4.7 Article

Impacts of Long-Term Exposure to Supercritical Carbon Dioxide on Physicochemical Properties and Adsorption and Desorption Capabilities of Moisture-Equilibrated Coals

Journal

ENERGY & FUELS
Volume 35, Issue 15, Pages 12270-12287

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.energyfuels.1c01152

Keywords

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Funding

  1. National Natural Science Foundation of China [41762013, U19B6003]
  2. Yunnan Ten Thousand Talents Plan Young & Elite Talents Project [YNWR-QNBJ-2019-164]
  3. Open Foundation of Key Laboratory of Shale Oil and Gas Exploration & Production, SINOPEC [G5800-20-ZS-KFZY008]

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The long-term exposure of coal to scCO2-H2O significantly decreases mesopores in all coal types, while having minor effects on micropore surface area and volume. Additionally, the main oxygenic functional groups of coal are reduced and the Neimark fractal dimension increases after exposure, indicating increased pore surface roughness.
Regarding CO2 geologic sequestration in the coal seam, injected CO2 in the coal reservoir at an optimum depth often presents as supercritical fluid (scCO(2)), which is capable of changing the physicochemical properties of coal and further affecting its CO2 storage capacity. Aiming to better explore the aforementioned influences, we conducted a long-term scCO(2)-H2O-coal static interaction in the laboratory. The influences of scCO(2) exposure on the pore structure characteristics, the main oxygenic functional groups, and the high-pressure CO2 adsorption and desorption capabilities of four rank coals were explored. The results show that long-term scCO(2)-H2O exposure has minor effects on the coal micropore surface area and volume. On the contrary, it remarkably decreases the mesopore of all of the coals. The alterations in the coal pore structure parameters are mainly relevant to coal matrix swelling and mineral dissolution due to long-term scCO(2)-H2O exposure. In general, long-term scCO(2)-H2O exposure increases the Neimark fractal dimension of coals, further implying an elevated pore surface roughness and a more complex pore structure. Moreover, the main oxygenic functional groups, including C-O, C=O, and -COOH, of coals after long-term scCO(2) exposure are reduced. The aforementioned changes in the physicochemical properties of coals further affect their CO2 adsorption and desorption capabilities. In particular, the maximum CO2 adsorption capacity of high-rank coals decreases after exposure, whereas that of low-rank coals increases. Furthermore, the CO2 adsorption and desorption hystereses of coals become pronounced after long-term scCO(2)-H2O exposure, implying more stable CO2 sequestration in the coal seam. In conclusion, the implementation of CO2 sequestration in the coal seam should focus on the long-term scCO(2)-H2O-coal interaction.

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