Abstract

Carbon capture is a crucial part of global warming mitigation. Carbon capture via clathrate hydrate is an attractive approach due to its high capture capacity, high carbon dioxide purity, water-based benign process, ease of recycling, and robustness to contaminants. In this work, we propose a two-stage hydrate-based carbon dioxide separation system integrated with cold energy for carbon capture from flue gases. A thermodynamic cycle consisting of two sub-cycles was constructed to simulate the process. Operating conditions were optimized within the range of 274.15–282.15 K and 0.1–28.04 MPa, resulting in the lowest electricity consumption of 2.22 MJ/kg CO2 with 95.24 mol% CO2 purity and 65.97 % CO2 recovery. A higher CO2 recovery rate can be achieved by recycling the residual gas of Sub-cycle 2. Gas compression to the high operating pressure (16.01 MPa) is the major contributor to electricity consumption. By incorporating 100 % expansion work recovery from the high-pressure gases, the electricity consumption can be reduced to 0.43 MJ/kg CO2 (i.e., 0.119 kWh/kg CO2). A more realistic scenario assuming 80 % compression/pumping efficiency and 90 % expansion work recovery gives an electricity consumption of 1.16 MJ/kg CO2 (i.e., 0.322 kWh/kg CO2), representing an energy penalty of 33.1 % for a coal-fired power plant. Future direction for further improvement could be a paradigm shift to hydrate process with thermodynamic promoters, which can potentially reduce the operation pressure by over 90 % and thus cut down the energy consumption dramatically. This work established a framework to simulate the hydrate-based carbon capture process, evaluated its minimum energy consumption and examined how operating conditions affect the separation performance. The results could offer valuable guidelines for the design and optimization of real hydrate-based carbon capture systems.

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