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Peer-reviewedCC BY-NC-ND 4.0Environmental Science & Technology

Quantitative Study of Methane Sequestration by Hydrate-Encapsulated Bubbles at Cold Seeps: Kinetic Characteristics and Environmental Implications

4 affiliations
  1. 1Laoshan Laboratory, Qingdao 266237, China
  2. 2Qingdao Marine Science and Technology Center, Qingdao 266237, China
  3. 3Shandong Key Laboratory of Mineralization Processes and Resources Utilization of Strategic Metal Minerals, Shandong Institute of Geological Sciences, Jinan 250013, China
  4. 4Key Laboratory of Ocean Observation and Forecasting, Key Laboratory of Marine Geology and Environment & Center of Deep Sea Research, Institute of Oceanology, Chinese Academy of Sciences, Qingdao 266071, China

Abstract

Cold seeps are a major source of natural methane emissions from the seafloor and regulate the global ocean carbon cycle. Hydrate formation serves as a key natural barrier restricting methane escape, but its kinetic mechanisms remain poorly quantified due to limited in situ monitoring capabilities. Here, we employ time-series Raman spectroscopy to conduct quantitative monitoring of methane hydrate growth kinetics and coupled methane sequestration behavior across various fluid-bubble flows. Time-resolved spectral data clearly capture real-time variations in the concentration and conversion ratio of multiphase methane during hydrate growth, quantitatively revealing the dynamic evolution patterns and regulatory mechanisms in cold-seep environments. Experimental results indicate that the growth rate accelerates and the occupancy of large cages in cold-seep bubble flows increases by 15% relative to that of small cages influenced by low salinity and small solid particles. Furthermore, field model estimates indicate that the annual methane sequestration by hydrate-encapsulated bubbles at Site F is estimated to be about 0.34–2.77 t/yr, which accounts for roughly 3.3%–26.9% of the total methane leakage flux in this region. These findings fill critical quantitative gaps in understanding cold-seep methane sequestration dynamics and provide key parameters for incorporating hydrate-mediated sequestration into ocean carbon cycle models.

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BibTeX
@article{zhang2026quantitative,
  title = {{Quantitative Study of Methane Sequestration by Hydrate-Encapsulated Bubbles at Cold Seeps: Kinetic Characteristics and Environmental Implications}},
  author = {Yitong Zhang and Shichuan Xi and Liang Ma and Lianfu Li and Wanying He and Zengfeng Du and Zhicheng Wang and Jun Tao and Xin Zhang},
  journal = {Environmental Science \& Technology},
  year = {2026},
  month = sep,
  doi = {10.1021/acs.est.6c11347},
  url = {https://doi.org/10.1021/acs.est.6c11347},
  note = {CC BY-NC-ND 4.0},
}
RIS
TY  - JOUR
TI  - Quantitative Study of Methane Sequestration by Hydrate-Encapsulated Bubbles at Cold Seeps: Kinetic Characteristics and Environmental Implications
AU  - Yitong Zhang
AU  - Shichuan Xi
AU  - Liang Ma
AU  - Lianfu Li
AU  - Wanying He
AU  - Zengfeng Du
AU  - Zhicheng Wang
AU  - Jun Tao
AU  - Xin Zhang
PY  - 2026
DA  - 2026/09/30
JO  - Environmental Science & Technology
DO  - 10.1021/acs.est.6c11347
UR  - https://doi.org/10.1021/acs.est.6c11347
AB  - Cold seeps are a major source of natural methane emissions from the seafloor and regulate the global ocean carbon cycle. Hydrate formation serves as a key natural barrier restricting methane escape, but its kinetic mechanisms remain poorly quantified due to limited in situ monitoring capabilities. Here, we employ time-series Raman spectroscopy to conduct quantitative monitoring of methane hydrate growth kinetics and coupled methane sequestration behavior across various fluid-bubble flows. Time-resolved spectral data clearly capture real-time variations in the concentration and conversion ratio of multiphase methane during hydrate growth, quantitatively revealing the dynamic evolution patterns and regulatory mechanisms in cold-seep environments. Experimental results indicate that the growth rate accelerates and the occupancy of large cages in cold-seep bubble flows increases by 15% relative to that of small cages influenced by low salinity and small solid particles. Furthermore, field model estimates indicate that the annual methane sequestration by hydrate-encapsulated bubbles at Site F is estimated to be about 0.34–2.77 t/yr, which accounts for roughly 3.3%–26.9% of the total methane leakage flux in this region. These findings fill critical quantitative gaps in understanding cold-seep methane sequestration dynamics and provide key parameters for incorporating hydrate-mediated sequestration into ocean carbon cycle models.
SN  - 0013-936X
SN  - 1520-5851
ER  -