion and changes in porosity. Although this is beneficial for the infiltration and contact of reaction fluids in the initial stage, the sharp decline in pore permeability due to the precipitation of carbonate minerals has a negative feedback effect on fluid flow. Due to the differences in precipitation kinetics between the two, the final products show different precipitation distributions in high-flow and low-flow areas. The passivation layer formed at the solid-liquid interface limits mineral dissolution and carbonate precipitation, severely restricting the serpentinization and carbonation processes. In the future, conditions can be optimized to enhance carbon sequestration efficiency and hydrogen production rate, and further research can be conducted on ion migration in the coupled reactions to effectively control the clogging of pores and the formation of passivation layers near the dissolution sites. At the same time, efforts should be made to promote the practical application of in-situ carbon sequestration-hydrogen production technology, providing a solution that offers dual benefits of "carbon sequestration" and "hydrogen production" for addressing climate change and meeting energy demands.
- Peridotite /
- Serpentinization /
- Hydrogen production /
- Carbon sequestration /
- Feedback mechanism

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橄榄岩蛇纹石化和碳酸盐化反应动力学、反馈机制及固碳-产氢效应

doi: 10.3799/dqkx.2025.301

作者简介:
张宓 (2003-), 硕士研究生, 从事蛇纹石化过程中碳的地球化学行为实验研究. ORCID: 0009-0003-2896-3044. E-mail: zhangmi200307@163.com

通讯作者:
黄瑞芳(1986-),博士,研究员,从事蛇纹石化反应机制及其地球宜居性效应研究.ORCID:0000-0002-3052-5890.E-mail:rfhuang@scsio.ac.cn

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Kinetics of Serpentinization and Carbonation of Peridotite and Their Feedback Mechanisms: Implications for Carbon Sequestration Coupled with Hydrogen Production

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橄榄岩蛇纹石化和碳酸盐化反应动力学、反馈机制及固碳-产氢效应

doi: 10.3799/dqkx.2025.301

作者简介: 张宓 (2003-), 硕士研究生, 从事蛇纹石化过程中碳的地球化学行为实验研究. ORCID: 0009-0003-2896-3044. E-mail: zhangmi200307@163.com

通讯作者: 黄瑞芳(1986-),博士,研究员,从事蛇纹石化反应机制及其地球宜居性效应研究.ORCID:0000-0002-3052-5890.E-mail:rfhuang@scsio.ac.cn

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Kinetics of Serpentinization and Carbonation of Peridotite and Their Feedback Mechanisms: Implications for Carbon Sequestration Coupled with Hydrogen Production

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出版历程

目录

作者简介:
张宓 (2003-), 硕士研究生, 从事蛇纹石化过程中碳的地球化学行为实验研究. ORCID: 0009-0003-2896-3044. E-mail: zhangmi200307@163.com

通讯作者:
黄瑞芳(1986-),博士,研究员,从事蛇纹石化反应机制及其地球宜居性效应研究.ORCID:0000-0002-3052-5890.E-mail:rfhuang@scsio.ac.cn