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<p>During subsea CO<sub>2</sub> solidification and storage processes, as well as deepwater hydrate development, the presence of micron-sized sand and memory effect can efficiently promote hydrate reformation, but simultaneously increase the risk of pipeline blockage. Moreover, the micro-mechanism underlying the memory effect still remains controversial. In this study, sum frequency generation and flow loop experiments were conducted to investigate the CO<sub>2</sub> hydrate reformation and blocking with micro-sized sand. For the first time, we revealed the synergistic and symbiotic relationship between supersaturated gas molecules and residual cage structures in creating and intensifying the memory effect at the molecular scale. The roles of water films on sand in protecting and catalyzing residual cage structures were also identified. Considering the enlarged gas-liquid interface area and the richness of residual cage structures, novel kinetic models of hydrate reformation were established, with verified errors less than 12%. Two early warning signs and one late warning sign, characterizing the severity of blocking evolution, were proposed. The synergistic effect accelerating the blocking of the memory effect and micro-sized sand was realized by creating more aggregation-available interfaces for aggregates of bubble-hydrate shell and sand-hydrate. This work presents a novel perspective on the micro-mechanism of memory effect, and provides new predictive models and early warning methods for hydrate reformation-blocking in CCUS and hydrate development technologies.</p>

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Micro-mechanisms and macro-patterns of synergy between micron-sized sand and memory effect in CO2 hydrate reformation and blocking

  • 期刊论文

  • 发表日期：

    2026年3月12日

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  • Qingwen Kong,
  • Zhiyuan Wang,
  • Huan Diao,
  • Jie Zhong,
  • Qingjie Du,
  • Jianbo Zhang,
  • Heng Wang,
  • Weiqi Fu,
  • Zhiwei Yue

摘要

During subsea CO2 solidification and storage processes, as well as deepwater hydrate development, the presence of micron-sized sand and memory effect can efficiently promote hydrate reformation, but simultaneously increase the risk of pipeline blockage. Moreover, the micro-mechanism underlying the memory effect still remains controversial. In this study, sum frequency generation and flow loop experiments were conducted to investigate the CO2 hydrate reformation and blocking with micro-sized sand. For the first time, we revealed the synergistic and symbiotic relationship between supersaturated gas molecules and residual cage structures in creating and intensifying the memory effect at the molecular scale. The roles of water films on sand in protecting and catalyzing residual cage structures were also identified. Considering the enlarged gas-liquid interface area and the richness of residual cage structures, novel kinetic models of hydrate reformation were established, with verified errors less than 12%. Two early warning signs and one late warning sign, characterizing the severity of blocking evolution, were proposed. The synergistic effect accelerating the blocking of the memory effect and micro-sized sand was realized by creating more aggregation-available interfaces for aggregates of bubble-hydrate shell and sand-hydrate. This work presents a novel perspective on the micro-mechanism of memory effect, and provides new predictive models and early warning methods for hydrate reformation-blocking in CCUS and hydrate development technologies.