Abstract:
Integration of mine disaster prevention with flue gas emission reduction can be achieved by injecting power plant flue gas into coal mine goafs, which is aligned with the national theme of green technology development. However, it is shown by field measurements that large-volume flue gas is often found to contain high oxygen levels, whereby the risk of spontaneous combustion of residual coal in the goafs is increased. Therefore, efficient and economical deoxygenation theories, technologies, and equipment tailored to the characteristics of power plant flue gas are urgently needed. Coal-based activated carbon is modified with iron nitrate to enhance its deoxygenation performance in a flue gas atmosphere. "The structures of the iron-based activated carbons are characterized by scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (SEM-EDS), X-ray diffraction (XRD), hydrogen temperature-programmed reduction (H
2-TPR), and Fourier transform infrared spectroscopy (FTIR). On this basis, simultaneous thermal analysis (STA) combined with non-isothermal kinetic theory is employed to reveal the oxidation kinetic behavior and mechanism of the iron-based activated carbons in a flue gas environment. Finally, the catalytic deoxygenation performance is verified on a fixed-bed reactor coupled with gas chromatography. The results indicate that Fe oxide clusters, typified by Fe
3O
4, with a diameter of approximately 1 μm, are formed on the surfaces of activated carbons through ferric nitrate modification, and the proportion of oxygen-containing functional groups on the activated carbon surfaces is increased; this proportion rises as the Fe loading is increased. The ignition temperatures of the activated carbons are reduced and the comprehensive combustion characteristic indices is enhanced by Fe oxide loading. At a 9% Fe loading, the ignition temperature is decreased by up to 21 ℃, and the comprehensive combustion characteristic index is increased by 10.6%. Furthermore, a linear correlation is observed between the amount of Fe-based oxide loading and the characteristic temperatures of the activated carbons in flue gas, including the maximum weight loss temperature, maximum heat release temperature, and burnout temperature. All these characteristic temperatures are decreased as the Fe oxide loading is increased. It is revealed by kinetic analysis that the oxidation activation energies of the activated carbons in a flue gas environment are significantly reduced, achieving a maximum reduction of 52.75 kJ/mol, a decrease of nearly 50%. Moreover, it is indicated by thermodynamic analysis that the entropy changes of the activated carbons oxidation process are reduced by the catalytic effect of Fe-based oxides, thereby accelerating gas adsorption during the reaction. Fixed-bed deoxygenation tests verify the performance advantages of the Fe-based activated carbons: a lower O
2 concentration and a higher CO
2 concentration in the exhaust gas are achieved; meanwhile, the deoxygenation reaction temperatures are reduced and CO emission is decreased by up to 81.5%. Theoretical guidance is thus provided for flue-gas-based fire prevention and extinguishing technologies.