[논문]Rapid Formation of Hydrogen-Enriched Hydrocarbon Gas Hydrates under Static Conditions

Lee, Wonhyeong; Kang, Dong Woo; Ahn, Yun-Ho; Lee, Jae W.

doi:10.1021/acssuschemeng.1c00807

[해외논문] Rapid Formation of Hydrogen-Enriched Hydrocarbon Gas Hydrates under Static Conditions

ACS sustainable chemistry et engineering, v.9 no.25, 2021년, pp.8414 - 8424

Lee, Wonhyeong (Department of Chemical and Biomolecular Engineering , Korea Advanced Institute of Science and Technology (KAIST) , 291 Daehak-ro , Yuseong-gu , Daejeon 34141 , Republic of Korea) , Kang, Dong Woo (Department of Chemical and Biomolecular Engineering , Korea Advanced Institute of Science and Technology (KAIST) , 291 Daehak-ro , Yuseong-gu , Daejeon 34141 , Republic of Korea) , Ahn, Yun-Ho , Lee, Jae W.

Abstract ▼ AI-Helper

This work introduces a “hydrate seed solution”, a 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-H2 and C2H6-H2 mixtures with the cyclopentane (CP) hydrate seed. The CP hydrate seed, which is immiscible with water, dominantly induces the growth of CH4-H2 and C2H6-H2 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-H2 or C2H6-H2 hydrate, and the overall reaction was much slower than the CP hydrate seed case. For the C2H6-H2 gas mixture, C2H6 molecules could not occupy the small cage of hydrates, but H2 mainly occupied the small cage. The THF hydrate seed provided a higher storage ratio of H2 than the CP hydrate seed because the seed-templated sII C2H6-H2 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.Hydrate seeds enable the rapid formation and storage of H2-blended natural gas in clathrate hydrate media without any energy-intensive agitation.[FIG OMISSION]

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