期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 25, 页码 8414-8424出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c00807
关键词
Clathrate hydrates; Hydrogen-enriched natural gas; Hydrate seed; Gas storage; Inclusion compounds
资金
- Ministry of Science and ICT (MIST), Republic of Korea [1711100593, N11190162, NRF-2019H1A2A1076070]
- National Research Foundation of Korea [N11190162] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
This study introduces a hydrate seed solution for the rapid formation of hydrogen-enriched hydrocarbon mixed hydrates, showing that the type of hydrate seed solution used can significantly impact the growth and structure of the resulting gas hydrates. THF hydrate seed provides a higher storage ratio of hydrogen compared to CP hydrate seed, indicating potential for enhanced formation of hydrogen-natural gas clathrates for sustainable energy gas storage.
This work introduces a hydrate seed solution, surfactant solution containing pre-constructed structure II (sII) hydrate crystals, for the rapid formation of hydrogen-enriched hydrocarbon mixed hydrates. We observed the instantaneous nucleation and fast growth of mixed gas hydrates for both CH4-H-2 and C2H6-H-2 mixtures with the cyclopentane (CP) hydrate seed. The CP hydrate seed, which is immiscible with water, dominantly induces the growth of CH4-H-2 and C2H6-H-2 mixed gas hydrates with thermodynamically favorable sI structure. However, the THF hydrate seed, which is miscible with water, induced the formation of seed-templated sII CH4-H-2 and C2H6-H(2 )hydrate, and the overall reaction was much slower than the CP hydrate seed case. For the C2H6-H-2 gas mixture, C2H6 molecules could not occupy the small cage of hydrates, but H-2 mainly occupied the small cage. The THF hydrate seed provided a higher storage ratio of H-2 than the CP hydrate seed because the seed-templated sII C2H6-H-2 gas hydrates have a larger number of small cages than does the structure I (sI) hydrate. As the CP hydrate seed concentration decreased from 2.78 to 0.278 mol %, the growth of the mixed gas hydrates was extremely accelerated, and the overall conversion was completed within 1 h. The growth kinetics of hydrogen-enriched hydrocarbon mixed hydrates in the non-stirred system was much faster than that in prior agitation-applied studies. These findings suggest a way forward to an enhanced formation of hydrogen-natural gas clathrates for sustainable energy gas storage.
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