Abstract
Carbon capture from flue gas and natural gas offers a green path to construct a net-zero emissions economic system. Selective adsorption-based gas separation by employing metal-organic frameworks (MOFs) is regarded as a promising technology due to the advantages of simple processing, easy regeneration and high efficiency. We synthesized two Zirconium MOFs (UiO-66 and UiO-66-NH2) nanocrystals for selective capture and further removal of CO2 from flue gas and natural gas. In particular, UiO-66-NH2 nanocrystals have a smaller grain size, a large amount of defects, and pending –NH2 groups inside their pores which display effective CO2 selective adsorption abilities over CH4 and N2 with the theoretical separation factors of 20 and 7. This breakthrough experiment further verified the selective adsorption-based separation process of natural gas and flue gas. In one further step, we used the Monte Carlo simulation to investigate the optimized adsorption sites and energy of CO2, N2 and CH4 molecules in the gas mixture. The significantly large adsorption energy of CO2 (0.32 eV) over N2 (0.19 eV) and N2 (0.2 eV) may help us to reveal the selective adsorption mechanism.
Highlights
Carbon dioxide (CO2 ) is regarded as the primary anthropogenic culprit for global warming and climate change, which is produced by fossil fuel [1]
The major demand for carbon capture comes from the treatment of CO2 mixture gas including power-plant flue gas, raw natural gas, coal-bed gas, and biogas in which CO2 is in wide concentration range and is mixed with different gases
About 5%–15% of CO2 is majorly mixed with N2 in power-plant flue gas, and a wide range of CO2 is regarded as an impurity of methane (CH4 ) for the raw natural gas (CH4 : >90%, CO2 : 0.5–1%) and coal-bed (CH4 : >50%, N2 : ~40%, CO2 : ~1%) [5] gas as well as biogas (CH4 : ~50%, CO2 : ~50%) [6]
Summary
Carbon dioxide (CO2 ) is regarded as the primary anthropogenic culprit for global warming and climate change, which is produced by fossil fuel [1]. The major demand for carbon capture comes from the treatment of CO2 mixture gas including power-plant flue gas, raw natural gas, coal-bed gas, and biogas in which CO2 is in wide concentration range and is mixed with different gases. About 5%–15% of CO2 is majorly mixed with N2 in power-plant flue gas, and a wide range of CO2 is regarded as an impurity of methane (CH4 ) for the raw natural gas (CH4 : >90%, CO2 : 0.5–1%) and coal-bed (CH4 : >50%, N2 : ~40%, CO2 : ~1%) [5] gas as well as biogas (CH4 : ~50%, CO2 : ~50%) [6]
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