Various emerging carbon capture technologies depend on being able to reliably and consistently grow carbon dioxide hydrate, particularly in packed media. However, there are limited kinetic data for carbon dioxide hydrates at this length scale. In this work, carbon dioxide hydrate propagation rates and conversion were evaluated in a high pressure silicon microfluidic device. The carbon dioxide phase boundary was first measured in the microfluidic device, which showed little deviation from bulk predictions. Additionally, measuring the phase boundary takes on the order of hours compared to weeks or longer for larger scale experimental setups. Next, propagation rates of carbon dioxide hydrate were measured in the channels at low subcoolings (<2 K from phase boundary) and moderate pressures (200β500 psi). Growth was dominated by mass transfer limitations until a critical pressure was reached, and reaction kinetics limited growth upon further increases in pressure. Additionally, hydrate conversion was estimated from Raman spectroscopy in the microfluidics channels. A maximum value of 47% conversion was reached within 1 h of a constant flow experiment, nearly 4% of the time required for similar results in a large scale system. The rapid reaction times and high throughput allowed by high pressure microfluidics provide a new way for carbon dioxide gas hydrate to be characterized.
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21 March 2021
Research Article|
March 18 2021
Carbon dioxide hydrate in a microfluidic device: Phase boundary and crystallization kinetics measurements with micro-Raman spectroscopy
Special Collection:
Fluids in Nanopores
Jonathan D. Wells
;
Jonathan D. Wells
1
Center for Hydrate Research, Chemical and Biological Engineering Department, Colorado School of Mines
, Golden, Colorado 80401, USA
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Weiqi Chen;
Weiqi Chen
2
Department of Chemical and Biomolecular Engineering, New York University
, Brooklyn, New York 11201, USA
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Ryan L. Hartman
;
Ryan L. Hartman
a)
2
Department of Chemical and Biomolecular Engineering, New York University
, Brooklyn, New York 11201, USA
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Carolyn A. Koh
Carolyn A. Koh
a)
1
Center for Hydrate Research, Chemical and Biological Engineering Department, Colorado School of Mines
, Golden, Colorado 80401, USA
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Note: This paper is part of the JCP Special Topic on Fluids in Nanopores.
J. Chem. Phys. 154, 114710 (2021)
Article history
Received:
December 03 2020
Accepted:
March 04 2021
Citation
Jonathan D. Wells, Weiqi Chen, Ryan L. Hartman, Carolyn A. Koh; Carbon dioxide hydrate in a microfluidic device: Phase boundary and crystallization kinetics measurements with micro-Raman spectroscopy. J. Chem. Phys. 21 March 2021; 154 (11): 114710. https://doi.org/10.1063/5.0039533
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