Oxygen vacancies can capture and activate gaseous oxygen, forming surface chemisorbed oxygen, which plays an important role in the Hg 0 oxidation process. Fine control of oxygen vacancies is necessary and a major challenge in this field. A novel method for facet control combined with morphology control was used to synthesize Co 3 O 4 nanosheets preferentially growing (220) facet to give more oxygen vacancies. X-ray photoelectron spectroscopy (XPS) results show that the (220) facet has a higher Co 3+ /Co 2+ ratio, leading to more oxygen vacancies via the Co 3+ reduction process. Density functional theory (DFT) calculations confirm that the (220) facet has a lower oxygen vacancy formation energy. Furthermore, scanning electron microscopy (SEM) and transmission electron microscopy (TEM) results suggest that Co 3 O 4 nanosheets yield more defects during the synthesis process. These results are the reasons for the greater number of oxygen vacancies in Co 3 O 4 nanosheets, which is confirmed by electron energy loss spectroscopy (EELS), Raman spectroscopy, and photoluminescence (PL) spectroscopy. Therefore, Co 3 O 4 nanosheets show excellent Hg 0 removal efficiency over a wide temperature range of 100−350 °C at a high gas hourly space velocity (GHSV) of 180 000 h −1 . Additionally, the catalytic efficiency of Co 3 O 4 nanosheets is still greater than 83%, even after 80 h of testing, and it recovers to its original level after 2 h of in situ thermal treatment at 500 °C.
Sorbent of αMnO2 nanorods coating TiO2 shell (denoted as αMnO2-NR@TiO2) was prepared to investigate the elemental mercury (Hg0) removal performance in the presence of SO2. Due the core-shell structure, αMnO2-NR@TiO2 has a better SO2 resistance when compared to αMnO2 nanorods (denoted as αMnO2-NR). Kinetic studies have shown that both the sorption rates of αMnO2-NR and αMnO2-NR@TiO2, which can be described by pseudo second-order models and SO2 treatment, did not change the kinetic models for both the two catalysts. In contrast, X-ray photoelectron spectroscopy (XPS) results showed that, after reaction in the presence of SO2, S concentration on αMnO2-NR@TiO2 surface is lower than on αMnO2-NR surface, which demonstrated that TiO2 shell could effectively inhibit the SO2 diffusion onto MnO2 surface. Thermogravimetry-differential thermosgravimetry (TG-DTG) results further pointed that SO2 mainly react with TiO2 forming Ti(SO4)O in αMnO2-NR@TiO2, which will protect Mn from being deactivated by SO2. These results were the reason for the better SO2 resistance of αMnO2-NR@TiO2.
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